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1. Gas barrier properties of polylactide/cellulose nanocrystals nanocomposites

Author

Hajar Faraj, Nadège Follain, Cyrille Sollogoub, Giana Almeida, Corinne Chappey, Stéphane Marais, Sylvie Tencé-Girault, Fabrice Gouanvé, Eliane Espuche, and Sandra Domenek

Subjects
PLA, CNC, Nanocomposites, Gas barrier properties, Nielsen model, Biocomposites, Polymers and polymer manufacture, TP1080-1185
Abstract

The development of polylactide (PLA)/cellulose nanocrystals (CNC) nanocomposites in the aim to increase gas barrier properties has been widely studied, but gave rise to conflicting results. To better understand the underlying gas transport mechanisms, PLA/CNC nanocomposites were produced at concentrations between 5 and 50 wt%. The role of the PLA/CNC interface for the permeability was investigated using three different CNC surface grafts, namely lauric acid (slightly interacting with PLA), stearic acid (non-interacting with PLA), and poly glycidyl methacrylate bearing a reactive epoxy end-group (crosslinking with PLA). While PLA/CNC composites contained a large number of aggregates, homogenously dispersed nanocomposites were obtained with surface modified CNCs even at high concentration of CNC (up to 30 wt%). All nanocomposites had better O2 and CO2 barrier properties than PLA. Surprisingly, the nanocomposites prepared with surface grafted CNC did not perform better than the ones prepared with neat CNC. The diffusion coefficient was successfully modeled with Nielsen's law, showing the importance of the shape factor and resulting tortuosity for the barrier performance notwithstanding PLA/CNC surface compatibility. The analysis of the dual-mode O2 sorption isotherm showed the creation of a similar quantity of supplementary sorption sites in nanocomposites prepared with neat or lauric acid grafted CNC. PGMA grafts induced a higher number of sorption sites. The most important advantage of CNC surface grafts was the shielding of CNC against water vapor uptake. As a result, the O2 barrier properties could be maintained constant up to 90% relative humidity.

Published
2022
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2. Novel Poly(Vinylidene Fluoride)/Montmorillonite Polymer Inclusion Membrane: Application to Cr(VI) Extraction from Polluted Water

Author

Ferhat Sellami, Ounissa Kebiche-Senhadji, Stéphane Marais, Charles Lanel, and Kateryna Fatyeyeva

Subjects
polymer inclusion membrane, Cr(VI) removal, montmorillonite, membrane rigidity, stability, Chemical technology, TP1-1185, Chemical engineering, TP155-156
Abstract

Novel hybrid polymer inclusion membranes (PIMs) based on poly(vinylidene fluoride) (PVDF) (polymer matrix) and Aliquat 336 (ion carrier) and containing native sodium (Cloisite Na+ (CNa)) and organo-modified (Cloisite 30B (C30B)) Montmorillonites were elaborated and tested for the removal of toxic Cr(VI) ions from the aqueous solution. The influence of the nanoclay incorporation on the physicochemical properties of PVDF-based PIMs was studied and the resulting membrane transport properties of the Cr(VI) ions were investigated in detail. The water contact angle measurements reveal that the incorporation of the CNa nanofiller affects the membrane wettability as less hydrophilic surface is obtained in this case—~47° in the presence of CNa as compared with ~15° for PIMs with C30B. The membrane rigidity is found to be dependent on the type and size of the used Montmorillonite. The increase of Young’s modulus is higher when CNa is incorporated in comparison with C30B. The stiffness of the PIM is strongly increased with CNa amount (four times higher with 30 wt %) which is not the case for C30B (only 1.5 times). Higher Cr(VI) permeation flux is obtained for PIMs containing CNa (~2.7 µmol/(m2·s)) owing to their porous structure as compared with membranes loaded with C30B and those without filler (~2 µmol/(m2·s) in both cases). The PIM with 20 wt % of native sodium Montmorillonite revealed satisfactory stability during five cycles of the Cr(VI) transport due to the high membrane rigidity and hydrophobicity. Much lower macromolecular chain mobility in this case allows limiting the carrier loss, thus increasing the membrane stability. On the contrary, a deterioration of the transport performance is recorded for the membrane filled with C30B and that without filler. The obtained results showed the possibility to extend the PIM lifetime through the incorporation of nanoparticles that diminish the carrier loss (Aliquat 336) from the membrane into the aqueous phase by limiting its mobility within the membrane by tortuosity effect and membrane stiffening without losing its permselective properties.

Published
2021
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3. Structural and Barrier Properties of Compatibilized PE/PA6 Multinanolayer Films

Author

Quentin Lozay, Quentin Beuguel, Nadège Follain, Laurent Lebrun, Alain Guinault, Guillaume Miquelard-Garnier, Sylvie Tencé-Girault, Cyrille Sollogoub, Eric Dargent, and Stéphane Marais

Subjects
PE/PA6 multinanolayer films, barrier properties, forced assembly coextrusion process, interphase, mechanical properties, serial model of diffusion, Chemical technology, TP1-1185, Chemical engineering, TP155-156
Abstract

The barrier performance and structural lightening of organic materials are increasingly desired and constitute a major challenge for manufacturers, particularly for transport and packaging. A promising technique which tends to emerge in recent years is that of multinanolayer coextrusion. The advantage is that it can produce multilayers made of thousands of very thin layers, leading to new properties due to crystalline morphology changes induced by confinement. This paper is focusing on the study of multinanolayered films with alternated polyethylene (PE), compatibilizer (PEgMA) and polyamide 6 (PA6) layers and made by a forced assembly coextrusion process equipped with layer multiplying elements (LME). PE/PA6 multilayer films consisting of 5 to 2049 layers (respectively 0 to 9 LME) were successfully obtained with well-organized multilayered structure. The evolution of the morphology and the microstructure of these two semi-crystalline polymers, when the thickness of each polymer layer decreases from micro-scale to nano-scale, was correlated to the water and gas transport properties of the PE/PA multilayers. The expected improvement of barrier properties was limited due to the on-edge orientation of crystals in very thin PE and PA6 layers. Despite this change of crystalline morphology, a slight improvement of the gas barrier properties was shown by comparing experimental results with permeabilities predicted on the basis of a serial model developed by considering a PE/PA6 interphase. This interphase observed by TEM images and the on-edge crystal orientation in multilayers were evidenced from mechanical properties showing an increase of the stiffness and the strength.

Published
2021
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4. Biodegradable PLA/PBSA Multinanolayer Nanocomposites: Effect of Nanoclays Incorporation in Multinanolayered Structure on Mechanical and Water Barrier Properties

Author

Tiphaine Messin, Nadège Follain, Quentin Lozay, Alain Guinault, Nicolas Delpouve, Jérémie Soulestin, Cyrille Sollogoub, and Stéphane Marais

Subjects
biodegradable polymers, coextrusion, multilayer film, barrier properties, montmorillonite fillers, Chemistry, QD1-999
Abstract

Biodegradable PLA/PBSA multinanolayer nanocomposites were obtained from semi-crystalline poly(butylene succinate-co-butylene adipate) (PBSA) nanolayers filled with nanoclays and confined against amorphous poly(lactic acid) (PLA) nanolayers in a continuous manner by applying an innovative coextrusion technology. The cloisite 30B (C30B) filler incorporation in nanolayers was considered to be an improvement of barrier properties of the multilayer films additional to the confinement effect resulting to forced assembly during the multilayer coextrusion process. 2049-layer films of ~300 µm thick were processed containing loaded PBSA nanolayers of ~200 nm, which presented certain homogeneity and were mostly continuous for the 80/20 wt% PLA/PBSA composition. The nanocomposite PBSA films (monolayer) were also processed for comparison. The presence of exfoliated and intercalated clay structure and some aggregates were observed within the PBSA nanolayers depending on the C30B content. A greater reduction of macromolecular chain segment mobility was measured due to combined effects of confinement effect and clays constraints. The absence of both polymer and clays interdiffusions was highlighted since the PLA glass transition was unchanged. Besides, a larger increase in local chain rigidification was evidenced through RAF values due to geometrical constraints initiated by close nanoclay contact without changing the crystallinity of PBSA. Tortuosity effects into the filled PBSA layers adding to confinement effects induced by PLA layers have caused a significant improvement of water barrier properties through a reduction of water permeability, water vapor solubility and water vapor diffusivity. The obtaining barrier properties were successfully correlated to microstructure, thermal properties and mobility of PBSA amorphous phase.

Published
2020
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5. Polyimide/Ionic Liquid Composite Membranes for Middle and High Temperature Fuel Cell Application: Water Sorption Behavior and Proton Conductivity

Author

Kateryna Fatyeyeva, Sergiy Rogalsky, Stanislav Makhno, Oksana Tarasyuk, Jorge Arturo Soto Puente, and Stéphane Marais

Subjects
porous polyimide membrane, ionic liquid, conductivity, vapour sorption, thermal stability, Chemical technology, TP1-1185, Chemical engineering, TP155-156
Abstract

Four water insoluble room-temperature protic ionic liquids (PILs) based on the N-alkylimidazolium cation with the alkyl chain length from 1 to 4 and bis(trifluoromethylsulfonyl)imide anion were synthesized and their chemical structure was confirmed by the 1H NMR and 19F NMR analysis. PILs were revealed to be thermally stable up to 360 and 400 °C. At the same time, the proton conductivity of PILs was found to be dependent mostly on the temperature and, to a less extent, on the type of the cation, i.e., the increase of the conductivity from ~3 × 10−4 S/cm at 25 °C to 2 × 10−2 S/cm at 150 °C was observed. The water vapour sorption capacity of PILs was evaluated as a function of relative humidity and the influence of the alkyl chain length on the phase behaviour in the PIL-water system was discussed. The composite polyimide/PILs membranes were prepared by the PIL immobilization in the porous polymer (Matrimid® 5218) film. The composite membranes showed a high level of proton conductivity (~10−3 S/cm) at elevated temperatures (up to 160 °C). The obtained results reveal that the elaborated composite polyimide/PIL membranes are promising candidates for the application as proton exchange membrane at middle and high temperatures.

Published
2020
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6. Enhanced water and oxygen barrier performance of flexible polyurethane membranes for biomedical application

Author

Aracelys Marcano, Marc Grimme, Stéphane Marais, Malys Koun, Corinne Chappey, Pascal Dubuis, and Kateryna Fatyeyeva

Subjects
Materials science, Polyurethanes, Delamination, Food Packaging, Metals and Alloys, Biomedical Engineering, Water, Permeation, Oxygen, Biomaterials, Crystallinity, Oxygen permeability, chemistry.chemical_compound, Membrane, Chemical engineering, chemistry, Ceramics and Composites, Polyvinyls, Layer (electronics), Deposition (law), Polyurethane
Abstract

In order to improve water and oxygen barrier properties, the surface of two commercial medical grade polyurethane (PU) membranes (Chronoflex® AR-LT and Bionate® II) was modified by a spray deposited film of poly(ethylene-co-vinyl alcohol) (EVOH). The influence of the temperature, the deposited layer thickness and the EVOH ethylene group percentage (27%, 32%, and 44% for EVOH27, EVOH32, and EVOH44, respectively) on the barrier properties of the PU/EVOH multilayered membranes was investigated. The increase of the EVOH layer thickness leads to higher oxygen barrier properties (the highest barrier improvement factor of 412 was obtained). However, in case of the deposited layer thickness higher than 18 μm, microcracks appeared on the treated surface promote a significant loss of the barrier effect. Due to its higher crystallinity degree, EVOH27 provides a higher oxygen barrier effect compared to EVOH32 and EVOH44. On the contrary, an increase of the water barrier properties was observed with the increase of the percentage of ethylene groups. Moreover, the delamination of the EVOH layer was noted after water permeation, especially in case of EVOH44, which is the most hydrophobic layer. Nevertheless, significant decrease of the water and oxygen permeability of the modified PU membranes was achieved, thus showing the benefit of using the EVOH spray deposition for the biomedical application, which requires high performance material with flexible and barrier properties.

Published
2021
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7. Polyoxadiazoles as proton exchange membranes for fuel cell application

Author

Kateryna Fatyeyeva, Yaroslav L. Kobzar, Stéphane Marais, Corinne Chappey, and Nicolas Desilles

Subjects
Materials science, Proton, General Chemical Engineering, 02 engineering and technology, Conductivity, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Membrane, Chemical engineering, Fuel cells, Thermal stability, 0210 nano-technology
Abstract

The number of researches on the ion exchange membrane has increased considerably in recent years showing interest in fuel cell technology for the automobile and portable applications. The most promising fuel cell technology for low-temperature operation (80 °C

Published
2021
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9. PVC/EVA-based polymer inclusion membranes with improved stability and Cr(VI) extraction capacity: Water plasticization effect

Author

Ferhat Sellami, Ounissa Kebiche-Senhadji, Stéphane Marais, and Kateryna Fatyeyeva

Subjects
History, Environmental Engineering, Polymers and Plastics, Health, Toxicology and Mutagenesis, Environmental Chemistry, Business and International Management, Pollution, Waste Management and Disposal, Industrial and Manufacturing Engineering
Abstract

Polymer inclusion membranes (PIMs) are far investigated for their ability to extract heavy metals and small organic compounds from aqueous media. Polyvinyl chloride (PVC) is one of the most widely used base polymers for the PIM elaboration. However, its use requires the incorporation of a relatively expensive liquid plasticizer. In the present work, poly(ethylene-co-vinyl acetate) (EVA) serves as a polymer plasticizer for the elaboration of PIMs based on PVC as a base polymer and Aliquat 336 as a carrier. The composition of PIMs was optimized in terms of the PVC/EVA ratio and the vinyl acetate (VA) groups content (x) of EVA (i.e. EVA

Published
2022

10. Preparation and study of the thermal, barrier and antibacterial properties of Polylactic acid-Fluorphlogopite-Silver nanoparticles nanocomposite films

Author

Abderrahmane Nabgui, Nadège Follain, Elvira Vidović, Jamal El Haskouri, Stéphane Marais, Abdellatif El Meziane, Mohamed Lahcini, and Pascal Thébault

Subjects
General Chemical Engineering, Organic Chemistry, Materials Chemistry, antimicrobial food packaging, polylactic acid, fluorphlogopite silver nanoparticles, antibacterial activity, barrier properties, thermal properties, Surfaces, Coatings and Films
Abstract

Nowadays, there is an increasing need to develop new green biodegradable materials for active antimicrobial food packaging applications. In this work, polylactic acid-2 % Fluorphlogopite-1.5%silver nanoparticles (AgNPs) composites were prepared using melt extrusion. Films were characterized using Scanning Electron Microscopy, Transmission Electron Microscopy, X-Ray Diffraction, Differential Scanning Calorimetry, and Water Contact Angle measurements. Results showed a good dispersion of both fluorphlogopite and AgNPs in PLA which increased the surface roughness and hydrophobicity of PLA. Subsequently, the thermal, mechanical, and barrier properties of PLA nanocomposites were assessed. PLA-2%Fluorphlogopite-1.5%AgNPs showed a higher thermal stability than neat PLA while the mechanical properties remained unchanged. Furthermore, the excellent barrier properties of PLA were also unaffected by the introduction of fluorphlogopite and AgNPs. Finally, the antibacterial activity of the nanocomposites was assessed against three bacteria, S. aureus, E. faecalis, and E. coli and PLA-2%Fluorphlogopite-1.5%AgNPs inhibited almost completely the bacterial adhesion on the surface of the films.

Published
2022

11. Novel Ionic Conducting Composite Membrane Based on Polymerizable Ionic Liquids

Author

Ghania Azzouz, Corinne Chappey, Kateryna Fatyeyeva, Stéphane Marais, Yaroslav L. Kobzar, Annie-Claude Gaumont, Laurence Lecamp, Isabelle Dez, Hashim Albadri, and Jocelyne Levillain

Subjects
chemistry.chemical_classification, Materials science, Polymers and Plastics, Synthetic membrane, Organic chemistry, Ionic bonding, General Chemistry, Polymer, Electrolyte, Article, fuel cell, chemistry.chemical_compound, QD241-441, Membrane, Chemical engineering, chemistry, Polymerization, Ionic liquid, photopolymerization, Thermal stability, conductivity, polymerizable ionic liquid, polymer membranes
Abstract

In this work, the design and characterization of new supported ionic liquid membranes, as medium-temperature polymer electrolyte membranes for fuel-cell application, are described. These membranes were elaborated by the impregnation of porous polyimide Matrimid® with different synthesized protic ionic liquids containing polymerizable vinyl, allyl, or methacrylate groups. The ionic liquid polymerization was optimized in terms of the nature of the used (photo)initiator, its quantity, and reaction duration. The mechanical and thermal properties, as well as the proton conductivities of the supported ionic liquid membranes were analyzed in dynamic and static modes, as a function of the chemical structure of the protic ionic liquid. The obtained membranes were found to be flexible with Young’s modulus and elongation at break values were equal to 1371 MPa and 271%, respectively. Besides, these membranes exhibited high thermal stability with initial decomposition temperatures &gt, 300 °C. In addition, the resulting supported membranes possessed good proton conductivity over a wide temperature range (from 30 to 150 °C). For example, the three-component Matrimid®/vinylimidazolium/polyvinylimidazolium trifluoromethane sulfonate membrane showed the highest proton conductivity—~5 × 10−2 mS/cm and ~0.1 mS/cm at 100 °C and 150 °C, respectively. This result makes the obtained membranes attractive for medium-temperature fuel-cell application.

Published
2021

12. Novel Poly(Vinylidene Fluoride)/Montmorillonite Polymer Inclusion Membrane: Application to Cr(VI) Extraction from Polluted Water

Author

Kateryna Fatyeyeva, Charles Lanel, Ferhat Sellami, Stéphane Marais, and Ounissa Kebiche-Senhadji

Subjects
Aqueous solution, membrane rigidity, Process Chemistry and Technology, Chemical technology, Aqueous two-phase system, Filtration and Separation, montmorillonite, TP1-1185, Aliquat 336, Membrane transport, Permeation, stability, Article, polymer inclusion membrane, chemistry.chemical_compound, Membrane, Montmorillonite, Chemical engineering, chemistry, Chemical Engineering (miscellaneous), TP155-156, Fluoride, Cr(VI) removal
Abstract

Novel hybrid polymer inclusion membranes (PIMs) based on poly(vinylidene fluoride) (PVDF) (polymer matrix) and Aliquat 336 (ion carrier) and containing native sodium (Cloisite Na+ (CNa)) and organo-modified (Cloisite 30B (C30B)) Montmorillonites were elaborated and tested for the removal of toxic Cr(VI) ions from the aqueous solution. The influence of the nanoclay incorporation on the physicochemical properties of PVDF-based PIMs was studied and the resulting membrane transport properties of the Cr(VI) ions were investigated in detail. The water contact angle measurements reveal that the incorporation of the CNa nanofiller affects the membrane wettability as less hydrophilic surface is obtained in this case—~47° in the presence of CNa as compared with ~15° for PIMs with C30B. The membrane rigidity is found to be dependent on the type and size of the used Montmorillonite. The increase of Young’s modulus is higher when CNa is incorporated in comparison with C30B. The stiffness of the PIM is strongly increased with CNa amount (four times higher with 30 wt %) which is not the case for C30B (only 1.5 times). Higher Cr(VI) permeation flux is obtained for PIMs containing CNa (~2.7 µmol/(m2·s)) owing to their porous structure as compared with membranes loaded with C30B and those without filler (~2 µmol/(m2·s) in both cases). The PIM with 20 wt % of native sodium Montmorillonite revealed satisfactory stability during five cycles of the Cr(VI) transport due to the high membrane rigidity and hydrophobicity. Much lower macromolecular chain mobility in this case allows limiting the carrier loss, thus increasing the membrane stability. On the contrary, a deterioration of the transport performance is recorded for the membrane filled with C30B and that without filler. The obtained results showed the possibility to extend the PIM lifetime through the incorporation of nanoparticles that diminish the carrier loss (Aliquat 336) from the membrane into the aqueous phase by limiting its mobility within the membrane by tortuosity effect and membrane stiffening without losing its permselective properties.

Published
2021

13. Structural and Barrier Properties of Compatibilized PE/PA6 Multinanolayer Films

Author

Sylvie Tencé-Girault, Quentin Beuguel, Quentin Lozay, Nadège Follain, Cyrille Sollogoub, Laurent Lebrun, Guillaume Miquelard-Garnier, Stéphane Marais, Alain Guinault, Eric Dargent, Polymères Biopolymères Surfaces (PBS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Groupe de physique des matériaux (GPM), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Procédés et Ingénierie en Mécanique et Matériaux (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-Centre National de la Recherche Scientifique (CNRS)-Arts et Métiers Sciences et Technologies, HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM), ANR-16-CE08-0035,IMMUNE,Matériaux Innovants par procédé d'extrusion multi-nanocouches(2016), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Polymères, biopolymères, membranes (PBM), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), and Normandie Université (NU)

Subjects
Morphology (linguistics), Materials science, barrier properties, Filtration and Separation, 02 engineering and technology, mechanical properties, Sciences de l'ingénieur, lcsh:Chemical technology, 010402 general chemistry, 01 natural sciences, Article, chemistry.chemical_compound, [CHIM]Chemical Sciences, Chemical Engineering (miscellaneous), General Materials Science, lcsh:TP1-1185, lcsh:Chemical engineering, Composite material, ComputingMilieux_MISCELLANEOUS, PE/PA6 multinanolayer films, chemistry.chemical_classification, Thin layers, Process Chemistry and Technology, lcsh:TP155-156, forced assembly coextrusion process, [CHIM.MATE]Chemical Sciences/Material chemistry, Polymer, Polyethylene, interphase, 021001 nanoscience & nanotechnology, Microstructure, 0104 chemical sciences, serial model of diffusion, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Polyamide, Interphase, 0210 nano-technology, Layer (electronics)
Abstract

The barrier performance and structural lightening of organic materials are increasingly desired and constitute a major challenge for manufacturers, particularly for transport and packaging. A promising technique which tends to emerge in recent years is that of multinanolayer coextrusion. The advantage is that it can produce multilayers made of thousands of very thin layers, leading to new properties due to crystalline morphology changes induced by confinement. This paper is focusing on the study of multinanolayered films with alternated polyethylene (PE), compatibilizer (PEgMA) and polyamide 6 (PA6) layers and made by a forced assembly coextrusion process equipped with layer multiplying elements (LME). PE/PA6 multilayer films consisting of 5 to 2049 layers (respectively 0 to 9 LME) were successfully obtained with well-organized multilayered structure. The evolution of the morphology and the microstructure of these two semi-crystalline polymers, when the thickness of each polymer layer decreases from micro-scale to nano-scale, was correlated to the water and gas transport properties of the PE/PA multilayers. The expected improvement of barrier properties was limited due to the on-edge orientation of crystals in very thin PE and PA6 layers. Despite this change of crystalline morphology, a slight improvement of the gas barrier properties was shown by comparing experimental results with permeabilities predicted on the basis of a serial model developed by considering a PE/PA6 interphase. This interphase observed by TEM images and the on-edge crystal orientation in multilayers were evidenced from mechanical properties showing an increase of the stiffness and the strength.

Published
2021
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14. Biodegradable PLA/PBSA Multinanolayer Nanocomposites: Effect of Nanoclays Incorporation in Multinanolayered Structure on Mechanical and Water Barrier Properties

Author

Nadège Follain, Jérémie Soulestin, Tiphaine Messin, Nicolas Delpouve, Alain Guinault, Stéphane Marais, Cyrille Sollogoub, Quentin Lozay, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Polymères, biopolymères, membranes (PBM), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU), Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Procédés et Ingénierie en Mécanique et Matériaux (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-Centre National de la Recherche Scientifique (CNRS)-Arts et Métiers Sciences et Technologies, HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM), Groupe de physique des matériaux (GPM), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Département Technologie des Polymères et Composites & Ingénierie Mécanique (TPCIM), École des Mines de Douai (Mines Douai EMD), and Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-Ministère de l'Économie, des Finances et de l'Industrie [Paris, France]

Subjects
Materials science, General Chemical Engineering, barrier properties, 02 engineering and technology, coextrusion, 010402 general chemistry, 01 natural sciences, Article, lcsh:Chemistry, Crystallinity, montmorillonite fillers, Monolayer, [CHIM]Chemical Sciences, General Materials Science, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Nanocomposite, Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Microstructure, Biodegradable polymer, 0104 chemical sciences, Amorphous solid, [CHIM.POLY]Chemical Sciences/Polymers, Chemical engineering, chemistry, lcsh:QD1-999, biodegradable polymers, multilayer film, 0210 nano-technology, Glass transition
Abstract

Biodegradable PLA/PBSA multinanolayer nanocomposites were obtained from semi-crystalline poly(butylene succinate-co-butylene adipate) (PBSA) nanolayers filled with nanoclays and confined against amorphous poly(lactic acid) (PLA) nanolayers in a continuous manner by applying an innovative coextrusion technology. The cloisite 30B (C30B) filler incorporation in nanolayers was considered to be an improvement of barrier properties of the multilayer films additional to the confinement effect resulting to forced assembly during the multilayer coextrusion process. 2049-layer films of ~300 &micro, m thick were processed containing loaded PBSA nanolayers of ~200 nm, which presented certain homogeneity and were mostly continuous for the 80/20 wt% PLA/PBSA composition. The nanocomposite PBSA films (monolayer) were also processed for comparison. The presence of exfoliated and intercalated clay structure and some aggregates were observed within the PBSA nanolayers depending on the C30B content. A greater reduction of macromolecular chain segment mobility was measured due to combined effects of confinement effect and clays constraints. The absence of both polymer and clays interdiffusions was highlighted since the PLA glass transition was unchanged. Besides, a larger increase in local chain rigidification was evidenced through RAF values due to geometrical constraints initiated by close nanoclay contact without changing the crystallinity of PBSA. Tortuosity effects into the filled PBSA layers adding to confinement effects induced by PLA layers have caused a significant improvement of water barrier properties through a reduction of water permeability, water vapor solubility and water vapor diffusivity. The obtaining barrier properties were successfully correlated to microstructure, thermal properties and mobility of PBSA amorphous phase.

Published
2020
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15. The Impact of Reactive Ionic Liquids Addition on the Physicochemical and Sorption Properties of Poly(Vinyl Alcohol)-Based Films

Author

Guoqiang Li, Kateryna Fatyeyeva, Zbigniew Rafiński, Stéphane Marais, Joanna Kujawa, Andrzej Wolan, Krzysztof Dzieszkowski, Corinne Chappey, Edyta Rynkowska, and Wojciech Kujawski

Subjects
sorption kinetics, Vinyl alcohol, Thermogravimetric analysis, Materials science, Polymers and Plastics, Synthetic membrane, Sorption, General Chemistry, Article, poly(vinyl alcohol), lcsh:QD241-441, chemistry.chemical_compound, Membrane, lcsh:Organic chemistry, chemistry, Chemical engineering, Bromide, Ionic liquid, Fourier transform infrared spectroscopy, reactive ionic liquids, polymer membranes
Abstract

A new type of hybrid polymeric-based film containing 1-(1,3-diethoxy-1,3-dioxopropan-2-ylo)-3-methylimidazolium bromide (RIL1_Br) and 1-(2-etoxy-2-oxoethyl)-3-methylimidazolium bromide (RIL2_Br) reactive ionic liquids was elaborated. Poly(vinyl alcohol) (PVA)-based films with 9–33 wt % of RILs were subsequently characterized using Fourier transform infrared spectroscopy with attenuated total reflectance (FTIR-ATR), scanning electron microscopy (SEM), atomic force microscopy (AFM), thermogravimetric analysis (TGA) and TGA-FTIR. PVA-RIL films were also studied in tensile tests, contact angle and sorption measurements. RIL incorporation enhanced thermal and mechanical stability of PVA membranes due to the hydrogen bonds between RILs and polymer chains. Membrane swelling behavior in water (H2O), ethanol (EtOH), and propan-2-ol (IPA) and the kinetics of water sorption process revealed that PVA-RILs membranes possess the highest affinity towards water. It was pointed out that both the RIL type and the RIL amount in the polymer matrix have significant influence on the membrane swelling behavior and the water sorption kinetics.

Published
2020

16. Polyimide/Ionic Liquid Composite Membranes for Middle and High Temperature Fuel Cell Application: Water Sorption Behavior and Proton Conductivity

Author

Sergiy Rogalsky, Jorge Arturo Soto Puente, Kateryna Fatyeyeva, Stanislav Makhno, Oksana Tarasyuk, and Stéphane Marais

Subjects
Materials science, Proton exchange membrane fuel cell, Filtration and Separation, 02 engineering and technology, Conductivity, 010402 general chemistry, lcsh:Chemical technology, 01 natural sciences, Article, thermal stability, chemistry.chemical_compound, Chemical Engineering (miscellaneous), Thermal stability, porous polyimide membrane, lcsh:TP1-1185, lcsh:Chemical engineering, Alkyl, ionic liquid, vapour sorption, chemistry.chemical_classification, Process Chemistry and Technology, lcsh:TP155-156, Sorption, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Membrane, Chemical engineering, chemistry, Ionic liquid, conductivity, 0210 nano-technology, Polyimide
Abstract

Four water insoluble room-temperature protic ionic liquids (PILs) based on the N-alkylimidazolium cation with the alkyl chain length from 1 to 4 and bis(trifluoromethylsulfonyl)imide anion were synthesized and their chemical structure was confirmed by the 1H NMR and 19F NMR analysis. PILs were revealed to be thermally stable up to 360 and 400 &deg, C. At the same time, the proton conductivity of PILs was found to be dependent mostly on the temperature and, to a less extent, on the type of the cation, i.e., the increase of the conductivity from ~3 &times, 10&minus, 4 S/cm at 25 &deg, C to 2 &times, 2 S/cm at 150 &deg, C was observed. The water vapour sorption capacity of PILs was evaluated as a function of relative humidity and the influence of the alkyl chain length on the phase behaviour in the PIL-water system was discussed. The composite polyimide/PILs membranes were prepared by the PIL immobilization in the porous polymer (Matrimid&reg, 5218) film. The composite membranes showed a high level of proton conductivity (~10&minus, 3 S/cm) at elevated temperatures (up to 160 &deg, C). The obtained results reveal that the elaborated composite polyimide/PIL membranes are promising candidates for the application as proton exchange membrane at middle and high temperatures.

Published
2020

17. Imidazolium-based protic ionic liquids with perfluorinated anions: Influence of chemical structure on thermal properties

Author

Kateryna Fatyeyeva, Ya. L. Kobzar, A. Martin, Stéphane Marais, H. Oulyadi, and Y. Prykhodko

Subjects
chemistry.chemical_classification, Thermogravimetric analysis, Chemistry, Chemical structure, Condensed Matter Physics, Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials, chemistry.chemical_compound, Differential scanning calorimetry, Polymer chemistry, Ionic liquid, Materials Chemistry, Side chain, Thermal stability, Physical and Theoretical Chemistry, Fourier transform infrared spectroscopy, Spectroscopy, Alkyl
Abstract

The influence of the cation chemical structure, namely its side chain, on the thermal properties of imidazolium-based protic ionic liquids (PILs) with different perfluorinated anions (trifluoromethanesulfonimide (TFSI), trifluoromethanesulfonic (TFS), and trifluoroacetic (TFA) acids) was studied. With that purpose, twenty-one PILs with various alkyl (methyl-, ethyl-, butyl- and vinyl-) and fluorinated (-CH2CF3, -CH2CHF2, and -CH2CH2F) side chains were successfully synthesized. Special attention was paid to an optimization of their synthesis conditions. The structure of synthesized fluorinated and alkyl-substituted PILs was confirmed by means of nuclear magnetic resonance (NMR) analysis (1D: 1H, 19F, 13C and 2D: 1H – 19F HOESY experiments) and Fourier transform infrared (FTIR) spectroscopy, while PILs thermal behavior was determined by differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) in dynamic and isothermal modes. The correlation between the PILs chemical structure and their thermal stability was established. It has been found that an increase of the length of alkyl side chain (methyl

Published
2022
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18. New ionic liquid-based polyoxadiazole electrolytes for hydrogen middle- and high-temperature fuel cells

Author

Ye.V. Lobko, Yu.V. Yakovlev, Ya. L. Kobzar, T. Hrbek, Stéphane Marais, and Kateryna Fatyeyeva

Subjects
chemistry.chemical_classification, Materials science, Polyvinylpyrrolidone, Hydrogen, chemistry.chemical_element, Filtration and Separation, Polymer, Electrolyte, Atmospheric temperature range, Biochemistry, chemistry.chemical_compound, Membrane, chemistry, Chemical engineering, Ionic liquid, medicine, General Materials Science, Thermal stability, Physical and Theoretical Chemistry, medicine.drug
Abstract

New polyoxadiazole-based supported ionic liquid membranes were designed and elaborated for the first time to be used as a middle- and high-temperature polymer electrolyte membrane for fuel cell application. The proposed membrane molecular design combined hydroxyl-functionalized sulfonated polyoxadiazole, hydrophilic polyvinylpyrrolidone and specific protic ionic liquid, thus allowing elaboration of membranes with remarkable physical-chemical characteristics. It is found that the fine tuning of the membranes properties is possible by varying the ratio of polyoxadiazole and polyvinylpyrrolidone. The obtained membranes reveal high thermal stability in dynamic and static modes (up to 350 °C), good oxidative stability, sufficient mechanical properties (Young's modulus of 0.3–21.4 MPa and elongation at break from of 6 to 174%), high degree of ionic liquid impregnation (up to 297%), stable and relatively high conductivity (up to 1.3 mS∙cm−1) in a wide temperature range (from 40 to 120 °С) and under dry conditions. All these properties make the elaborated membranes very attractive for middle- and high-temperature fuel cell application.

Published
2021
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19. Polycarbonate/mica extrusion using mixing elements: Improvement of transparency and thermal, mechanical and water and gas barrier properties

Author

José Ortiz, Kateryna Fatyeyeva, Bassidi Diawara, and Stéphane Marais

Subjects
chemistry.chemical_classification, Molar mass, Water transport, Materials science, Polymers and Plastics, Organic Chemistry, Polymer, chemistry, visual_art, Materials Chemistry, visual_art.visual_art_medium, Thermal stability, Extrusion, Mica, Polycarbonate, Composite material, Dispersion (chemistry)
Abstract

Polycarbonate (PC) was loaded with mica fillers by melt mixing process using a twin-screw extruder. The influence of the mica content on the PC properties was analyzed. Also, the presence of mixing elements of grid shape on the mica distribution during the PC extrusion was discussed. These elements allowed us to significantly improve the fillers dispersion in the polymer matrix. As a consequence, the transparency of the PC films was maintained up to 5 wt% of mica due to reducing the aggregates formation and the homogeneous mica dispersion. Despite a slight decrease of the polymer molar mass, a strong improvement of the PC thermal stability, mechanical resistance as well as barrier properties towards water and gases (N2, O2 and CO2) was obtained due to the reinforce and tortuosity effects induced by mica fillers in the PC matrix. The gas and water transport properties of the PC/mica films were well-fitted using a predictive empirical model, that took into account the double tortuosity and immobility effect of mica particles. In addition, mica fillers were found to have specific interactions with water molecules, that led to enhancement of the moisture resistance of PC, thus improving its performance.

Published
2021
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20. Physicochemical properties and pervaporation performance of dense membranes based on cellulose acetate propionate (CAP) and containing polymerizable ionic liquid (PIL)

Author

Stéphane Marais, Edyta Rynkowska, Andrzej Wolan, Antoine Lancien, Krzysztof Dzieszkowski, Kateryna Fatyeyeva, Anthony Szymczyk, Joanna Kujawa, Wojciech Kujawski, Stanisław Koter, Nicolaus Copernicus University [Toruń], Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), DEC-2015/18/M/ST5/00635, NCN, Narodowe Centrum Nauki, Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Filtration and Separation, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biochemistry, Cellulose acetate propionate, chemistry.chemical_compound, medicine, [CHIM]Chemical Sciences, Organic chemistry, General Materials Science, Physical and Theoretical Chemistry, Plasticization, Plasticizer, Polymerizable ionic liquids, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Hildebrand solubility parameter, Monomer, Membrane, Hydrophilic pervaporation, chemistry, Chemical engineering, Ionic liquid, Pervaporation, Swelling, medicine.symptom, 0210 nano-technology, Hybrid material, Hansen's solubility parameters
Abstract

International audience; The new type of efficient pervaporative separation hybrid materials based on cellulose acetate propionate (CAP) and doped with 1-methyl-3-(4-vinylbenzyl)-1H-imidazol-3-ium chloride polymerizable ionic liquid (PIL) monomers (12.3–44.4 wt%) were elaborated for dehydration of propan-2-ol. Broad material and physicochemical characterization of membranes was performed including assessment of physicochemical, equilibrium, transport, and separation properties. Incorporation of PIL results in the plasticization of CAP based membranes. Additionally, with increasing loading of PIL from 12.3 to 44.4 wt% values of thickness-normalized Pervaporation Separation Index (PSIN) increase 1.6–2.4 times comparing to unloaded membrane (pure CAP). The distance parameters calculated on the base of the Hansen's solubility parameters were additionally employed to interpret swelling and pervaporative properties of membranes as well as to discuss interactions between solvents and prepared membranes. Lower value of distance parameter between pristine CAP and ethanol corresponds to the highest molar swelling degree of CAP based membranes. Swelling of CAP-PIL membranes in contact with water, ethanol, and propan-2-ol increased with of the increasing PIL content due to the hydrophilic character of ionic liquid. The gathered data provided insight into the potential applicability of the novel hybrid separation materials for pervaporative separation of liquid-liquid mixtures. © 2017 Elsevier B.V.

Published
2017
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21. How the chemical structure of the plasma-deposited SiOx film modifies its stability and barrier properties: FTIR study

Author

Thanh Hien Tran, Fabienne Poncin-Epaillard, Stéphane Marais, Dominique Debarnot, D.B. Au, Bassidi Diawara, J. Ortiz, Kateryna Fatyeyeva, Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Centre National de la Recherche Scientifique (CNRS), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)

Subjects
Materials science, General Chemical Engineering, PECVD, 02 engineering and technology, Substrate (electronics), engineering.material, 010402 general chemistry, 01 natural sciences, Coating, X-ray photoelectron spectroscopy, Materials Chemistry, inorganic silicon, [CHIM]Chemical Sciences, Fourier transform infrared spectroscopy, Thin film, Polycarbonate, ComputingMilieux_MISCELLANEOUS, density, Organic Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, Permeation, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Surfaces, Coatings and Films, [CHIM.POLY]Chemical Sciences/Polymers, Chemical engineering, visual_art, engineering, visual_art.visual_art_medium, permeation, Wetting, 0210 nano-technology, fluorinated silicon
Abstract

Organosilicon thin films issued from the gas mixture of oxygen and hexamethyledisiloxane (HMDSO), 2,4,6,8-tetramethylcyclotetrasiloxane (TMCTS), or fluorotriethoxysilane (FTEOS) deposited on polycarbonate (PC) substrate were obtained thanks to a RF plasma source. The chemical structure of the two types of inorganic SiOx (HMDSO/O2, TMCTS/O2) and fluorinated SiOxCyFz (FTEOS/O2, FTEOS/O2/TMCTS) coatings have been investigated by FTIR and XPS spectroscopies, and wettability measurement. Network structure and density of SiOx and SiOxCyFz thin films were discussed as a function of the νSiOSi band shifting observed in their respective FTIR spectra. The influence of various plasma parameters (such as discharge power, precursor/O2 ratio and, duration) on the film properties was studied in order to optimize the growth of both inorganic and fluorinated thin films. The ageing of such layers either at ambient atmosphere or even at reduced pressure showed a chemical alteration of the thin films surface and bulk, which stabilized after 15 days of storage. Such phenomenon is explained by the hydrophobicity recovery that may induce the observed network alteration. Water and oxygen permeation and transport properties of treated PC films were correlated with the coating structure and composition; then TMCTS was identified as the most efficient precursor for enhancing water barrier property. Furthermore, the permeation properties of these deposits seem to be more controlled by the material density than by their chemistry.

Published
2019
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22. Evolution of mechanical and barrier properties of thermally aged polycarbonate films

Author

Bassidi Diawara, José Ortiz, Corinne Chappey, Kateryna Fatyeyeva, Laurent Colasse, Stéphane Marais, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), and Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Filtration and Separation, 02 engineering and technology, Thermal treatment, 010402 general chemistry, 01 natural sciences, Biochemistry, Contact angle, Ultimate tensile strength, General Materials Science, Physical and Theoretical Chemistry, Composite material, Polycarbonate, ComputingMilieux_MISCELLANEOUS, Relaxation (NMR), [CHIM.MATE]Chemical Sciences/Material chemistry, Permeation, 021001 nanoscience & nanotechnology, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.POLY]Chemical Sciences/Polymers, Volume (thermodynamics), visual_art, visual_art.visual_art_medium, 0210 nano-technology, Glass transition
Abstract

Polycarbonate (PC) films of two different grades (Macrolon® LED 2245 and Macrolon® AL 2447) were elaborated and thermally aged at 100, 120 and 140 °C during intermediate and long times of aging. The physical aging effect on the film properties was analyzed by infrared spectroscopy, water contact angle, thermal and tensile tests, and water and gas permeation and sorption measurements. The effect of thermal treatment on PC properties was revealed, especially for the film aged at 120 °C. Aging caused a continual increase of PC glass transition temperature and relaxation enthalpy, an increase in Young's modulus and yield strength values and a decrease in the elongation at break. These results were attributed to the reduction of the free volume because of the PC conformational changes. The film barrier properties using liquid water and gas (N2, O2 and CO2) molecules as probes were studied in order to highlight the free volume evolution. It was shown that physical aging caused a reduction of water and gas permeability. This fact was mainly explained by the decrease of the solubility coefficient with the aging time increase.

Published
2019
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23. Chemically and Thermally Crosslinked PVA-Based Membranes: Effect on Swelling and Transport Behavior

Author

Wojciech Kujawski, Joanna Kujawa, Stéphane Marais, Kateryna Fatyeyeva, and Edyta Rynkowska

Subjects
Vinyl alcohol, Polymers and Plastics, Synthetic membrane, Alcohol, macromolecular substances, Thermal treatment, contact angle measurements, Article, lcsh:QD241-441, chemistry.chemical_compound, lcsh:Organic chemistry, medicine, Dehydration, sulfosuccinic acid, technology, industry, and agriculture, General Chemistry, medicine.disease, water permeation, poly(vinyl alcohol), Membrane, Chemical engineering, chemistry, Methanol, Swelling, medicine.symptom, chemical and thermal crosslinking
Abstract

The novel poly(vinyl alcohol) (PVA)-based membranes were prepared using the two-step crosslinking approach: the chemical crosslinking of PVA using sulfosuccinic acid (SSA) (0&ndash, 50 wt.%) and the thermal treatment (120&ndash, 160 &deg, C). The membrane composition and crosslinking temperature were optimized in terms of the mechanical and transport properties. The FTIR-ATR analysis revealed that the increase of the SSA concentration and crosslinking temperature resulted in the rise of the ester bond bands intensity due to the esterification reaction between PVA and SSA. As a consequence, the PVA-based membrane with 50 wt % SSA and crosslinked at 140 &deg, C showed the reduced Young&rsquo, s modulus (from 1266.2 MPa to 1.4 MPa) and elongation at break (from 316% to 66%) in comparison with the pure PVA membrane. The studied swelling behavior of the obtained membranes revealed significantly higher water sorption than that in methanol and propal-2-ol whatever the crosslinking temperature. The performed studies provide a new way of tailoring the membrane physicochemical properties, in particular, the surface hydrophilicity. In addition, the obtained results are crucial for the design and elaboration of the polymer membranes for the pervaporative separation of the liquid-liquid mixtures, in particular, for the alcohol dehydration.

Published
2019
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24. Water molecular state in 1-hexylpyridinium hexafluorophosphate: Water mean cluster size as a function of water concentration

Author

Dominique Langevin, Stéphane Marais, Kateryna Fatyeyeva, Corinne Chappey, Abdellatif Dahi, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), and Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Tetrafluoroborate, Water activity, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, chemistry.chemical_compound, Hexafluorophosphate, Materials Chemistry, Physical and Theoretical Chemistry, Spectroscopy, ComputingMilieux_MISCELLANEOUS, Hydrogen bond, Sorption, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 6. Clean water, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Ionic liquid, Gravimetric analysis, Physical chemistry, Pyridinium, 0210 nano-technology
Abstract

The water sorption behavior of representative pyridinium-based ionic liquid (IL), 1-hexylpyridinium hexafluorophosphate ([C6Py][PF6]), was studied over the whole range of the water activity a using a continuous gravimetric method. The analysis of the water sorption isotherm using the combination of a two-mode sorption (i.e. Henry-clustering) allowed to better understand [C6Py][PF6]-water interactions. At low and intermediate activity (a ≤ 0.8), the water molecules revealed a very low affinity to [C6Py][PF6] and, consequently, the water uptake was rather low. On the contrary, at high water activity (a > 0.8), the water uptake increased exponentially and the water clustering easily occurred. The constant of the Henry-clustering equation as well as the water clustering mechanism in [C6Py][PF6] were discussed and compared to those of imidazolium-based ILs: 1-hexyl-3-methylimidazolium hexafluorophosphate [C6C1im][PF6] (water-immiscible IL) and 1-butyl-3-methylimidazolium tetrafluoroborate [C4C1im][BF4] (water-miscible IL). It is shown that the sorption of water molecules by pyridinium-based ILs is controlled not only by the anion's nature, but also by the cation's nature. Moreover, the Zimm-Lundberg theory was used to determine the water mean cluster size (MCS) in [C6Py][PF6], [C6C1im][PF6] and [C4C1im][BF4]. The MCS results confirmed the strong capacity of water molecules to be aggregated in [C6Py][PF6]. In order to have a deeper insight into the water molecular state, infrared spectroscopy measurements were carried out as a function of the relative humidity value and the obtained results were correlated with the results of water sorption isotherms. It is found that at high water activity (a > 0.8), sorbed water molecules are strongly linked with ILs by hydrogen bonds and, therefore, are easily aggregated.

Published
2019
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25. Polymer inclusion membranes based on CTA/PBAT blend containing Aliquat 336 as extractant for removal of Cr(VI): Efficiency, stability and selectivity

Author

Stéphane Marais, Ferhat Sellami, Nicolas Couvrat, Kateryna Fatyeyeva, Ounissa Kebiche-Senhadji, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de procédés membranaires et de technique de séparation et de récupération (LPMSTR), Université A. Mira de Bejaia, Targa Ouzemmour 06000, Bejaia, Algeria, Sciences et Méthodes Séparatives (SMS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU), and Collaboration

Subjects
Polymers and Plastics, General Chemical Engineering, 02 engineering and technology, Aliquat 336, 010402 general chemistry, 01 natural sciences, Biochemistry, Chloride, Contact angle, chemistry.chemical_compound, Materials Chemistry, medicine, Environmental Chemistry, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Chemistry, General Chemistry, Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Cellulose triacetate, Membrane, [CHIM.POLY]Chemical Sciences/Polymers, Ionic liquid, 0210 nano-technology, Selectivity, Nuclear chemistry, medicine.drug
Abstract

Cellulose triacetate (CTA) and poly(butylene adipate-co-terephthalate) (PBAT)-based polymer inclusion membranes (PIMs) containing ionic liquid (tricaprylmethylammonium chloride (Aliquat 336)) as the carrier extractant were obtained for the facilitated and selective transport of Cr(VI) ions. The composition of PIMs was optimized in terms of the CTA/PBAT ratio. The obtained membranes were investigated using different techniques in order to show the influence of the membrane composition and the ionic liquid presence on the PIM resulting properties. The infrared analysis confirmed the presence of the intermolecular interactions of the hydroxyl groups of CTA with the carboxyl groups of PBAT and of the negatively charged carboxyl groups of CTA with the positively charged ammonium groups of Aliquat 336. The water contact angle measurements highlighted that the Aliquat 336 and PBAT presence modified the membrane hydrophobic/hydrophilic character. Moreover, it was shown that PIM containing the equivalent content of CTA and PBAT (35/35 wt%/wt%) with 30 wt% of Aliquat 336 revealed the optimized composition and was used for the Cr(VI) ions transport measurements. It was found that this PIM transported >99% of Cr(VI) in only 6 h and accumulated 120 h).

Published
2019
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26. Recent developments in the field of barrier and permeability properties of segmented polyurethane elastomers

Author

Kateryna Fatyeyeva, Malys Koun, Pascal Dubuis, Stéphane Marais, Aracelys Marcano, Marc Grimme, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Alten [Villeneuve d'Ascq], Alten, INOPROD, and Carmat SA

Subjects
Materials science, General Chemical Engineering, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Elastomer, 01 natural sciences, 0104 chemical sciences, Permeability (earth sciences), [CHIM.POLY]Chemical Sciences/Polymers, Composite material, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS, Segmented polyurethane
Abstract

Polyurethane (PU) elastomers represent an important class of segmented copolymers. Thanks to many available chemical compositions, a rather broad range of chemical, physical, and biocompatible properties of PU can be obtained. These polymers are often characterized by high tensile and tear strength, elongation, fatigue life, and wear resistance. However, their relatively high permeability towards gases and water as well as their biocompatibility still limits the PU’s practical application, especially for biomedical use, for example, in implants and medical devices. In this review, the barrier and permeability properties of segmented PUs related to their chemical structure and physical and chemical properties have been discussed, including the latest developments and different approaches to improve the PU barrier properties.

Published
2019
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27. Impact of water and thermal induced crystallizations in a PC/MXD6 multilayer film on barrier properties

Author

Cyrille Sollogoub, Valerie Gaucher, Nicolas Delpouve, Nadège Follain, Guillaume Miquelard-Garnier, Tiphaine Messin, Corinne Chappey, Stéphane Marais, Alain Guinault, Polymères Biopolymères Surfaces (PBS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Isolement, structure, transformations et synthèse de substances naturelles (ISTSSN), Université de Reims Champagne-Ardenne (URCA)-Centre National de la Recherche Scientifique (CNRS), Procédés et Ingénierie en Mécanique et Matériaux [Paris] (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM)-École Nationale Supérieure d'Arts et Métiers (ENSAM), Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM)-Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM)-Centre National de la Recherche Scientifique (CNRS), Groupe de physique des matériaux (GPM), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU), Unité Matériaux et Transformations - UMR 8207 (UMET), Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Institut National de la Recherche Agronomique (INRA), École Nationale Supérieure d'Arts et Métiers (ENSAM), HESAM Université (HESAM)-HESAM Université (HESAM)-Centre National de la Recherche Scientifique (CNRS)-Conservatoire National des Arts et Métiers [CNAM] (CNAM), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Procédés et Ingénierie en Mécanique et Matériaux (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-Centre National de la Recherche Scientifique (CNRS)-Arts et Métiers Sciences et Technologies, HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Institut National de la Recherche Agronomique (INRA)-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Conservatoire National des Arts et Métiers [CNAM] (CNAM)-Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), and Institut de Chimie du CNRS (INC)-Institut National de la Recherche Agronomique (INRA)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)

Subjects
Materials science, Polymers and Plastics, General Physics and Astronomy, chemistry.chemical_element, 02 engineering and technology, Adipamide, Sciences de l'ingénieur, 010402 general chemistry, 01 natural sciences, Oxygen, law.invention, Crystallinity, chemistry.chemical_compound, [SPI]Engineering Sciences [physics], law, Thermal, Materials Chemistry, Crystallization, Composite material, Polycarbonate, Organic Chemistry, 021001 nanoscience & nanotechnology, Nitrogen, 0104 chemical sciences, chemistry, 13. Climate action, visual_art, visual_art.visual_art_medium, Water of crystallization, 0210 nano-technology
Abstract

International audience; A multilayer film composed of alternating layers of polycarbonate (PC) and poly(m-xylene adipamide) (MXD6) was elaborated by using an innovative multilayer coextrusion process. Quasi-continuous thin MXD6 layers (nanolayers) alternating with PC layers were successfully obtained. The PC/MXD6 multilayer film showed a confining effect of MXD6 exerted by PC layers leading to an improvement of barrier properties despite a low degree of crystallinity (X c < 10 wt%). In order to further improve the barrier performances, crystallization treatments induced by water and by heating were then applied on the multilayer film and allowed reaching around 30 wt% of crystallinity in MXD6 layers. To decouple crystallization and geometrical constraint effects on the barrier properties in the multilayer films, the two treatments were also applied on MXD6 films. Surprisingly, despite an increase of the degree of crystallinity from 6 to 26%, water crystallization did not permit to improve gas barrier performances of the MXD6 film nor into the PC/MXD6 multilayer film. On the other hand, thermal crystallization of MXD6 in the multilayer film seems to be a more efficient route to strongly decrease the gas and moisture permeability, up to 75% for nitrogen, 58% for oxygen, 84% for carbon dioxide and 43% for water.

Published
2019
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28. Dimethylketene-based aliphatic polyketones: Copolymers and star-shaped polymers potentially useful in food packaging

Author

Fabrice Burel, Stéphane Marais, Hanbin Wang, Nadège Follain, Nicolas Desilles, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), and Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
chemistry.chemical_classification, Materials science, Polymers and Plastics, Organic Chemistry, Cationic polymerization, General Physics and Astronomy, 02 engineering and technology, Polymer, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Food packaging, Oxygen permeability, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Polyketone, Polymer chemistry, Materials Chemistry, Copolymer, Degradation (geology), Fourier transform infrared spectroscopy, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

This paper aims to design new aliphatic polyketones based on dimethylketene, by cationic polymerization. Previous works showed that the polyketone type of polydimethylketene presents excellent oxygen barrier properties even in the presence of humidity, enabling this material to compete with the polymers currently used in the food packaging industry. However, PDMK has a degradation temperature close to its melting temperature which may make processability uneasy. PDMK structure is thus modified to broaden the gap between these two temperatures: for the first time, a dimethylketene/ethylketene random copolymer and a star-shaped polydimethylketene are targeted by cationic polymerization. The obtained polymers are studied by 1H and 13C NMR, FTIR, and capillary viscosimetry, the thermal properties are more particularly analyzed by TGA and DSC, and the oxygen permeability is measured.

Published
2016
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29. Effect of the polar–nonpolar liquid mixtures on pervaporative behavior of perfluorinated sulfonic membranes in lithium form

Author

Edyta Rynkowska, Wojciech Kujawski, Joanna Kujawa, Anne-Marie Kelterer, Larisa Karpenko-Jereb, Kateryna Fatyeyeva, Stéphane Marais, Corinne Chappey, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Nicolaus Copernicus University, Faculty of Chemistry, Nicolaus Copernicus University [Toruń], and Graz University of Technology [Graz] (TU Graz)

Subjects
Methyl acetate, Analytical chemistry, Solvation, Filtration and Separation, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Biochemistry, Dissociation (chemistry), 0104 chemical sciences, chemistry.chemical_compound, [CHIM.POLY]Chemical Sciences/Polymers, Membrane, chemistry, Nafion, Organic chemistry, General Materials Science, Pervaporation, Methanol, Physical and Theoretical Chemistry, Dimethyl carbonate, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

Two ion-exchange membranes possessing perfluorinated backbone and sulfonic groups (i.e. Nafion ® 120 and IonClad™ R4010) with lithium(I) counter-ions were investigated. The interactions between solvents of different polarity and the ion-exchange membranes with various morphologies were taken into account in order to better understand solvation and dissociation phenomena of the ion-pairs. Pervaporation of polar (i.e. water, methanol)–nonpolar (i.e. methyl acetate, dimethyl carbonate) liquid mixtures was carried out. It was revealed that the increase of the polar component concentration above 2 wt% in the feed mixture leads to dissociation of ion-pairs in Nafion membrane, which is reflected by the rapid increase of the polar component partial flux. In the case of IonClad membrane the dissociation of the ion-pairs during pervaporation was observed only when water was a polar feed component. The dissociation of ion-pairs was also evidenced in infrared study by observing the shift of symmetric stretching vibrations (ν s ) bands of sulfonic groups to the lower wavenumbers, compared to the membrane in the dry state. The symmetric stretching vibrations (ν s ) bands of the dry Nafion membrane and membrane solvated with water and methanol were equal to 1071 cm −1 , 1058 cm −1 , and 1054 cm −1 , respectively. In the case of IonClad membrane the symmetric stretching vibration (ν s ) bands changed in contact with water from 1047 cm −1 (dry membrane) to 1037 cm −1 . The dissociation of the ion-pairs did not occur in IonClad membrane equilibrated with methanol, which is also consistent with the result obtained during pervaporation.

Published
2016
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30. Poly[(butylene succinate)-co-(butylene adipate)]-Montmorillonite Nanocomposites Prepared by Water-Assisted Extrusion: Role of the Dispersion Level and of the Structure-Microstructure on the Enhanced Barrier Properties

Author

Jérémie Soulestin, Stéphane Marais, Nadège Follain, Eric Dargent, Sébastien Charlon, Michel Sclavons, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d’Etude et de Caractérisation des Amorphes et des Polymères (AMME-LECAP EA 4528 International Laboratory), Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA), Département Technologie des Polymères et Composites & Ingénierie Mécanique (TPCIM), École des Mines de Douai (Mines Douai EMD), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-Ministère de l'Economie, des Finances et de l'Industrie, Institut Mines-Télécom [Paris] (IMT), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), and Université Catholique de Louvain = Catholic University of Louvain (UCL)

Subjects
Materials science, Nanocomposite, Composite number, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Microstructure, 01 natural sciences, Exfoliation joint, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Polybutylene succinate, chemistry.chemical_compound, General Energy, Montmorillonite, chemistry, Chemical engineering, Adipate, Polymer chemistry, Extrusion, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], Physical and Theoretical Chemistry, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

Composite films composed of a biodegradable poly[(butylene succinate)-co-(butylene adipate)] (PBSA) matrix with several contents (2.5; 5; 7.5; 10 wt %) of native (MMT) or organo-modified montmorillonite (OMMT) were successfully extruded using an innovative water-assisted extrusion process. As expected, better dispersion and exfoliation levels of nanofillers were obtained in PBSA+OMMT than in PBSA+MMT composite films, whatever the nanofiller content. Otherwise, the water-assisted extrusion process has also clearly enhanced the dispersion and exfoliation levels of native montmorillonite. This process was particularly efficient to delaminate and to disperse high amounts (≥5 wt %) of MMT in the PBSA matrix, which has highly increased tortuosity effects in the resulting composite films. The films prepared via the water-assisted extrusion have consequently exhibited better barrier properties to water and to gases than the films classically extruded and as the nanofiller content increases.

Published
2016
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31. Enhanced removal of Cr(VI) by polymer inclusion membrane based on poly(vinylidene fluoride) and Aliquat 336

Author

Ferhat Sellami, Laurent Colasse, Stéphane Marais, Ounissa Kebiche-Senhadji, Kateryna Fatyeyeva, Université Abderrahmane Mira [Béjaïa], Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), and Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
chemistry.chemical_classification, Facilitated diffusion, Metal ions in aqueous solution, Inorganic chemistry, Plasticizer, Filtration and Separation, 02 engineering and technology, Polymer, Aliquat 336, 021001 nanoscience & nanotechnology, Acceptor, Analytical Chemistry, chemistry.chemical_compound, Membrane, 020401 chemical engineering, chemistry, [CHIM]Chemical Sciences, 0204 chemical engineering, 0210 nano-technology, Fluoride
Abstract

New polymer inclusion membranes (PIMs) based on poly(vinylidene fluoride) (PVDF) (polymer matrix), tricaprylmethylammonium chloride (Aliquat 336) (ion carrier) and 2-nitrophenyloctylether (2NPOE) (plasticizer) were successfully elaborated by casting evaporation method and used in selectively facilitated transport of Cr(VI) ions in an acidic aqueous medium. Obtained PIMs are dense and homogeneous and are characterized by intermolecular interactions of the membrane components (i.e. polymer matrix, ion carrier and plasticizer). The presence of ion carrier and plasticizer enhances the membrane flexibility and its hydrophilic character. The decrease of the PVDF melting point is ascribed to the strong electrostatic interactions between liquid compounds (i.e. ion carrier and plasticizer) and polymer chains. PVDF-based PIM with only 20 wt% of Aliquat 336 ensures almost complete transport of Cr(VI) ions from the donor to acceptor phase. Moreover, the addition of 5 wt% of plasticizer significantly increases the transport flux. Also, Cr(VI) ions are selectively recovered (~97%) from a mixture containing other heavy metal ions (Cd(II), Pb(II), Fe(III), Zn(II), Cu(II), Ni(II), Co(II)) with such PIM. Elaborated PVDF-based PIMs reveal improved transport properties compared to other polymer-based PIMs, exhibiting high stability (more than 190 h) and lifetime durability and so they are suitable for long term application.

Published
2020
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32. Biodegradable PLA/PBS multinanolayer membrane with enhanced barrier performances

Author

Nadège Follain, Nicolas Delpouve, Valerie Gaucher, Cyrille Sollogoub, Tiphaine Messin, Stéphane Marais, Alain Guinault, Polymères Biopolymères Surfaces (PBS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Procédés et Ingénierie en Mécanique et Matériaux (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-Centre National de la Recherche Scientifique (CNRS)-Arts et Métiers Sciences et Technologies, HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM), Unité Matériaux et Transformations - UMR 8207 (UMET), Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), Groupe de physique des matériaux (GPM), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Conservatoire National des Arts et Métiers [CNAM] (CNAM)-Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Centrale Lille Institut (CLIL), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Procédés et Ingénierie en Mécanique et Matériaux [Paris] (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM)-École Nationale Supérieure d'Arts et Métiers (ENSAM), Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM)-Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM)-Centre National de la Recherche Scientifique (CNRS), Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), and Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université de Rouen Normandie (UNIROUEN)

Subjects
Matériaux [Sciences de l'ingénieur], Materials science, Diffusion, Filtration and Separation, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biochemistry, [SPI.MAT]Engineering Sciences [physics]/Materials, Crystallinity, Coextrusion, poly(butylene succinate), General Materials Science, Physical and Theoretical Chemistry, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Barrier properties, Thin layers, [CHIM.MATE]Chemical Sciences/Material chemistry, Polymer, Multilayer film, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Polybutylene succinate, Polyester, Membrane, chemistry, Chemical engineering, Barrier properties - Coextrusion - Multilayer film - poly(butylene succinate) - poly(lactic acid), Extrusion, poly(lactic acid), 0210 nano-technology
Abstract

International audience; Polyester multilayer membranes with more than 2000 alternating layers of poly(lactic acid) (PLA) and poly(butylene succinate) (PBS) were successfully prepared via a nanolayer coextrusion process equipped with a multiplying-element device. This process allows to make films consisting of very thin layers of polymers and in which a confinement effect of the semicrystalline polymer can be induced at point to significantly improve its physical properties. In this work, a homogeneous multinanolayer film of PLA/PBS was obtained without defaults or delamination, while the two polymers are immiscible. Continuous and homogeneous ultrathin layers of PBS (~45 nm) were obtained and the resulting confined structure of PBS led to an improvement of its barrier performances until 30% for oxygen, 40% for water and 70% for carbon dioxide. This improvement was explained by a decrease of the solubility coefficient and surprisingly not by the diffusion coefficient. This result was attributed to a slight orientation of the crystals in the extrusion direction and to the probable presence of an interphase between the layers of PLA and PBS.

Published
2020
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33. Tunable gas barrier properties of filled-PCL film by forming percolating cellulose network

Author

Julien Bras, Alain Dufresne, Sabrina Belbekhouche, Stéphane Marais, Corinne Chappey, Nadège Follain, Gilberto Siqueira, Polymères Biopolymères Surfaces (PBS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie et des Matériaux Paris-Est (ICMPE), Institut de Chimie du CNRS (INC)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Génie des procédés papetiers (LGP2 ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), and Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Gas permeation, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Nanocellulose, Nanocomposites, Percolating network, [SPI.MAT]Engineering Sciences [physics]/Materials, chemistry.chemical_compound, Crystallinity, [SPI]Engineering Sciences [physics], Colloid and Surface Chemistry, Phase (matter), [CHIM]Chemical Sciences, Cellulose, Nanocomposite, Gas diffusion, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, [CHIM.POLY]Chemical Sciences/Polymers, Chemical engineering, chemistry, Nanocrystal, 0210 nano-technology, Caprolactone
Abstract

International audience; Herein, a three-dimensional percolating cellulose nanocrystal network has been successfully entangled into a poly(caprolactone) (PCL) film to prepare fully biodegradable bio-nanocomposites. To strongly assembly the reinforcing dense cellulose phase and PCL chains and limit the incompatibility effect, the cellulose surface was chemically modified using a long-chain isocyanate as grafting agent. Structural effects are highlighted through gas transport examination using several diffusing probes. A peculiar and unexpected behavior is evidenced: both permeability and diffusivity increased, whereas solubility is reduced, compared to the unfilled PCL film. One can suspect that the formation of the reinforcing cellulose network and its anchoring to PCL chains are the cause of structural defects facilitating the gas transfer localized in interfacial regions. The resulting structure of the film plays a main role on gas barrier performances compared to the change in crystallinity and tortuosity effect induced by rod-like nanoparticles.

Published
2018
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34. Vapour sorption and permeation behaviour of supported ionic liquid membranes: application for organic solvent/water separation

Author

Kateryna Fatyeyeva, Sergiy Rogalsky, Oksana Tarasyuk, Corinne Chappey, Stéphane Marais, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Institute of Bioorganic Chemistry and Petrochemistry, and National Academy of Sciences of Ukraine (NASU)

Subjects
Polymers and Plastics, Cyclohexane, General Chemical Engineering, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biochemistry, chemistry.chemical_compound, Materials Chemistry, Non-random two-liquid model, Environmental Chemistry, Thermal stability, Alkyl, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Chemistry, Sorption, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, Permeation, 021001 nanoscience & nanotechnology, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Membrane, [CHIM.POLY]Chemical Sciences/Polymers, Chemical engineering, Ionic liquid, 0210 nano-technology
Abstract

The imidazolium-based ionic liquids (ILs) (1-n-alkyl-3-methylimidazolium tetrafluoroborate, where n = 4, 6–8, 12) were synthesized and characterized in terms of their spectral characteristics, thermal stability, and water, ethanol and cyclohexane vapour sorption behaviour. It was found that the highest hydrophilic character had IL with the shortest alkyl chain on the cation. At the same time, the IL thermal stability was decreased with the increase of the cation alkyl chain length. D'Arcy and Watt and NRTL sorption models allowed to well describe the vapour sorption experimental data. The supported ionic liquid membranes (SILMs) were prepared by impregnation of the porous poly(vinylidene fluoride) (PVDF) membrane with the synthesized ILs. The sorption capacity of PVDF was found to increase after its swelling in IL. An experimental evaluation of the SILMs permeability was carried out for water, ethanol and cyclohexane. The effect of operation parameters such as temperature and concentration of the permeant was studied. It was observed that the presence of the IL strongly influenced the permeability performance of the membrane by reducing the pore sizes and changing the hydrophobic/hydrophilic balance. It is found from the permeation kinetics curves that the SILMs have high potential for separation of organic solvent/water mixtures.

Published
2018
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35. Gas Transport Through Polymer/Clay Nanocomposites

Author

Stéphane Marais and Nadège Follain

Subjects
Materials science, Nanocomposite, Polymer nanocomposite, Sorption, Permeation, engineering.material, Thermal diffusivity, Polymer clay, symbols.namesake, symbols, engineering, van der Waals force, Composite material, Solubility
Abstract

This chapter introduces gas transport properties exhibited by polymer nanocomposite films. It starts by presenting a little review of elaboration methods of nanocomposite films. It is thereafter mentioned the filler morphology within a thermoplastic matrix obtained depending on the filler dispersion level, on the filler origin, on the filler surface-chemical modification, and on filler/matrix compatibility. The influence of the filler morphology on gas transport properties of the resulting hybrid films and the role played by filler/matrix interfacial regions is then examined. By the end of the chapter, the nanocomposite structure/gas transport performances relationships are explained through permeation kinetics, the choice of gas diffusing species (differing in Van der Waals molar volumes), and the corresponding parameters such as gas permeability, diffusivity, and solubility. The permeation parameter rankings for the nanocomposite films as a function of gas molecules are featured to be compatible with Van Krevelen's statements.

Published
2018
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36. Improvement of barrier properties of bio-based polyester nanocomposite membranes by water-assisted extrusion

Author

Jérémie Soulestin, Nadège Follain, Sébastien Charlon, Eric Dargent, Michel Sclavons, Stéphane Marais, Corinne Chappey, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d’Etude et de Caractérisation des Amorphes et des Polymères (AMME-LECAP EA 4528 International Laboratory), Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA), Département Technologie des Polymères et Composites & Ingénierie Mécanique (TPCIM), École des Mines de Douai (Mines Douai EMD), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-Ministère de l'Economie, des Finances et de l'Industrie, and Université Catholique de Louvain = Catholic University of Louvain (UCL)

Subjects
Materials science, Plastics extrusion, Filtration and Separation, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biochemistry, Polymer chemistry, General Materials Science, Thermal stability, Physical and Theoretical Chemistry, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Nanocomposite, [CHIM.MATE]Chemical Sciences/Material chemistry, Polymer, 021001 nanoscience & nanotechnology, Exfoliation joint, 0104 chemical sciences, [CHIM.POLY]Chemical Sciences/Polymers, Membrane, Chemical engineering, chemistry, Extrusion, 0210 nano-technology, Dispersion (chemistry)
Abstract

Hybrid membranes made of a biopolymer matrix poly(butylene succinate) (PBS) or poly(butylene succinate-co-butylene adipate) (PBSA) loaded with 5 wt% of native (CNa) or organo-modified (C30B) montmorillonites were successfully extruded using new extrusion conditions where liquid water was introduced into the extruder barrel to improve the nanofiller dispersion and exfoliation levels. The C30B incorporation in both matrices leads to the degradation of polymer chains and the reduction of the thermal stability while the CNa introduction combined with the water injection presents no effect on the polymer molecular weight and the thermal stability. The water-assisted extrusion process enables the increase in CNa dispersion and exfoliation levels in both matrices, which improves barrier properties to gases and water by tortuosity effects. In the case of C30B, the positive effect of dispersion induced by water injection was much less pronounced since C30B particles were already well dispersed and exfoliated in both matrices. The use of the water injection at high pressure during the extrusion process was found really efficient for native montmorillonite and so appears as a promising process for dispersing hydrophilic particles in polymers having a low hydrophilic character, without preliminary chemical modification of the fillers.

Published
2015
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37. Multifunctional hydrolyzed EVA membranes with tunable microstructure and water barrier properties

Author

Eric Dargent, Kateryna Fatyeyeva, Stéphane Marais, Jorge Arturo Soto Puente, Polymères Biopolymères Surfaces (PBS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Groupe de physique des matériaux (GPM), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), and Normandie Université (NU)

Subjects
Vinyl alcohol, Water transport, Materials science, Filtration and Separation, Sorption, [CHIM.MATE]Chemical Sciences/Material chemistry, Microstructure, Biochemistry, [SPI]Engineering Sciences [physics], chemistry.chemical_compound, Crystallinity, [CHIM.POLY]Chemical Sciences/Polymers, Membrane, chemistry, Chemical engineering, 13. Climate action, Desorption, Polymer chemistry, Vinyl acetate, [CHIM]Chemical Sciences, General Materials Science, Physical and Theoretical Chemistry, ComputingMilieux_MISCELLANEOUS
Abstract

A new functional membrane based on poly(ethylene- co -vinyl acetate) (EVA) and poly(ethylene- co -vinyl alcohol) (EVOH) was obtained by hydrolysis reaction on both surfaces of an EVA film, and as a result a three-layered structure (EVOH/EVA/EVOH) was formed. The chemical modification of the film and the thickness of hydrolyzed layer were controlled by FTIR and fluorescent microscopy measurements, respectively. The influence of the hydrolysis time ( t h ) on the thermal properties and membrane microstructure, studied by thermal analysis and X-ray diffraction measurements, indicated the evolution from the amorphous state to the semicrystalline one. The impact of the microstructure modification on the water transport properties was evaluated by permeability and sorption measurements. The plasticization effect of the three-layered membrane was found to be 2 times higher than that in the case of the completely hydrolyzed membrane ( t h >72 h). Such behavior was related to the amorphous/crystalline state of EVOH in the membrane. The results of water sorption measurements indicated that the water desorption is delayed at the highest temperatures in the case of the three-layered membranes. A strong correlation between the water properties of the hydrolyzed EVA membranes and the EVOH structure was observed. In addition, to providing details on structural characteristics of the three-layered multifunctional membrane with tunable water barrier properties, some possible applications where controlled moisture is necessary (such as food packaging or proton exchange fuel cell membrane) were discussed.

Published
2015
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38. Designing Biodegradable PHA-Based 3D Scaffolds with Antibiofilm Properties for Wound Dressings: Optimization of the Microstructure/Nanostructure

Author

Jean Marc Valleton, Naila Bou Haidar, Aracelys Marcano, Stéphane Marais, A.C. Duncan, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), and Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Nanostructure, Biomedical Engineering, 02 engineering and technology, [SDV.BC]Life Sciences [q-bio]/Cellular Biology, 010402 general chemistry, 01 natural sciences, Biomaterials, Polymer chemistry, medicine, Dispersin B, [SDV.IB.BIO]Life Sciences [q-bio]/Bioengineering/Biomaterials, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Polyvinylpyrrolidone, Substrate (chemistry), Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Microstructure, 0104 chemical sciences, Solvent, Membrane, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Chemical engineering, [SDV.IB]Life Sciences [q-bio]/Bioengineering, 0210 nano-technology, medicine.drug
Abstract

One major factor inhibiting natural wound-healing processes is infection through bacterial biofilms, particularly in the case of chronic wounds. In this study, the micro/nanostructure of a wound dressing was optimized in order to obtain a more efficient antibiofilm protein-release profile for biofilm inhibition and/or detachment. A 3D substrate was developed with asymmetric polyhydroxyalkanoate (PHA) membranes to entrap Dispersin B (DB), the antibiofilm protein. The membranes were prepared using wet-induced phase separation (WIPS). By modulating the concentration and the molecular weight of the porogen polymer, polyvinylpyrrolidone (PVP), asymmetric membranes with controlled porosity were obtained. PVP was added at 10, 30, and 50% w/w, relative to the total polymer concentration. The physical and kinetic properties of the quaternary nonsolvent/solvent/PHA/PVP systems were studied and correlated with the membrane structures obtained. The results show that at high molecular weight (Mw = 360 kDa) and high PV...

Published
2017
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39. Sulfonic Membrane Sorption and Permeation Properties: Complementary Approaches to Select a Membrane for Pervaporation

Author

Wojciech Kujawski, Larisa Karpenko-Jereb, Anne-Marie Kelterer, Edyta Rynkowska, Stéphane Marais, Corinne Chappey, Kateryna Fatyeyeva, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Nicolaus Copernicus University, Faculty of Chemistry, Nicolaus Copernicus University [Toruń], and Graz University of Technology [Graz] (TU Graz)

Subjects
Chemistry, Inorganic chemistry, Membrane structure, Sorption, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, Permeation, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Dissociation (chemistry), 0104 chemical sciences, Surfaces, Coatings and Films, chemistry.chemical_compound, [CHIM.POLY]Chemical Sciences/Polymers, Membrane, Materials Chemistry, Semipermeable membrane, Pervaporation, Methanol, Physical and Theoretical Chemistry, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

In this contribution, the physical and chemical properties of the dense sulfonic membrane IonClad R4010 in the lithium form were studied to evaluate its potential application in pervaporation. To develop new membrane materials, it is necessary to know the influence of the membrane structure on the membrane equilibrium and transport properties. For this purpose, the sorption and permeation measurements of water and methanol in the liquid and vapor states were performed and correlated to the ion pairs/solvent interactions analyzed by the infrared spectroscopy. The IonClad R4010 equilibrium and transport properties were found to be quite different depending on the permeant nature. The sorption and diffusion behavior of water and methanol was well described by means of the type II sorption model (BET theory). The swelling capacity of the IonClad R4010 membrane in methanol was found to be much lower than that in liquid water. In contrast to methanol, the total dissociation of the ion pairs in the IonClad R4010 membrane was obtained in the presence of water but only at high activity (∼0.8). Besides, the dispersion of the water molecules in the membrane was found to be homogeneous. The infrared spectroscopy results revealed that the methanol molecules had weaker interactions with the sulfonic groups of IonClad R4010 in agreement with the sorption data. The permeation properties were investigated by means of the sweeping gas and gravimetric methods in order to evaluate the membrane performance for pervaporation. The permeation results are in accordance with those obtained by sorption, thus confirming the complementariness of the two approaches.

Published
2017
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40. Physicochemical properties and biological activities of novel blend films using oxidized pectin/chitosan

Author

Meriem Elkolli, Nadège Follain, Stéphane Marais, Didier Le Cerf, Mahmoud Bounekhel, Asma Chetouani, Djafer Benachour, Christophe Rihouey, Université Ferhat-Abbas Sétif 1 [Sétif] (UFAS1), Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), and Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
food.ingredient, Chemical Phenomena, Biocompatibility, Pectin, Size-exclusion chromatography, 02 engineering and technology, macromolecular substances, 010402 general chemistry, Hemolysis, 01 natural sciences, Biochemistry, Chitosan, Biomaterials, chemistry.chemical_compound, food, Differential scanning calorimetry, Structural Biology, Oxidation, Humans, Organic chemistry, Molecular Biology, Schiff Bases, Sodium periodate, Periodate, General Medicine, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Haemolysis, Anti-Bacterial Agents, 0104 chemical sciences, Molecular Weight, carbohydrates (lipids), [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Pectins, Antibacterial activity, Blood compatibility, 0210 nano-technology, Oxidation-Reduction, Nuclear chemistry
Abstract

International audience; Pectin has been widely used in a variety of biomedical applications. In this study, it was modified with sodium periodate as an oxidant and characterized by physicochemical methods Periodate oxidation increased the contents of dialdehyde units and carboxyl groups in pectin, and a decrease in pectin viscosity was measured. The oxidization reaction led to a significant decrease in all values of molecular weight and size (Mn, Mw, [η] and Rh) as determined by size exclusion chromatography (SEC), which allowed the selection of the oxidized pectin to be added to chitosan. Chitosan-based films were characterized by infra-red spectroscopy (FTIR), X-ray diffractometry (XRD), and differential scanning calorimetry (DSC) measurements. Thermal behaviour studies demonstrated that interactions existed between chitosan and oxidized pectin. The haemolysis percentages of films were found to be less than 5%, which indicated their good blood compatibility. Finally, the antibacterial activity was clearly improved. Cross-linking reactions between pectin and chitosan through ionic bonds and amide bonds and between chitosan and oxidized pectin through Schiff base formation were evidenced, which opens the way to extend applications of these polysaccharides; notably, the biocompatibility and biodegradability of these new networks is convenient for pharmaceutical, biomedical or cosmetic applications.

Published
2017
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41. Confinement effect in PC/MXD6 multilayer films: Impact of the microlayered structure on water and gas barrier properties

Author

Nadège Follain, Guillaume Miquelard-Garnier, Stéphane Marais, Alain Guinault, Cyrille Sollogoub, Valerie Gaucher, Nicolas Delpouve, Tiphaine Messin, Polymères Biopolymères Surfaces (PBS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Procédés et Ingénierie en Mécanique et Matériaux [Paris] (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM)-École Nationale Supérieure d'Arts et Métiers (ENSAM), Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM)-Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM)-Centre National de la Recherche Scientifique (CNRS), Normandie Université (NU), Unité Matériaux et Transformations - UMR 8207 (UMET), Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Institut National de la Recherche Agronomique (INRA), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Procédés et Ingénierie en Mécanique et Matériaux (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM)-Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM), Institut de Chimie du CNRS (INC)-Institut National de la Recherche Agronomique (INRA)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL), Institut National de la Recherche Agronomique (INRA)-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-Centre National de la Recherche Scientifique (CNRS)-Arts et Métiers Sciences et Technologies, and HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)

Subjects
Confined structure, Matériaux [Sciences de l'ingénieur], Chemical substance, Filtration and Separation, 02 engineering and technology, 010402 general chemistry, poly(m-xylene adipamide), 01 natural sciences, Biochemistry, Permeability, [SPI.MAT]Engineering Sciences [physics]/Materials, Crystallinity, Multilayer, General Materials Science, Physical and Theoretical Chemistry, Polycarbonate, Barrier properties, Mécanique [Sciences de l'ingénieur], Chemistry, Permeation, [SPI.MECA]Engineering Sciences [physics]/Mechanics [physics.med-ph], 021001 nanoscience & nanotechnology, 0104 chemical sciences, Amorphous solid, Polycarbonate, poly(m-xylene adipamide), Membrane, Chemical engineering, Permeability (electromagnetism), visual_art, visual_art.visual_art_medium, 0210 nano-technology, Science, technology and society
Abstract

Films of PC and MXD6 were prepared via multilayer coextrusion. Films presenting stretched nodules/lamellas of MXD6 in the PC matrix, and films with quasi-continuous thin MXD6 layers alternating with PC layers were obtained. The transport properties were specifically investigated from water and gas permeation kinetics, and the corresponding permeation parameters were determined. The confinement effect of MXD6 in the multilayer structure was highlighted by comparing the permeability predicted from the series model equation with the experimental data. Although the MXD6 layers were not homogeneous and continuous for all membranes, water and gas permeabilities of the PC/MXD6 multilayer film were largely reduced. Such improvement of barrier properties was related to the change of the MXD6 structure, considering that the confinement of the MXD6 layers induced by PC layers allowed to bring chain orientation and to reduce the chain segment mobility in the MXD6 amorphous constrained zones. In addition, in the case of a PC/MXD6 multilayer structure well defined with continuous layers and relatively homogeneous thicknesses, the degree of crystallinity was slightly increased.

Published
2017
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42. Layered Poly(ethylene- co -vinyl acetate)/Poly(ethylene- co -vinyl alcohol) Membranes with Enhanced Water Separation Selectivity and Performance

Author

Eric Dargent, Kateryna Fatyeyeva, Corinne Chappey, Stéphane Marais, J. A. Soto Puente, Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d’Etude et de Caractérisation des Amorphes et des Polymères (AMME-LECAP EA 4528 International Laboratory), Université de Rouen Normandie (UNIROUEN), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)

Subjects
Vinyl alcohol, Materials science, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Hydrolysis, chemistry.chemical_compound, Crystallinity, Polymer chemistry, otorhinolaryngologic diseases, Vinyl acetate, General Materials Science, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, Permeation, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Membrane, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], sense organs, 0210 nano-technology, Selectivity
Abstract

A three-layered membrane based on poly(ethylene-co-vinyl acetate) (EVA) and hydrolyzed EVA–poly(ethylene-co-vinyl alcohol) (EVOH), was elaborated by the surface hydrolysis of a dense EVA membrane. Because of the chemical modifications, the three-layered EVOH/EVA/EVOH membrane was characterized by the particular microstructure (amorphous EVA and semicrystalline EVOH) and the tunable hydrophilic/hydrophobic balance. Also, these modifications led to the membrane with the selective barrier properties compared with the pure EVA and completely hydrolyzed EVOH membranes. The water barrier behavior was related to the strong hydrogen-bond interactions of water and vinyl alcohol groups, whereas the weak chemical interactions were revealed for gases (N2 and O2). Furthermore, the influence of the polymer rubbery or glassy state on the permeation kinetics was established. In the case of the three-layered membrane, the considerably high selectivity values were obtained for H2O/O2 (∼11 900) and H2O/N2 (∼48 000) at 25 °C...

Published
2017
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43. Structure and Barrier Properties of Multinanolayered Biodegradable PLA/PBSA Films: Confinement Effect via Forced Assembly Coextrusion

Author

Nicolas Delpouve, Cyrille Sollogoub, Valerie Gaucher, Stéphane Marais, Alain Guinault, Nadège Follain, Tiphaine Messin, Polymères Biopolymères Surfaces (PBS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Procédés et Ingénierie en Mécanique et Matériaux [Paris] (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM)-École Nationale Supérieure d'Arts et Métiers (ENSAM), Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM)-Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM)-Centre National de la Recherche Scientifique (CNRS), Unité Matériaux et Transformations - UMR 8207 (UMET), Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Institut National de la Recherche Agronomique (INRA), Groupe de physique des matériaux (GPM), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU), Institut National de la Recherche Agronomique (INRA)-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Procédés et Ingénierie en Mécanique et Matériaux (PIMM), Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-Centre National de la Recherche Scientifique (CNRS)-Arts et Métiers Sciences et Technologies, HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM), Institut National de la Recherche Agronomique (INRA)-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Conservatoire National des Arts et Métiers [CNAM] (CNAM)-Arts et Métiers Sciences et Technologies, HESAM Université (HESAM)-HESAM Université (HESAM), Institut de Chimie du CNRS (INC)-Institut National de la Recherche Agronomique (INRA)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN)

Subjects
Matériaux [Sciences de l'ingénieur], Materials science, multilayer polymer film, Diffusion, barrier properties, 02 engineering and technology, coextrusion, 010402 general chemistry, 01 natural sciences, [SPI.MAT]Engineering Sciences [physics]/Materials, Crystallinity, General Materials Science, poly(butylene succinate-co-butylene adipate), Composite material, chemistry.chemical_classification, Mécanique [Sciences de l'ingénieur], confined crystallization, Polymer, Permeation, [SPI.MECA]Engineering Sciences [physics]/Mechanics [physics.med-ph], 021001 nanoscience & nanotechnology, Microstructure, 0104 chemical sciences, Amorphous solid, Polyester, chemistry, multilayer polymer film, coextrusion, confined crystallization, permeability, poly(lactic acid), poly(butylene succinate-co-butylene adipate), barrier properties, poly(lactic acid), permeability, 0210 nano-technology, Layer (electronics)
Abstract

International audience; Multilayer coextrusion processing was applied to produce 2049-layer film of poly(butylene succinate-co-butylene adipate) (PBSA) confined against poly(lactic acid) (PLA) using forced assembly, where the PBSA layer thickness was about 60 nm. This unique technology allowed to process semicrystalline PBSA as confined polymer and amorphous PLA as confining polymer in a continuous manner. The continuity of PBSA layers within the 80/20 wt % PLA/PBSA layered films was clearly evidenced by atomic force microscopy (AFM). Similar thermal events to the reference films were revealed by thermal studies; indicating no diffusion of polymers during the melt-processing. Mechanical properties were measured for the multilayer film and the obtained results were those expected considering the fraction of each polymer, revealing the absence of delamination in the PLA/PBSA multinanolayer film. The confinement effect induced by PLA led to a slight orientation of the crystals, an increase of the rigid amorphous fraction (RAF) in PBSA with a densification of this fraction without changing film crystallinity. These structural changes allowed to strongly improve the water vapor and gas barrier properties of the PBSA layer into the multilayer film up to two decades in the case of CO2 gas. By confining the PBSA structure in very thin and continuous layers, it was then possible to improve the barrier performances of a biodegradable system and the resulting barrier properties were successfully correlated to the effect of confinement on the microstructure and the chain segment mobility of the amorphous phase. Such investigation on these multinanolayers of PLA/PBSA with the aim of evidencing relationships between microstructure implying RAF and barrier performances has never been performed yet. Besides, gas and water permeation results have shown that the barrier improvement obtained from the multilayer was mainly due to the reduction of solubility linked to the reduction of the free volume while the tortuosity effect, as usually expected, was not really observed. This work brings new insights in the field of physicochemical behaviors of new multilayer films made of biodegradable polyesters but also in interfacial processes due to the confinement effect induced in these multinanolayer structures obtained by the forced assembly coextrusion. This original coextrusion process was a very advantageous technique to produce eco-friendly materials with functional properties without the help of tie layer, additives, solvents, surface treatments, or inorganic fillers.

Published
2017
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44. List of Contributors

Author

Ahmad Allahbakhsh, Cecilia I. Alvarez Igarzabal, Ana Vera Alves Machado, Marina Patricia Arrieta, Gabriela B. Baldino, Silvia E. Barbosa, Nuria Burgos, Luciana A. Castillo, Corinne Chappey, Cintia B. Contreras, Viviane Dalmoro, Ana M. Díez-Pascual, Tungalag Dong, Karolth Espinosa, Kateryna Fatyeyeva, Emmanuel Flores-Huicochea, Esther García-Serna, Isabel Gonçalves de Moura, Agustín González, Tatjana Haramina, Tina Harifi, Alfonso Jiménez, José María Kenny, Alain Largeteau, Daniel López, Juan López, Ana Sofia Lemos Machado Abreu, Giulio Malucelli, Stéphane Marais, Ana Cristina Mellinas, Pawan Kumar Mishra, Katarzyna Mitura, Majid Montazer, Aleksandra R. Nesic, Luciane Oliveira, Shweta Pandey, Laura Peponi, Marcia Pires, Mythili Prakasam, J. Rodolfo Rendón-Villalobos, Iva Rezić, Tonči Rezić, Francisco Rodríguez-González, Sanja I. Seslija, Harshita Sharma, Adriane Simanke, Javier Solorza-Feria, Iman Soltani, Richard J. Spontak, Miriam C. Strumia, Sushama Talegaonkar, Arsénio Vasconcelos de Sá, Rupert Wimmer, Konrad Wyre˛bski, Xueyan Yun, Paweł K. Zarzycki, and Joao Henrique Zimnoch dos Santos

Published
2017
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45. Biopolymer/clay nanocomposites as the high barrier packaging material: recent advances

Author

Kateryna Fatyeyeva, Corinne Chappey, and Stéphane Marais

Subjects
Flexibility (engineering), Nanocomposite, Materials science, Moisture, Food industry, business.industry, Active packaging, Nanotechnology, 02 engineering and technology, engineering.material, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Durability, 0104 chemical sciences, Food packaging, engineering, Biopolymer, 0210 nano-technology, business
Abstract

Food nanotechnology is an area of new possibilities for the food industry, which is of great interest nowadays. The main trends of the nanotechnology application and functionality in developing food packaging include: the improvement of plastic material barriers, the introduction of the active components that can deliver additional functional attributes compared to the conventional active packaging, and the sensing and indication of relevant information. The main problem is extending the shelf life of packed products, preserving all organoleptic characteristics for as long as possible. Therefore, the high barrier materials (in particular it applies to oxygen, carbon dioxide, flavor compounds, and water vapor) are required to be used in the food packaging. Owing to the combination of the physical and morphological properties, the introduction of nanofillers into biopolymers is a promising strategy to overcome some critical issues, such as poor water resistivity and low mechanical properties. Thus, this chapter reviews different types of edible and biodegradable biobased nanocomposites with special emphasis on the advantages of nanotechnology application for improving the barrier properties of the polymer matrices. These properties include rigidity, stiffness or flexibility, durability, temperature and moisture stability, and the barrier properties against water, oxygen, and other gases.

Published
2017
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46. Water Sorption Behavior in Different Aromatic Ionomer Composites Analyzed with a 'New Dual-Mode Sorption' Model

Author

Yongli Li, Quang T. Nguyen, Kateryna Fatyeyeva, and Stéphane Marais

Subjects
chemistry.chemical_classification, Ketone, Polymers and Plastics, Organic Chemistry, Sorption, Ether, complex mixtures, Inorganic Chemistry, chemistry.chemical_compound, Hysteresis, Solvation shell, chemistry, Materials Chemistry, Molecule, Composite material, Ionomer, Water vapor
Abstract

A new dual-mode sorption model (NDMS) was applied to sigmoid-shaped isotherms of water vapor sorption in composites of sulfonated or nonsulfonated polysulfones with a sulfonic-modified laponite clay and in blends of sulfonated poly(ether ether ketone) with sulfonated polyether sulfone cardo, respectively. The three NDMS parameters, Cp, A′, and k′ can be correlated to the amount of water molecules sorbed in the first hydration shell, the subsequent sorption on the sulfonic-sites and the tendency for water molecules to form clusters at very high water activities, respectively. The fitted values were used to study the relationship between sorption behaviors and component structure or organization in the composites. The analysis of the sorption–desorption cycles shows that the sorption hysteresis increases with the ionomer chain rigidity. An analytical expression for the mean cluster size (MCS) as a function of activity was deduced and validated by correlating to sorption kinetics. It has been shown that MCS ...

Published
2014
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47. Polyimide/ionic liquid composite membranes for fuel cells operating at high temperatures

Author

Sergiy Rogalsky, Dominique Langevin, Stéphane Marais, Corinne Chappey, Kateryna Fatyeyeva, Abdellatif Dahi, and Oksana Tarasyuk

Subjects
Materials science, General Chemical Engineering, Proton exchange membrane fuel cell, Electrolyte, Conductivity, Dielectric spectroscopy, chemistry.chemical_compound, Membrane, chemistry, Chemical engineering, Nafion, Ionic liquid, Electrochemistry, Organic chemistry, Ionic conductivity
Abstract

Supported ionic liquid membranes (SILMs) were prepared by impregnating a porous Matrimid ® membrane with protic room-temperature ionic liquids (RTILs): 1-n-methylimidazolium dibutylphosphate ([C 1 im][DBP]), 1-n-butylimidazolium dibutylphosphate ([C 4 im][DBP]) and 1-n-butylimidazolium bis(2-ethylhexyl)phosphate ([C 4 im][BEHP]). After immersion of the porous Matrimid ® membrane in each RTIL, the prepared SILMs were composed of 53 ± 3% of RTIL phase. The control of the full impregnation of the porous Matrimid ® membrane by the RTILs was verified by FTIR spectroscopy. From the bubble point test, the SILMs displayed a good retention of their RTIL phase and, thus, showed a good stability against the increased pressure on one of the faces. The ionic conductivity of SILMs, used as electrolyte membranes for proton exchange membrane fuel cell (PEMFC) was measured by impedance spectroscopy. Unlike the Nafion ® , the conductivity of the SILMs still increases at high temperatures (> 80 °C). The [C 4 im][DBP]-impregnated SILM showed the best result in terms of conductivity (2.0 10 −2 S/cm at 115 °C). Moreover, all SILMs showed satisfactory stability since they retained a large amount of the RTIL phase in the membrane pores.

Published
2014
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48. Supported ionic liquid membranes for water and volatile organic compounds separation: Sorption and permeation properties

Author

Dominique Langevin, Stéphane Marais, Oksana Tarasyuk, Abdellatif Dahi, Kateryna Fatyeyeva, Corinne Chappey, Sergiy Rogalsky, and Amel Benamor

Subjects
Materials science, Cyclohexane, Filtration and Separation, Sorption, Permeation, Biochemistry, chemistry.chemical_compound, Membrane, chemistry, Chemical engineering, Phase (matter), Ionic liquid, Organic chemistry, General Materials Science, Bubble point, Physical and Theoretical Chemistry, Phase inversion
Abstract

Supported ionic liquid membranes (SILMs) were prepared by immobilizing the room temperature ionic liquids (RTILs) ([C4C1im][BF4] and [CnC1im][PF6] (n=4 and 6)) in a porous Matrimid membrane. The Matrimid membrane was prepared by water vapor-induced phase inversion, and its porous structure was characterized by SEM. After immersion of the porous Matrimid membrane in RTILs, the prepared SILMs were composed of 60% of RTIL phase. From the bubble point test, the SILMs displayed an excellent retention of their RTIL phase, and thus showed a good stability in the face of increased pressure on one of their faces. The feasibility of the prepared SILMs for the separation of water and volatile organic compounds (VOCs) such as ethanol and cyclohexane by vapor permeation was investigated. For this purpose, a preliminary study of water and VOC vapor sorption in RTILs was necessary to determine the affinity between each solute and RTILs. Only [C4C1im][BF4] showed both the best sorption capacities and the good sorption selectivities. The vapor permeation measurements were therefore carried out only through the SILMs impregnated with [C4C1im][BF4]. The SILM permeability was found to increase in the same sorption affinity order as for [C4C1im][BF4], i.e. cyclohexane

Published
2014
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49. Structure and Barrier Properties of Biodegradable Polyhydroxyalkanoate Films

Author

Nadège Follain, Frédéric Chivrac, Eric Dargent, Corinne Chappey, Raphaël Crétois, Stéphane Marais, Polymères, biopolymères, membranes (PBM), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU), Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d’Etude et de Caractérisation des Amorphes et des Polymères (AMME-LECAP EA 4528 International Laboratory), Université de Rouen Normandie (UNIROUEN), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)

Subjects
Materials science, Diffusion, Plasticizer, Sorption, Permeation, Thermal diffusivity, Polyhydroxyalkanoates, [SPI.MAT]Engineering Sciences [physics]/Materials, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, [SPI]Engineering Sciences [physics], Crystallinity, [CHIM.POLY]Chemical Sciences/Polymers, General Energy, Chemical engineering, [CHIM]Chemical Sciences, Organic chemistry, Physical and Theoretical Chemistry, ComputingMilieux_MISCELLANEOUS, Water vapor
Abstract

The water vapor sorption and permeation to water and gas molecules of films prepared from industrially available polyhydroxyalkanoates (PHAs) were analyzed in detail. Two film-forming processes were compared through their transport properties. The presence of additives, which can alter the barrier properties of films, was highlighted in some commercial-grade PHAs by investigating the physicochemical properties of these films. The water vapor sorption results were simulated using the appropriate Park model, highlighting the moisture resistance, the entrance of water molecules into films, and the impact of the process used and were then discussed through the analysis of diffusion coefficients. A significant reduction in water permeability was evidenced with the increase of degree of crystallinity of the biopolyesters. Water diffusivity was found to be dependent on water concentration and this was due to the plasticization effect induced by water molecules. In terms of gas permeation, a singular behavior pec...

Published
2014
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50. Effect of cold plasma treatment on surface properties and gas permeability of polyimide films

Author

Corinne Chappey, Stéphane Marais, Dominique Langevin, Abdellatif Dahi, Jean-Marc Valleton, Kateryna Fatyeyeva, and Fabienne Poncin-Epaillard

Subjects
chemistry.chemical_classification, Materials science, General Chemical Engineering, Analytical chemistry, General Chemistry, Surface finish, Plasma, Polymer, Permeation, Contact angle, X-ray photoelectron spectroscopy, chemistry, Surface modification, Polyimide
Abstract

The surface functionalization of polyimide (Matrimid® 5218) films was carried out by cold plasma treatment with CF4, N2 and O2 gases using a radio frequency discharge and the optimum plasma conditions were evaluated by water contact angle measurements. The surface hydrophobicity of polyimide films was obtained after CF4 plasma treatment, while O2 and N2 plasma treatments contributed to the hydrophilic surface functionalization. X-ray photoelectron spectroscopy (XPS) results revealed the presence of CFx, amino or oxygen-containing groups attached to the polyimide film surface depending on the treatment gas. A strong influence of the used plasma gas on the film roughness was determined by atomic force microscopy (AFM) measurements. The influence of the surface modification on CO2, N2 and O2 gas permeation through the plasma treated films was evaluated. The permeation behaviour was characterized in terms of transport parameters, namely, coefficients of permeability, diffusion and solubility. The permeability coefficient of all plasma treated polyimide films for the studied gases (CO2, N2 and O2) was found to decrease following the order of increasing the kinetic molecular diameter of the penetrant gas. Besides, the selectivity coefficient was found to be significantly increased after the plasma treatments – αCO2/N2 was increased up to 36% and 98% for O2 and N2 plasma treated Matrimid® 5218 films, respectively. The relationship between the gas permeation behaviour and the surface modification of polymer film by cold plasma was discussed.

Published
2014
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