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1. In Situ Infrared and UV–Vis Ellipsometries to Probe The Varnish Ageing and Swelling of G. Bellini 'Transfiguration'

Author

Hélène Pasco, Arnaud Lesaine, Angela Cerasuolo, Cédric Boissière, Philippe Walter, Clément Sanchez, Laurence deViguerie, and Marco Faustini

Subjects
environmental ellipsometry, solvent, swelling, varnish, Physics, QC1-999, Technology
Abstract

Abstract Varnish layers are optical coatings that act as physico‐chemical barrier between the historical paint layers and the environment. Understanding how varnish materials protect historical paintings over time and in the presence of humidity or organic vapors is of central importance for art preservation. However, probing the behavior of varnish after aging in real conditions remains a challenge. Here the question is addressed by “reshaping” the varnish material from the masterpiece of G. Bellini, the “Transfiguration”, into an optical layer; coupling in situ Ultraviolet‐Visible (UV–vis) and Infrared (IR) ellipsometries, the chemical state is correlated, optical properties and swelling of the varnish in presence of water and organic vapors. It shows that the varnish material aged since the 1950s still exhibits effective water repellence. The methodology may be applied to other relevant historical systems beyond paintings and may help in establishing more efficient preservation strategies for historical artworks.

Published
2024
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2. Investigating the impact of chemical structures on the photocatalytic degradation rates over ZnO nanorods: An oxidative pathways perspective

Author

Elie A. Daher, Cédric Boissière, Christel Laberty Robert, and Wael Hamd

Subjects
ZnO Nanorods, Photocatalysis, Organic pollutants, Molecular structures, Degradation rate, Pseudo-first order, Chemistry, QD1-999
Abstract

Zinc oxide (ZnO) nanorods were coated on glass substrates and used as photocatalysts to evaluate the kinetic behavior of three different aromatic structures: i) single aromatic ring (phenol), ii) poly-aromatic ring (methylene blue), and iii) complex macromolecule (humic acid). The kinetics of all the tested molecules obey a pseudo-first-order model regardless of their initial concentrations. The apparent rate constants are largely controlled by the bond dissociation energy and the number of oxidation steps in each organic molecule. For instance, methylene blue presents the weakest dissociation bond energy and the highest degradation rate constant compared to humic acid and phenol.

Published
2023
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3. Revealing the Dependency of Dye Adsorption and Photocatalytic Activity of ZnO Nanoparticles on Their Morphology and Defect States

Author

Yuri Hendrix, Erwan Rauwel, Keshav Nagpal, Ryma Haddad, Elias Estephan, Cédric Boissière, and Protima Rauwel

Subjects
nanoparticles, ZnO, green photocatalysis, surface defects, ROS, Chemistry, QD1-999
Abstract

ZnO is an effective photocatalyst applied to the degradation of organic dyes in aqueous media. In this study, the UV-light and sunlight-driven photocatalytic activities of ZnO nanoparticles are evaluated. A handheld Lovibond photometer was purposefully calibrated in order to monitor the dye removal in outdoor conditions. The effect of ZnO defect states, i.e., the presence of zinc and oxygen defects on the photocatalytic activity was probed for two types of dyes: fuchsin and methylene blue. Three morphologies of ZnO nanoparticles were deliberately selected, i.e., spherical, facetted and a mix of spherical and facetted, ascertained via transmission electron microscopy. Aqueous and non-aqueous sol-gel routes were applied to their synthesis in order to tailor their size, morphology and defect states. Raman spectroscopy demonstrated that the spherical nanoparticles contained a high amount of oxygen vacancies and zinc interstitials. Photoluminescence spectroscopy revealed that the facetted nanoparticles harbored zinc vacancies in addition to oxygen vacancies. A mechanism for dye degradation based on the possible surface defects in facetted nanoparticles is proposed in this work. The reusability of these nanoparticles for five cycles of dye degradation was also analyzed. More specifically, facetted ZnO nanoparticles tend to exhibit higher efficiencies and reusability than spherical nanoparticles.

Published
2023
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4. The origin of the high electrochemical activity of pseudo-amorphous iridium oxides

Author

Marine Elmaalouf, Mateusz Odziomek, Silvia Duran, Maxime Gayrard, Mounib Bahri, Cédric Tard, Andrea Zitolo, Benedikt Lassalle-Kaiser, Jean-Yves Piquemal, Ovidiu Ersen, Cédric Boissière, Clément Sanchez, Marion Giraud, Marco Faustini, and Jennifer Peron

Subjects
Science
Abstract

The origins of the superior catalytic activity of poorly crystallized Ir-based oxide material for the OER in acid is still under debate. Here, authors synthesize porous IrMo oxides to deconvolute the effect of Ir oxidation state from short-range ordering and show the latter to be a key factor.

Published
2021
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5. Producing cold from heat with aluminum carboxylate-based metal-organic frameworks

Author

Effrosyni Gkaniatsou, Chaoben Chen, Frédéric S. Cui, Xiaowei Zhu, Paul Sapin, Farid Nouar, Cédric Boissière, Christos N. Markides, Jan Hensen, and Christian Serre

Subjects
metal-organic frameworks, sorption cooling, solar cooling, thermally driven, aluminum carboxylate, upscale synthesis, Physics, QC1-999
Abstract

Summary: Worldwide cooling energy demands will increase by four times by 2050. Thermally driven cooling technology is an alternative solution to electric heat pumps in removing hazardous refrigerants and harnessing renewables and waste heat. We highlight the advantages of water-stable microporous aluminum-carboxylate-based metal-organic frameworks, or Al-MOFs, as sorbents in the application of producing cold from heat. Here, we synthesize the Al-MOFs with green and scalable processes, which are prerequisites for exploring various industrial and civil applications. A proof-of-concept full-scale adsorption chiller with different Al-MOFs is built up with optimized configurations derived from various characterization techniques. The tested Al-MOFs achieve thermal efficiency above 0.6 and specific cooling power over 1 kW/kg in typical cooling scenarios. Notably, when solar thermal energy is used as the heat source in an outdoor validation, Al-MOFs are weather-resilient solutions that exhibit a stable energy conversion efficiency under fluctuating operating conditions (ambient temperature and solar irradiation).

Published
2022
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6. Preparations and Characterizations of Luminescent Two Dimensional Organic-inorganic Perovskite Semiconductors

Author

Sanjun Zhang, Pierre Audebert, Yi Wei, Antoine Al Choueiry, Gaëtan Lanty, Antoine Bréhier, Laurent Galmiche, Gilles Clavier, Cédric Boissière, Jean-Sébastien Lauret, and Emmanuelle Deleporte

Subjects
organic-inorganic perovskites, hybrid materials, multi-quantum wells, nanoparticles, spin coating, X-ray diffraction, absorption spectrum, photoluminescence, Technology, Electrical engineering. Electronics. Nuclear engineering, TK1-9971, Engineering (General). Civil engineering (General), TA1-2040, Microscopy, QH201-278.5, Descriptive and experimental mechanics, QC120-168.85
Abstract

This article reviews the synthesis, structural and optical characterizations of some novel luminescent two dimensional organic-inorganic perovskite (2DOIP) semiconductors. These 2DOIP semiconductors show a self-assembled nano-layered structure, having the electronic structure of multi-quantum wells. 2DOIP thin layers and nanoparticles have been prepared through different methods. The structures of the 2DOIP semiconductors are characterized by atomic force microscopy and X-ray diffraction. The optical properties of theb DOIP semiconductors are characterized from absorption and photoluminescence spectra measured at room and low temperatures. Influences of different components, in particular the organic parts, on the structural and optical properties of the 2DOIP semiconductors are discussed.

Published
2010
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7. Optical-Quality Thin Films with Tunable Thickness from Stable Colloidal Suspensions of Lanthanide Oxysulfide Nanoplates

Author

Léna Meyniel, Cédric Boissière, Natacha Krins, and Sophie Carenco

Subjects
Electrochemistry, General Materials Science, Surfaces and Interfaces, Condensed Matter Physics, Spectroscopy
Abstract

In modern laser technologies, there is a need for coatings that would be compatible with flexible substrates while retaining the advantages of inorganic compounds in terms of robustness. As a first step in this direction, we developed here thin films of lanthanide oxysulfide, of optical quality, prepared by low-temperature dip coating. As a model compound in the family of oxysulfides, (Gd,Ce)

Published
2022

9. High-Entropy-Alloy Nanocrystal Based Macro- and Mesoporous Materials

Author

Maria Letizia De Marco, Walid Baaziz, Sharmin Sharna, François Devred, Claude Poleunis, Alexandre Chevillot-Biraud, Sophie Nowak, Ryma Haddad, Mateusz Odziomek, Cédric Boissière, Damien P. Debecker, Ovidiu Ersen, Jennifer Peron, and Marco Faustini

Subjects
General Engineering, General Physics and Astronomy, General Materials Science
Abstract

High-entropy-alloy (HEA) nanoparticles are attractive for several applications in catalysis and energy. Great efforts are currently devoted to establish composition-property relationships to improve catalytic activity or selectivity. Equally importantly, developing practical fabrication methods for shaping HEA-based materials into complex architectures is a key requirement for their utilization in catalysis. However, shaping nano-HEAs into hierarchical structures avoiding demixing or collapse remains a great challenge. Herein, we overcome this issue by introducing a simple soft-chemistry route to fabricate ordered macro- and mesoporous materials based on HEA nanoparticles, with high surface area, thermal stability, and catalytic activity toward CO oxidation. The process is based on spray-drying from an aqueous solution containing five different noble metal precursors and polymer latex beads. Upon annealing, the polymer plays a double role: templating and reducing agent enabling formation of HEA nanoparticle-based porous networks at only 350 °C. The formation mechanism and the stability of the macro- and mesoporous materials were investigated by a set of

Published
2022

10. Revealing the Dependency of Dye Adsorption and Photocatalytic Activity of ZnO Nanoparticles on Their Morphology and Defect States

Author

Rauwel, Yuri Hendrix, Erwan Rauwel, Keshav Nagpal, Ryma Haddad, Elias Estephan, Cédric Boissière, and Protima

Subjects
nanoparticles, ZnO, green photocatalysis, surface defects, ROS
Abstract

ZnO is an effective photocatalyst applied to the degradation of organic dyes in aqueous media. In this study, the UV-light and sunlight-driven photocatalytic activities of ZnO nanoparticles are evaluated. A handheld Lovibond photometer was purposefully calibrated in order to monitor the dye removal in outdoor conditions. The effect of ZnO defect states, i.e., the presence of zinc and oxygen defects on the photocatalytic activity was probed for two types of dyes: fuchsin and methylene blue. Three morphologies of ZnO nanoparticles were deliberately selected, i.e., spherical, facetted and a mix of spherical and facetted, ascertained via transmission electron microscopy. Aqueous and non-aqueous sol-gel routes were applied to their synthesis in order to tailor their size, morphology and defect states. Raman spectroscopy demonstrated that the spherical nanoparticles contained a high amount of oxygen vacancies and zinc interstitials. Photoluminescence spectroscopy revealed that the facetted nanoparticles harbored zinc vacancies in addition to oxygen vacancies. A mechanism for dye degradation based on the possible surface defects in facetted nanoparticles is proposed in this work. The reusability of these nanoparticles for five cycles of dye degradation was also analyzed. More specifically, facetted ZnO nanoparticles tend to exhibit higher efficiencies and reusability than spherical nanoparticles.

Published
2023
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11. From waste incineration by-products to functional materials: a 'Chimie douce' route to VOCs mineral adsorbents

Author

Alexis Corbin, Lise Guichaoua, Hiva Baradari, Flavien Gueneau, Xavier Chaucherie, Bruno Gilardin, Thierry Gosset, Cédric Boissière, Lionel Nicole, and Clément Sanchez

Subjects
Biomaterials, Materials Chemistry, Ceramics and Composites, General Chemistry, Condensed Matter Physics, Electronic, Optical and Magnetic Materials
Abstract

One of today’s major world challenges is the accumulation and the storage of tens of millions of tons per year of final materials resulting from the incineration of domestic and industrial waste. This raises the question of the recycling of these “raw materials”, while making allowance for environmental, economic, social and public health aspects. Our strategy targets the incorporation of waste incineration by-products in a totally circular economy. We propose an innovative process combining templated sol–gel growth of an inorganic or hybrid silica-based network with a solubilized fraction of bottom ash coming from the combustion of industrial and household wastes. The resulting materials engineered via aerosol processing demonstrate maximum adsorption capacity of model pollutant compounds (1-2 dichlorobenzene) competitive with activated carbons currently used in modern incineration plants. We believe that they have the potential to replace conventional activated carbon commonly used in incineration plants, enabling the first step of the long road of recycling final waste.

Published
2022

12. Mind the gap! tailoring sol–gel ceramic mesoporous coatings on labile metal–organic frameworks through kinetic control

Author

Elisa Bindini, Marco Möller, Dorleta Otaegui, Tanja Lüdtke, Cédric Boissière, Sergio Moya, and Ryma Haddad

Subjects
Inorganic Chemistry, Materials science, Nanocomposite, Chemical engineering, Coating, engineering, Nanoparticle, Metal-organic framework, Mesoporous silica, engineering.material, Mesoporous material, Dissolution, Sol-gel
Abstract

Surface engineering of metal–organic frameworks (MOFs) with a mesoporous silica coating can improve MOF mechanical properties and provide an easy way to decorate MOF nanoparticles with organic or biological molecules though silane chemistry or electrostatic interactions, while retaining open access to MOF porosity. Silica coating would be highly beneficial for employing MOFs in a wide range of applications such as catalysis or drug delivery. However, obtaining a stable, controlled core–shell structure using MOF nanoparticles as seeds is challenging because of their intrinsic chemically labile nature. Here we analyze the factors that destabilize the core of the Zeolitic Imidazolate Framework-8 (ZIF-8) MOFs during the sol–gel deposition of a mesoporous silica shell causing a partial or total etching of the MOF material. Silicates in solution are found to scavenge Zn2+ ions removing them from the ZIF structure and causing a partial or complete dissolution of the ZIF seed. By carefully tuning the silicate concentration in solution simultaneous control can be obtained over both the ZIF-8 dissolution and the silica condensation kinetics, resulting in the growth of a uniform mesoporous silica shell while preserving the integrity of ZIF-8. The core–shell nanoparticles obtained show a compact core shell structure with no gap between the MOF core and the silica shell, even after calcination, while the crystalline ZIF-8 structure is retained. Overall, a general synthetic approach is presented for producing nanocomposite core–shell materials which can be applied to other MOF labile seeds to design new hierarchical materials.

Published
2022

13. In Operando Spectroscopic Ellipsometry Investigation of MOF Thin Films for the Selective Capture of Acetic Acid

Author

Sanchari Dasgupta, Subharanjan Biswas, Kevin Dedecker, Eddy Dumas, Nicolas Menguy, Bruno Berini, Bertrand Lavedrine, Christian Serre, Cédric Boissière, Nathalie Steunou, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Centre de Recherche sur la Conservation (CRC ), Muséum national d'Histoire naturelle (MNHN)-Ministère de la Culture et de la Communication (MCC)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and This work was supported by the Ecole Universitaire de recherche PSGS HCH Humanities, Creation, Heritage, Investissement d’Avenir ANR-17-EURE-0021 - Fondation des sciences du patrimoine. This work has been sponsored by the Ile-de-France Region in the framework of Respore, the Île-de-France network of Excellence in Porous Solids. The authors acknowledge Ali Saad for SEM experiments.

Subjects
Ellipsometry, adsorption, Thin films, [SDE]Environmental Sciences, [CHIM]Chemical Sciences, General Materials Science, Volatile organic compounds, MOFs
Abstract

International audience; The emission of polar volatile organic compounds (VOCs) is a major worldwide concern of air quality and equally impacts the preservation of cultural heritage (CH). The challenge is to design highly efficient adsorbents able to selectively capture traces of VOCs such as acetic acid (AA) in the presence of relative humidity (RH) normally found at storage in museums (40-80%). Although the selective capture of VOCs over water is still challenging, Metal-Organic Frameworks (MOFs) possess highly tunable features (Lewis, Bronsted or redox metal sites, functional groups, hydrophobicity…) suitable to selectively capture a large variety of VOCs. In this context, we have explored the adsorption efficiency of a series of MOFs thin films (ZIF-8(Zn), MIL-101(Cr) and UiO-66(Zr)-2CF3) for the selective capture of AA based on a UV/Vis and FT-IR spectroscopic ellip-sometry in operando study (2-6% of relative pressure of AA under 40% of RH), namely conditions close to the realistic envi-ronmental storage conditions of cultural artefacts. For that purpose, optical quality thin films of MOFs were prepared by dip-coating and their AA adsorption capacity and selectivity were evaluated under humid conditions by measuring the variation of the refractive index as a function of the vapor pressures while the chemical nature of the co-adsorbed analytes (water and AA) was identified by FT-IR ellipsometry. While thin films of ZIF-8(Zn) strongly degraded when exposed to AA/water va-pors, films of MIL-101(Cr) and UiO-66(Zr)-2CF3 present a high chemical stability under those conditions. It was shown that MIL-101(Cr) presents a high AA adsorption capacity due to its high pore volume, but exhibits a poor AA adsorption selectivi-ty under humid conditions. In contrast, UiO-66(Zr)-2CF3 was shown to overpass MIL-101(Cr) in terms of AA/ H2O adsorp-tion selectivity and AA adsorption/desorption cycling stability thanks to its high hydrophobic character, suitable pore size for adequate confinement and specific interactions.

Published
2023

14. Mind the Gap! Tailoring Sol-gel Ceramic Mesoporous Coatings on Labile Metal-organic Frameworks through Kinetic Control

Author

Marco Möller, Ryma Haddad, Dorleta Otaegui, Elisa Bindini, Cédric Boissière, Tanja Lüdtke, and Sergio Moya

Subjects
Nanocomposite, Materials science, Coating, Chemical engineering, engineering, Nanoparticle, Metal-organic framework, engineering.material, Mesoporous silica, Mesoporous material, Dissolution, Sol-gel
Abstract

Surface engineering of metal-organic frameworks (MOFs) with a mesoporous silica coating can improve MOF mechanical properties and provide an easy way to decorate MOF nanoparticles with organic or biological molecules though silane chemistry or electrostatic interactions, while retaining open access to MOF porosity. Silica coating would be highly beneficial for employing MOFs in a wide range of applications such as catalysis or drug delivery. However, obtaining a stable, controlled core-shell structure using MOF nanoparticles as seed is challenging because of their intrinsic chemically labile nature. Here we analyze the factors that destabilize the core of the Zeolitic Imidazolate Framework-8 (ZIF-8) MOFs during the sol-gel deposition of a mesoporous silica shell causing a partial or total etching of the MOF material. Silicates in solution are found to scavenge Zn2+ ions removing them from the ZIF structure and causing a partial or complete dissolution of the ZIF seed. By carefully tuning the silicate concentration in solution simultaneous control can be obtained over both the ZIF-8 dissolution and the silica condensation kinetics, resulting in the growth of a uniform mesoporous silica shell while preserving the integrity of ZIF-8. The core-shell nanoparticles obtained show a compact core shell structure with no gap between the MOF core and the silica shell, even after calcination, while the crystalline ZIF-8 structure is retained. Overall, a general synthetic approach is presented for producing nanocomposite core-shell materials which can be applied to other MOF labile seed to design new hierarchical materials.

Published
2021

15. Metal-Organic Framework Photonic Balls: Single Object Analysis for Local Thermal Probing

Author

Marco Faustini, Cédric Boissière, Civan Avci, Caroline Byun, Maria Letizia De Marco, Jonathan Perrin, Mario Scheel, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), and Centre National de la Recherche Scientifique (CNRS)

Subjects
Fabrication, Materials science, photonics, Physics::Optics, Nanotechnology, photothermal sensing, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Microscopy, Thermal, General Materials Science, spray-drying, Porosity, metal-organic frameworks, business.industry, Mechanical Engineering, [CHIM.MATE]Chemical Sciences/Material chemistry, Photothermal therapy, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Mechanics of Materials, Proof of concept, hyperspectral microscopy, Metal-organic framework, thermal probes, Photonics, 0210 nano-technology, business
Abstract

International audience; Due to their high porosity and chemical versatility, metal-organic frameworks (MOFs) exhibit physical properties appealing for photonic-based applications. While several MOF photonic structures have been reported, examples of applications thereof are mainly limited to chemical sensing. Herein, the range of application of photonic MOFs is extended to local thermal and photothermal sensing by integrating them into a new architecture: MOF photonic balls. Micrometric-sized photonic balls are made of monodispersed MOFs colloids that are self-assembled via spray-drying, a low-cost, green, and high-throughput method. The versatility of the process allows tuning the morphology and the composition of photonic balls made of several MOFs and composites with tailored optical properties. X-ray nanotomography and environmental hyperspectral microscopy enable analysis of single objects and their evolution in controlled atmosphere and temperature. Notably, in presence of vapors, the MOF photonic balls act as local, label-free temperature probes. Importantly, compared to other thermal probes, the temperature detection range of these materials can be adjusted "on-demand." As proof of concept, the photonic balls are used to determine local temperature profiles around a concentrated laser beam. More broadly, this work is expected to stimulate new research on the physical properties of photonic MOFs providing new possibilities for device fabrication.

Published
2021

16. The origin of the high electrochemical activity of pseudo-amorphous iridium oxides

Author

Cédric Boissière, Marine Elmaalouf, Clément Sanchez, Mounib Bahri, Jean-Yves Piquemal, Mateusz Odziomek, Andrea Zitolo, Ovidiu Ersen, Benedikt Lassalle-Kaiser, Maxime Gayrard, Marion Giraud, Silvia Duran, Jennifer Peron, Marco Faustini, Cédric Tard, HAL-SU, Gestionnaire, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de chimie moléculaire (LCM), École polytechnique (X)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Novel Advanced Nano-Objects (LCMCP-NANO), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique

Subjects
[CHIM.INOR] Chemical Sciences/Inorganic chemistry, Materials science, Science, General Physics and Astronomy, chemistry.chemical_element, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, Electrocatalyst, 01 natural sciences, Article, General Biochemistry, Genetics and Molecular Biology, law.invention, X-ray photoelectron spectroscopy, law, Oxidation state, Porous materials, Calcination, Iridium, Crystallization, [CHIM.MATE] Chemical Sciences/Material chemistry, Energy, Multidisciplinary, Structural properties, 010405 organic chemistry, Oxygen evolution, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, 0104 chemical sciences, Amorphous solid, Chemical engineering, chemistry, 13. Climate action, Nanoparticles, Electrocatalysis
Abstract

Combining high activity and stability, iridium oxide remains the gold standard material for the oxygen evolution reaction in acidic medium for green hydrogen production. The reasons for the higher electroactivity of amorphous iridium oxides compared to their crystalline counterpart is still the matter of an intense debate in the literature and, a comprehensive understanding is needed to optimize its use and allow for the development of water electrolysis. By producing iridium-based mixed oxides using aerosol, we are able to decouple the electronic processes from the structural transformation, i.e. Ir oxidation from IrO2 crystallization, occurring upon calcination. Full characterization using in situ and ex situ X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction and transmission electron microscopy allows to unambiguously attribute their high electrochemical activity to structural features and rules out the iridium oxidation state as a critical parameter. This study indicates that short-range ordering, corresponding to sub-2nm crystal size for our samples, drives the activity independently of the initial oxidation state and composition of the calcined iridium oxides., The origins of the superior catalytic activity of poorly crystallized Ir-based oxide material for the OER in acid is still under debate. Here, authors synthesize porous IrMo oxides to deconvolute the effect of Ir oxidation state from short-range ordering and show the latter to be a key factor.

Published
2021

17. Atomic Layer Deposition of Titania in Ordered Mesoporous Cerium Zirconium Oxide Thin Films: A Case Study

Author

Herbert Over, Andreas Beyer, Bernd M. Smarsly, Kerstin Volz, M. Göttlicher, Cédric Boissière, C. Becker, Pascal Cop, and Jörg Schörmann

Subjects
Anatase, Materials science, chemistry.chemical_element, 02 engineering and technology, Porosimetry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Atomic layer deposition, Cerium, General Energy, Chemical engineering, chemistry, Physical and Theoretical Chemistry, Thin film, 0210 nano-technology, Mesoporous material, High-resolution transmission electron microscopy, Layer (electronics)
Abstract

A strategy is presented to deposit defined layers of TiO2 onto the pore surface within ordered mesoporous, crystalline CeO2-ZrO2 thin films using atomic layer deposition (ALD). As structure-directing agent, a special diblock copolymer, poly(isobutylene)-block-poly(ethylene oxide), was used, resulting in a three-dimensional arrangement of spherical pores with diameter around 13 nm. High resolution transmission electron microscopy investigations evidence the presence of anatase TiO2 coatings within the mesopores, while ellipsometric porosimetry studies together with time-of-flight secondary-ion mass spectrometry depth profiles indicate the deposition inside the mesopores up to 50 ALD cycles. Afterward, the interconnecting channels between the mesopores are filled completely prohibiting further transport of the gaseous TiO2 precursor into the ordered structure of mesopores and hence, limit the layer growth on the surfaces of the pores. Therefore, the size of the mesopores and their connections are decisive w...

Published
2019

18. Biomimetic Tough Gels with Weak Bonds Unravel the Role of Collagen from Fibril to Suprafibrillar Self‐Assembly

Author

Alba Marcellan, Julie Brun, Biravena Raveendranathan, Nadine Nassif, Francisco M. Fernandes, Milena Lama, Cédric Boissière, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Sciences et Ingénierie de la Matière Molle (UMR 7615) (SIMM), Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut Universitaire de France (IUF), and Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.)

Subjects
collagen, biomimetism, Toughness, Materials science, Polymers and Plastics, Swine, microstructure, Bioengineering, 02 engineering and technology, 010402 general chemistry, Fibril, 01 natural sciences, Collagen Type I, Cornea, Biomaterials, Tissue engineering, Biomimetic Materials, Elastic Modulus, Tensile Strength, Ultimate tensile strength, Materials Chemistry, Stress relaxation, Animals, Humans, Cyclic loading, [PHYS]Physics [physics], Tissue Engineering, self-assembly, 021001 nanoscience & nanotechnology, gels, 0104 chemical sciences, Biophysics, mechanical behavior, Stress, Mechanical, Self-assembly, 0210 nano-technology, Type I collagen, Biotechnology
Abstract

International audience; Biological tissues rich in type I collagen exhibit specific hierarchical fibrillar structures together with remarkable mechanical toughness. However, the role of collagen alone in their mechanical response at different structural levels is not fully understood. Here, it is proposed to rationalize such challenging interplay from a materials science perspective through the subtle control of this protein self-assembly in vitro. It is relied on a spray-processing approach to readily use the collagen phase diagram and set a palette of biomimetic self-assembled collagen gels in terms of suprafibrillar organization. Their mechanical responses unveil the involvement of mechanisms occurring either at fibrillar or suprafibrillar scales. Noticeably, both modulus at early stage of deformations and tensile toughness probe the suprafibrillar organization, while durability under cyclic loading and stress relaxation reflect mechanisms at the fibril level. By changing the physicochemical environment, the interfibrillar interactions are modified toward more biomimetic mechanical responses. The possibility of making tissue-like materials with versatile compositions and toughness opens perspectives in tissue engineering.

Published
2021

19. Replacing Metals with Oxides in Metal-Assisted Chemical Etching Enables Direct Fabrication of Silicon Nanowires by Solution Processing

Author

Justine Voronkoff, Cédric Boissière, Marco Faustini, Andrea Cattoni, Maxime Gayrard, David Montero, Laurence Rozes, Jennifer Peron, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut des matériaux de Paris-Centre (IMPC), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre de Nanosciences et de Nanotechnologies (C2N), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)

Subjects
Sol-Gel, Fabrication, Materials science, Bioengineering, Nanotechnology, 02 engineering and technology, Electrocatalyst, Nanofabrication, Nanoimprint lithography, law.invention, law, Etching (microfabrication), General Materials Science, Nanoimprint, Lithography, Sol-gel, Mechanical Engineering, Block-copolymer, Oxides, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Isotropic etching, Nanolithography, Assisted Chemical Etching, 0210 nano-technology
Abstract

International audience; Metal-Assisted Chemical Etching (MACE) has emerged as effective method to fabricate high aspect ratio nanostructures. This method requires a catalytic mask that is generally composed by a metal. Here, we challenge the general view that the catalyst needs to be metal by introducing Oxide-assisted Chemical Etching (OACE). We perform etching with metal oxides such as RuO 2 and IrO 2 , by transposing materials used in electrocatalysis to nanofabrication. These oxides can be solution-processed as polymers exhibiting similar capabilities of metals for MACE. Nanopatterned oxides can be obtained by direct nanoimprint lithography or blockcopolymer lithography from chemical solution on large scale. High aspect ratio silicon nanostructures were obtained at the sub-20 nm scale exclusively by cost-effective solution processing by halving the number of fabrication steps compared to MACE. More in general, OACE is expected to stimulate new fundamental research on chemical etching assisted by other materials providing new possibilities for device fabrication.

Published
2021

20. Nanoconfined water vapour as a probe to evaluate plasmonic heating

Author

Marco Faustini, Corinne Chanéac, Zeinab Chehadi, Cédric Boissière, Lebanese University [Beirut] (LU), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Plasmonic nanoparticles, Phase transition, Materials science, Nanoporous, Nanotechnology, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, Photothermal therapy, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Thermal, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], General Materials Science, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], 0210 nano-technology, Nanoscopic scale, ComputingMilieux_MISCELLANEOUS, Plasmon, Water vapor
Abstract

Engineering photothermal effects in plasmonic materials is of paramount importance for many applications, such as cancer therapy, chemical synthesis, cold catalysis and, more recently, metasurfaces. The evaluation of plasmonic heating at the nanoscale is challenging and generally requires sophisticated equipments and/or temperature-sensitive probes such as fluorescent molecules or materials. Here, we propose to use water vapor as a probe to evaluate the local heating around plasmonic nanoparticles. We demonstrate the concept for the case of a plasmonic colloidal film characterized by bi-modal nanoporosity. In particular, we exploit the thermal and light water liquid–vapor phase transitions taking place in the nanoporous medium that can be triggered by external stimuli, such as heating or irradiation, to obtain structural and optical variations in the film. The local temperature is then estimated using spectroscopic ellipsometry data acquired by a multimodal chamber. More generally, this method offers a simple and general approach to determine the local temperature that only requires a nanoporous material and water vapor, such as environmental humidity. In addition, this approach can be further generalized to other materials, vapor molecules or optical techniques.

Published
2020

21. Following in Situ the Degradation of Mesoporous Silica in Biorelevant Conditions: At Last, a Good Comprehension of the Structure Influence

Author

Zeinab Chehadi, Corinne Chanéac, David Grosso, Omar Azzaroni, Clément Sanchez, Cédric Boissière, Pierre-Antoine Albouy, Marco Faustini, Andrea Cattoni, Elisa Bindini, Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre de Nanosciences et de Nanotechnologies (C2N), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Solides (LPS), Institut des Matériaux, de Microélectronique et des Nanosciences de Provence (IM2NP), Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas [La Plata] (INIFTA), Facultad de Ciencias Exactas [La Plata], Universidad Nacional de la Plata [Argentine] (UNLP)-Universidad Nacional de la Plata [Argentine] (UNLP), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Aix Marseille Université (AMU)-Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS), and Novel Advanced Nano-Objects (LCMCP-NANO)

Subjects
In situ, Materials science, Nanoparticle, Nanotechnology, 02 engineering and technology, therapeutic vectors, 010402 general chemistry, 01 natural sciences, dissolution kinetic, Drug Delivery Systems, Ellipsometry, [CHIM]Chemical Sciences, Humans, General Materials Science, mesoporous silica, Porosity, Drug Carriers, High loading, Proteins, Mesoporous silica, 021001 nanoscience & nanotechnology, Silicon Dioxide, 0104 chemical sciences, Drug Liberation, Kinetics, Drug delivery, Degradation (geology), Nanoparticles, 0210 nano-technology, protein, ellipsometry
Abstract

International audience; Mesoporous silica nanoparticles (MSNs) have seen a fast development as drug delivery carriers thanks to their tunable porosity and high loading capacity. The employ of MSNs in biomedical applications requires a good understanding of their degradation behavior both to control drug release and to assess possible toxicity issues on human health. In this work, we study mesoporous silica degradation in biologically relevant conditions through in situ ellipsometry on model mesoporous nanoparticle or continuous thin films, in buffer solution and in media containing proteins. In order to shed light on the structure/dissolution relationship, we performed dissolution experiments far from soluble silicate species saturation. Via a complete decorrelation of dissolution and diffusion contributions, we proved unambiguously that surface area of silica vectors is the main parameter influencing dissolution kinetics, while thermal treatment and open mesoporous network architecture have a minor impact. As a logical consequence of our dissolution model, we proved that the dissolution lag-time can be promoted by selective blocking of the mesopores that limits the access to the mesoporous internal surface. This study was broadened by studying the impact of the organosilanes in the silica structure, of the presence of residual structuring agents, and of the chemical composition of the dissolution medium. The presence of albumin at blood concentration was found affecting drastically the dissolution kinetics of the mesoporous structure, acting as a diffusion barrier. Globally, we could identify the main factors affecting mesoporous silica materials degradation and proved that we can tune their structure and composition for adjusting dissolution kinetics in order to achieve efficient drug delivery.

Published
2020

22. Aerosol synthesis of thermally stable porous noble metals and alloys by using bi-functional templates

Author

Mateusz Odziomek, Sophie Nowak, Mounib Bahri, Marco Faustini, Marion Giraud, Clément Sanchez, Cédric Tard, Benedikt Lassalle-Kaiser, Cédric Boissière, Jennifer Peron, Andrea Zitolo, Ovidiu Ersen, Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de photonique et de nanostructures (LPN), Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, Synchrotron SOLEIL (SSOLEIL), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Laboratoire de chimie moléculaire (LCM), École polytechnique (X)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace, Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA), Novel Advanced Nano-Objects (LCMCP-NANO), Interfaces, Traitements, Organisation et Dynamique des Systèmes [Depuis 2020] (ITODYS (UMR_7086)), Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie - UMR5182 (LC), École normale supérieure - Lyon (ENS Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Ecole Nationale Supérieure de Chimie de Paris- Chimie ParisTech-PSL (ENSCP)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SOLEIL), Dipartimento di Chimica, Università degli Studi di Roma 'La Sapienza' [Rome], Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace, Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), Laboratoire de physique de la matière condensée (LPMC), Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), École supérieure du professorat et de l'éducation - Académie de Grenoble (ESPE Grenoble), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Université Grenoble Alpes (UGA), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), Faustini, Marco, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)

Subjects
Nanostructure, Materials science, Absorption spectroscopy, Nanotechnology, 02 engineering and technology, engineering.material, 010402 general chemistry, Electrocatalyst, 01 natural sciences, Catalysis, [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, General Materials Science, Thermal stability, Electrical and Electronic Engineering, Porosity, Nanoscopic scale, [CHIM.MATE] Chemical Sciences/Material chemistry, Process Chemistry and Technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Mechanics of Materials, engineering, Noble metal, 0210 nano-technology
Abstract

International audience; Porous noble metal nanostructures providing high surface areas and large pore volumes are attractive for numerous applications especially catalysis. However, the synthesis of such architectures with nanoscale features is challenging because of i.e high surface energy. Previous reports are based on multi-step synthetic approaches with low yield thus not compatible with industrial scale. Herein, we demonstrate that hierarchical nanostructured noble metals and alloys, with thermal stability up to 800 °C, can be fabricated by a high throughput, green and straightforward aerosol-assisted synthesis using bi-functional reducing templates. We unravel the reduction mechanism at the solid/solid interface at the single-particle level using state-of-the-art techniques such as in situ Transmission Electron Microscopy, in situ synchrotron-based X-ray absorption spectroscopy. We propose a mechanism based on a radical process thermally triggered by the depolymerization of organic components. From a fundamental point of view, this study sheds light on the reduction processes of noble metals in the presence of organic compounds with important fundamental implications for catalysis and electrocatalysis.

Published
2020

23. Hollow zeolite microspheres as a nest for enzymes: a new route to hybrid heterogeneous catalyst

Author

Walid Baaziz, Valentin Smeets, Eric M. Gaigneaux, Ovidiu Ersen, Damien P. Debecker, Cédric Boissière, Clément Sanchez, Institut de la matière condensée et des nanosciences / Institute of Condensed Matter and Nanosciences (IMCN), Université Catholique de Louvain = Catholic University of Louvain (UCL), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and UCL - SST/IMCN/MOST - Molecules, Solids and Reactivity

Subjects
biology, Immobilized enzyme, 010405 organic chemistry, Glycidol, General Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, Heterogeneous catalysis, 01 natural sciences, 0104 chemical sciences, Catalysis, Chemistry, chemistry.chemical_compound, chemistry, Chemical engineering, Nanocrystal, biology.protein, Glucose oxidase, Zeolite, Macromolecule
Abstract

In the field of heterogeneous catalysis, the successful integration of enzymes and inorganic catalysts could pave the way to multifunctional materials which are able to perform advanced cascade reactions. However, such combination is not straightforward, for example in the case of zeolite catalysts for which enzyme immobilization is restricted to the external surface. Herein, this challenge is overcome by developing a new kind of hybrid catalyst based on hollow zeolite microspheres obtained by the aerosol-assisted assembly of zeolite nanocrystals. The latter spheres possess open entry-ways for enzymes, which are then loaded and cross-linked to form cross-linked enzyme aggregates (CLEAs), securing their entrapment. This controlled design allows the combination of all the decisive features of the zeolite with a high enzyme loading. A chemo-enzymatic reaction is demonstrated, where the structured zeolite material is used both as a nest for the enzyme and as an efficient inorganic catalyst. Glucose oxidase (GOx) ensures the in situ production of H2O2 subsequently utilized by the TS-1 zeolite to catalyze the epoxidation of allylic alcohol toward glycidol. The strategy can also be used to entrap other enzymes or combination of enzymes, as demonstrated here with combi-CLEAs of horseradish peroxidase (HRP) and glucose oxidase. We anticipate that this strategy will open up new perspectives, leveraging on the spray-drying (aerosol) technique to shape microparticles from various nano-building blocks and on the entrapment of biological macromolecules to obtain new multifunctional hybrid microstructures., A spray drying technique is used to prepare hollow zeolite microparticles into which an enzyme can be entrapped. Via this “Lego-like” strategy, we create hybrid heterogeneous catalysts that can run multistep chemo-enzymatic cascade reactions.

Published
2020

24. Homogeneous supported monolayer from microbial glycolipid biosurfactant

Author

Vincent Humblot, Niki Baccile, Cédric Boissière, Anyssa Derj, Ariane Deniset-Besseau, Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Franche-Comté Électronique Mécanique, Thermique et Optique - Sciences et Technologies (UMR 6174) (FEMTO-ST), Université de Technologie de Belfort-Montbeliard (UTBM)-Ecole Nationale Supérieure de Mécanique et des Microtechniques (ENSMM)-Université de Franche-Comté (UFC), Université Bourgogne Franche-Comté [COMUE] (UBFC)-Université Bourgogne Franche-Comté [COMUE] (UBFC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique D'Orsay (LCPO), and Université Paris-Sud - Paris 11 (UP11)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
glycolipids, Materials science, microbial biosurfactants, supported lipid bilayers, dip-coating, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Dip-coating, biosurfactants, Colloid, Lamellar phase, Monolayer, Amphiphile, Materials Chemistry, microbial glycolipids, Lamellar structure, Physical and Theoretical Chemistry, [NLIN.NLIN-AO]Nonlinear Sciences [physics]/Adaptation and Self-Organizing Systems [nlin.AO], Spectroscopy, Substrate (chemistry), lamellar, [CHIM.MATE]Chemical Sciences/Material chemistry, Adhesion, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Chemical engineering, 0210 nano-technology
Abstract

International audience; The development of supported glycosylated lipid layers is an important trend in the field of glyconanomaterials for their interest in understanding sugar-sugar and protein-sugar interactions, these being at the core of cellular, bacterial or viral adhesion. The conventional self-assembled monolayer (SAM) approach generally requires a thiolated glycoconjugate and a gold substrate. In this work, we show how glycolipid amphiphiles of natural origin, commonly known as microbial biosurfactants, can be easily deposited onto a substrate. Spontaneously produced by microorganisms but lacking a thiol group, one can take advantage of their self-assembly properties to prepare homogeneous supported lipid monolayers (SLM). We then choose a saturated glucolipid, G-C18:0, which forms a colloidal lamellar phase under diluted conditions. The lamellae can then be deposited onto a substrate (silicon, gold) using a physical method (dip coating). Dip coating is preferred over more classical deposition methods (Langmuir-Blodgett-LB-, vesicle fusion or spin-coating) because of its versatility, compatibility with aqueous solutions and robust control of the thickness below 10 nm. Defect-free glycosylated SLM from a microbial biosurfactant are then easily developed. A combination of ellipsometry, fluorescence microscopy, atomic force microscopy and infrared nanospectroscopy (AFMIR) show that the glycosylated SLM are defect-free, have a thickness of 2.8 ± 1.0 nm and they are highly homogeneous at scales going from the nm to cm.

Published
2022

25. Aerosol processing: a wind of innovation in the field of advanced heterogeneous catalysts

Author

Damien P. Debecker, Alexandra Chaumonnot, Solène Le Bras, Clément Sanchez, Cédric Boissière, Université Catholique de Louvain = Catholic University of Louvain (UCL), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), IFP Energies nouvelles (IFPEN), and Chaire Chimie des matériaux hybrides

Subjects
Materials science, Nanoparticle, Nanotechnology, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Catalysis, Nanomaterials, Aerosol, Suspension (chemistry), Methanation, Spray drying, [CHIM]Chemical Sciences, 0210 nano-technology, Porosity
Abstract

International audience; Aerosol processing is long known and implemented industrially to obtain various types of divided materials and nanomaterials. The atomisation of a liquid solution or suspension produces a mist of aerosol droplets which can then be transformed via a diversity of processes including spray-drying, spray pyrolysis, flame spray pyrolysis, thermal decomposition, micronisation, gas atomisation, etc. The attractive technical features of these aerosol processes make them highly interesting for the continuous, large scale, and tailored production of heterogeneous catalysts. Indeed, during aerosol processing, each liquid droplet undergoes well-controlled physical and chemical transformations, allowing for example to dry and aggregate pre-existing solid particles or to synthesise new micro- or nanoparticles from mixtures of molecular or colloidal precursors. In the last two decades, more advanced reactive aerosol processes have emerged as innovative means to synthesise tailored-made nanomaterials with tunable surface properties, textures, compositions, etc. In particular, the “aerosol-assisted sol–gel” process (AASG) has demonstrated tremendous potential for the preparation of high-performance heterogeneous catalysts. The method is mainly based on the low-cost, scalable, and environmentally benign sol–gel chemistry process, often coupled with the evaporation-induced self-assembly (EISA) concept. It allows producing micronic or submicronic, inorganic or hybrid organic–inorganic particles bearing tuneable and calibrated porous structures at different scales. In addition, pre-formed nanoparticles can be easily incorporated or formed in a “one-pot” bottom-up approach within the porous inorganic or hybrid spheres produced by such spray drying method. Thus, multifunctional catalysts with tailored catalytic activities can be prepared in a relatively simple way. This account is an overview of aerosol processed heterogeneous catalysts which demonstrated interesting performance in various relevant chemical reactions like isomerisation, hydrogenation, olefin metathesis, pollutant total oxidation, selective oxidation, CO2 methanation, etc. A short survey of patents and industrial applications is also presented. Our objective is to demonstrate the tremendous possibilities offered by the coupling between bottom up synthesis routes and these aerosol processing technologies which will most probably represent a major route of innovation in the mushrooming field of catalyst preparation research.

Published
2018

26. Hollow Iridium-Based Catalysts for the Oxygen Evolution Reaction in Proton Exchange Membrane Water Electrolyzers

Author

Jacques Rozière, Cédric Boissière, Deborah J. Jones, Jennifer Peron, Cédric Tard, Marco Faustini, Marion Giraud, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'Electrochimie Moléculaire (LEM (UMR_7591)), Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC)

Subjects
Aqueous solution, Chemistry, Inorganic chemistry, Oxygen evolution, Proton exchange membrane fuel cell, chemistry.chemical_element, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, Thermal treatment, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Catalysis, law.invention, law, Iridium, Crystallization, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

The performance of Proton Exchange Membrane Electrolyzers (PEMWE) is mostly impeded by the efficiency of the anode catalysts allowing for the Oxygen Evolution Reaction (OER) to occur. New catalytic materials should possess at least as high performance and stability as state of the art materials, since the price of electrolysis is mostly impacted by the price of electricity and higher overpotentials would render the catalysts not viable for application in PEMWE. The use of noble metal at the anode for the OER is at the current stage essential due to the highly oxidative and strongly acidic environment. Nevertheless, due to cost and resources considerations, it is necessary to reduce the noble metal content. In addition, according to present industrial requirements, PEMWE cells should be able to work at very high current density and under high pressure. Water and gases management are also a major challenge in PEMWE catalyst layers, and unlike in fuel cells or PEMWE cathodes the use of a cheap carbon based porous support for electronic conduction at the anode is highly undesirable due to highly anodic potential. We have developed a cheap, clean and easily scalable synthesis method to produce highly porous iridium-based materials. The materials are synthesized in aqueous solutions in presence of a porogen. The resulting material is further calcinated to remove the porogen and initiate crystallization of the inorganic phase. By adjusting reactant concentrations and calcination conditions, metallic iridium, iridium oxide or mixed oxides can be obtained. This last point is of high importance since in addition to reducing noble metals content compared to current technologies, the atomic neighborhood of dissimilar metals is expected to modify the monometallic behavior and potentially gives rise to new desired characteristics, i.e.to decrease the OER overpotential and/or increase the material stability. Structural characteristics and chemical composition of the materials have been determined using XRD, XPS and XRF. The influence of the thermal treatment has a strong impact on the crystallite size and the composition of the particle surface. SEM-FEG and BET characterizations have shown that the type of the porogen used for material synthesis directly impacts its morphology and porosity. To assess the catalytic performances of these hierarchically porous materials, a screening of the electrocatalytic activity of a series of prepared materials has been performed using a three-electrodes electrochemical setup. The optimized material shows lower overpotential than commercial Ir or IrO2 nanoparticles as shown on the figure thereafter. Finally, selected materials have been used to prepare anode catalyst layers and have been tested in a complete electrolysis device. With a loading of 2 mg cm-2 in Iridium, a potential of 1.65 V at 1 A cm-2 and of 1.85 V at 2 A cm-2 is obtained. The produced specific morphologies are very well adapted to the formation of porous percolating networks, which promote gases and water transport throughout the catalyst layer. Figure 1

Published
2017

27. Interfacial Mechanisms of Water Vapor Sorption into Cellulose Nanofibril Films as Revealed by Quantitative Models

Author

Marco Faustini, Tekla Tammelin, Minna Hakalahti, Cédric Boissière, Eero Kontturi, VTT Technical Research Centre of Finland (VTT), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Aalto University

Subjects
Langmuir, Materials science, ADSORPTION, Polymers and Plastics, SURFACE, FEATURES, Nanofibers, Analytical chemistry, Bioengineering, 02 engineering and technology, 010402 general chemistry, ISOTHERM, 01 natural sciences, Biomaterials, Adsorption, Piperidines, QUARTZ-CRYSTAL MICROBALANCE, Materials Chemistry, Cellulose, Oxidized, Relative humidity, ta216, ta116, ComputingMilieux_MISCELLANEOUS, ELLIPSOMETRY, ta1182, Humidity, Sorption, Quartz crystal microbalance, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, BET, TRANSPORT, 0104 chemical sciences, Steam, NANOCRYSTALS, Absorption, Physicochemical, Absorption (chemistry), POLYMERS, 0210 nano-technology, Water vapor
Abstract

Humidity is an efficient instrument for facilitating changes in local architectures of two-dimensional surfaces assembled from nanoscaled biomaterials. Here, complementary surface-sensitive methods are used to collect explicit and precise experimental evidence on the water vapor sorption into (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO) oxidized cellulose nanofibril (CNF) thin film over the relative humidity (RH) range from 0 to 97%. Changes in thickness and mass of the film due to water vapor uptake are tracked using spectroscopic ellipsometry and quartz crystal microbalance with dissipation monitoring, respectively. Experimental data is evaluated by the quantitative Langmuir/Flory-Huggins/clustering model and the Brunauer-Emmett-Teller model. The isotherms coupled with the quantitative models unveil distinct regions of predominant sorption modes: specific sorption of water molecules below 10% RH, multilayer build-up between 10 to 75% RH, and clustering of water molecules above 75% RH. The study reveals the sorption mechanisms underlying the well-known water uptake behavior of TEMPO oxidized CNF directly at the gas-solid interface.

Published
2017

28. Stability and degradation of PEO20PPO70PEO20 triblock copolymers in mesostructured silica

Author

Sandra Casale, Bénédicte Lebeau, Brindusa Dragoi, François Ribot, Guillaume Laurent, Anne Davidson, Mohamed Selmane, David Kreher, Taissire Benamor, Cédric Boissière, Patrick Schmidt, Laboratoire de Réactivité de Surface (LRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Alexandru Ioan Cuza University of Iași [Romania], Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Science des Matériaux de Mulhouse (IS2M), Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Centre de Biotechnologie de Borj Cédria (Hammam-Lif, Tunisie), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Novel Advanced Nano-Objects (LCMCP-NANO), Institut des matériaux de Paris-Centre (IMPC), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Eberhard Karls Universität Tübingen = Eberhard Karls University of Tuebingen, Chimie des polymères (LCP), Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut Parisien de Chimie Moléculaire (IPCM), Chimie Moléculaire de Paris Centre (FR 2769), École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Paris-Ile-de-France - SESAME program (700 MHz spectrometer), PERFORM-ERA ‘‘Post- doctoral Performance for Integration in the European Research Area’’ (ID-57649), financed by the European Social Fund and the Romanian Government, Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS), Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769), and Laurent, Guillaume

Subjects
[CHIM.POLY] Chemical Sciences/Polymers, Materials science, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biomaterials, Hydrolysis, chemistry.chemical_compound, Materials Chemistry, Copolymer, Propylene oxide, ordered, P123, structured, [CHIM.MATE] Chemical Sciences/Material chemistry, Ethylene oxide, Precipitation (chemistry), technology, industry, and agriculture, template, General Chemistry, NIR, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Decomposition, NMR, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Chemical engineering, Spray drying, Ceramics and Composites, Self-assembly, 0210 nano-technology
Abstract

International audience; Organic−inorganic hybrid mesostructured silicas are prepared, without stirring (at pH = 0.0) and with stirring (at pH = 0.6) to obtain isolated and gyroidal-like attached silica grains with incorporated triblock P123 poly (ethylene oxide)-poly (propylene oxide)–poly (ethylene oxide) copolymers. Selected hybrids are submitted to various thermal and aging treatments for studying hydrolysis and oxidation of PEO and PPO chains. Two complementary spectroscopic techniques are used: near-infrared (NIR) with measurements performed in diffuse reflectance, as well as 1H and 13C liquid- and solid-state nuclear magnetic resonance (NMR) to study the mobility and stability of PEO and PPO chains. With precipitated fresh hybrids, the ratio of PEO over (PEO + PPO) units is lower (30% ± 5%) than in theory. This ratio also decreases depending on temperature when a hydrothermal treatment is applied. An acidic hydrolysis involving both PEO and PPO chains, with generated fragments eliminated by washing with water and/or synthesis liquor, is then demonstrated. For comparison, another hybrid obtained by spray drying via evaporation-induced self assembly mechanism is also studied. Its NMR signals are much more stable than those of the samples prepared by precipitation. Depending on aging time, thermal history, and materials processing, the textural properties and template decomposition inside mesostructured silica are found significantly different. The influence of the hydrolysis and oxidation of the template onto final materials texture is likely to be as important as the processing conditions.

Published
2019

29. Interdiffusive Surfactant Procedure for the Preparation of Nanoarchitectured Porous Films: Application to the Growth of Titania Thin Films on Silicon Substrates

Author

Clément Sanchez, Cédric Boissière, Pilar Aranda, Javier Pérez-Carvajal, Eduardo Ruiz-Hitzky, Department of New Architectures in Materials Chemistry, Materials Science Institute of Madrid, Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Chaire Chimie des matériaux hybrides

Subjects
Materials science, Silicon, Nanoparticle, chemistry.chemical_element, 02 engineering and technology, engineering.material, 010402 general chemistry, 01 natural sciences, Pulmonary surfactant, Coating, Electrochemistry, General Materials Science, Thin film, Porosity, Spectroscopy, ComputingMilieux_MISCELLANEOUS, Surfaces and Interfaces, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, chemistry, Chemical engineering, engineering, 0210 nano-technology, Mesoporous material, Layer (electronics)
Abstract

Herein is reported the preparation of nanostructured mesoporous supported films, in this case, titanium dioxide nanoparticles on silicon wafer, according to a new approach taking place in two consecutive deposition steps: (i) coating of a homogeneous and continuous layer of a surfactant on the selected support and (ii) building up of a second layer of the fresh metal-oxide gel precursor, followed by thermal treatment to generate porosity. This approach represents an alternative way to soft-template procedures, as for instance, the largely applied evaporation-induced self-assembly (EISA) method, which typically consists of a single-step deposition of the mixture of gel precursor and surfactant used as a soft template to create porosity. The main advantage of the procedure reported here compared to the EISA method is the possibility of reaching tunable textural characteristics along the growing film (pore size, shape, and distribution of pores) by using gels with nanoparticles preformed at different stages via a simple regulation of the residence time of the precursors deposited on the support containing the surfactant.

Published
2019

30. Hollow zeolite microspheres as a nest for enzymes: a new route to hybrid heterogeneous catalysts for chemo-enzymatic cascade reactions

Author

Valentin Smeets, Walid Baaziz, Ovidiu Ersen, Eric M. Gaigneaux, Cédric Boissière, Clément Sanchez, and Damien Debecker

Abstract

Integrating enzymatic and heterogeneous catalysis can pave the way to new and performing cascade chemical processes. In this perspective, the preparation of bifunctional structures combining both an active inorganic catalyst and an enzyme is a key. However, such combinations are not straightforward, for example in the case of zeolite catalysts for which enzyme immobilization would be restricted to the external surface. We overcame this challenge by developing a new kind of hybrid catalysts based on hollow zeolite microspheres. The method leverages on the aerosol-assisted assembly of TS-1 nanocrystals to form hollow zeolite microspheres with tailored hierarchical texture and high epoxidation activity in water. The latter spheres were subsequently loaded with glucose oxidase enzymes which were then cross-linked to secure their entrapment. This controlled design allows to combine all the decisive features of the zeolite with a high enzyme loading. A chemo-enzymatic reaction is demonstrated, where the structured zeolite microsphere is used both as a nest for the enzyme and as an efficient inorganic heterogeneous catalyst. The enzyme ensures the in situ production of H2O2 subsequently utilized by the zeolite for the epoxidation of allylic alcohol. We anticipate our method will open up new perspectives in the field of hybrid catalysis. Starting from various catalytic nano-building blocks, hollow microspheres with open entry ways could be prepared using the aerosol process and could be used as vessels for enzymes or even multi-enzymatic systems, thereby giving access to a multitude of new heterogeneous chemo-biocatalysts.

Published
2019

31. Engineering of Silica Thin-Film Nanoporosity via Alkali-Ion-Assisted Reconstruction

Author

Mickaël Boudot, Ekaterina Burov, Cédric Boissière, Thierry Gacoin, Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Surface du Verre et Interfaces (SVI), Centre National de la Recherche Scientifique (CNRS), Laboratoire de physique de la matière condensée (LPMC), and École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, General Chemical Engineering, Fraction (chemistry), 02 engineering and technology, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, Mesoporous silica, 010402 general chemistry, 021001 nanoscience & nanotechnology, Alkali metal, 01 natural sciences, 0104 chemical sciences, Ion, Chemical engineering, Materials Chemistry, [CHIM]Chemical Sciences, Thin film, 0210 nano-technology, Porosity, ComputingMilieux_MISCELLANEOUS
Abstract

We report a method to prepare patterned mesoporous silica-based films with fine control of the pore sizes and the porous fraction by combining the sol–gel approach with an alkali ion post-treatment...

Published
2019

32. Aerosol-Assisted Sol-Gel Synthesis of Mesoporous TiO2 Materials, and Their Use as Support for Ru-Based Methanation Catalysts

Author

Damien P. Debecker, Bernard Haye, Capucine Sassoye, Clément Sanchez, Ara Kim, and Cédric Boissière

Subjects
Anatase, Crystallinity, Materials science, Chemical engineering, law, Methanation, Specific surface area, Nanoparticle, Calcination, Crystallization, Mesoporous material, law.invention
Abstract

Mesoporous TiO2 materials have been prepared by an aerosol process, which leverages on the acetic acid-mediated sol-gel chemistry and on the evaporation-induced self-assembly phenomenon to obtain materials with high specific surface area and large mesoporous volume. The obtained spherical particles are calcined to release the porosity. It is shown that the mesoscopic order can be preserved when the calcination is carried out at relatively low temperature (375 °C and below). Harsher calcination conditions lead to the progressive destruction of the mesostructured, concomitant with a progressive drop of textural properties and with the crystallization of larger anatase domains. The mesoporous TiO2 material calcined at 350°C (specific surface area = 260 m².g-1; pore volume = 0.36 cm³.-1; mean pore diameter = 5.4 nm) was selected as a promising support for preformed RuO2 nanoparticles, and subsequently annealed in air. It is shown that the presence of RuO2 nanoparticles and subsequent annealing provoke further intense modification of the texture and crystallinity of the TiO2 materials. In addition to a drop in the textural parameters, a RuO2-mediated crystallization of rutile TiO2 is highlighted at temperature as low as 250°C. After an in situ reduction in H2, the catalysts containing TiO2 rutile and relatively small RuO2 crystals showed the highest activity in the methanation of CO2.

Published
2019

33. Aerosol Route to TiO 2 –SiO 2 Catalysts with Tailored Pore Architecture and High Epoxidation Activity

Author

Valentin Smeets, Elise Peeters, Damien P. Debecker, Eric M. Gaigneaux, Michiel Dusselier, Bert F. Sels, Cédric Boissière, Clément Sanchez, Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Novel Advanced Nano-Objects (LCMCP-NANO), Chaire Chimie des matériaux hybrides, Unité de catalyse et chimie des matériaux divisés, Université Catholique de Louvain = Catholic University of Louvain (UCL), and Institute of Condensed Matter and Nanosciences (ICMN)

Subjects
Technology, Materials science, General Chemical Engineering, Materials Science, Epoxidation, Materials Science, Multidisciplinary, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, OXIDATION, 01 natural sciences, Catalysis, SELECTIVE EPOXIDATION, HYDROGEN-PEROXIDE, XEROGELS, Materials Chemistry, PARTICLES, spray-drying, Porosity, AEROGELS, Science & Technology, Chemistry, Physical, General Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, PERFORMANCE, 021001 nanoscience & nanotechnology, 3. Good health, 0104 chemical sciences, Aerosol, SILICA MIXED OXIDES, Chemistry, Chemical engineering, Physical Sciences, SOL-GEL ROUTES, 0210 nano-technology, Dispersion (chemistry), mesoporous, TITANIUM SILICALITE-1
Abstract

© 2019 American Chemical Society. Herein, we present the aerosol-assisted sol-gel preparation of hierarchically porous TiO 2 -SiO 2 catalysts having a spherelike shell morphology and a high Ti dispersion. In order to control the porosity at the micro-, meso-, and macrolevels, we use the evaporation-induced self-assembly (EISA) of a surfactant, possibly combined with polymer beads as hard templates. These catalysts are tested for the epoxidation of cyclohexene with cumene hydroperoxide as the oxidant, and their performance is compared to the reference TS-1 zeolite. The high catalytic performance observed with the catalysts prepared by aerosol stems from their high specific surface area, but also from the short diffusion path length generated by the meso-/macropore architecture which provides entryways for bulky reactants and products. Besides, these materials can incorporate a higher Ti loading than TS-1 zeolite, while ensuring a good control over the Ti speciation. Thus, the unique features of the aerosol process - which is also known to be scalable - allow us to prepare catalytic materials with high epoxidation activity, also for bulky olefins. ispartof: Chemistry of Materials vol:31 issue:5 pages:1610-1619 status: published

Published
2019

34. Hierarchically Structured Ultraporous Iridium-Based Materials: A Novel Catalyst Architecture for Proton Exchange Membrane Water Electrolyzers

Author

Mounib Bahri, Jacques Rozière, Thomas R. Porter, Marc Dupont, Marco Faustini, Cédric Tard, Deborah J. Jones, Jennifer Peron, Sophie Nowak, Marion Giraud, Ovidiu Ersen, Clément Sanchez, Cédric Boissière, Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Laboratoire d'Electrochimie Moléculaire (LEM (UMR_7591)), Laboratoire de photonique et de nanostructures (LPN), Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Novel Advanced Nano-Objects (LCMCP-NANO), Chaire Chimie des matériaux hybrides, Laboratoire de chimie moléculaire (LCM), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), École supérieure du professorat et de l'éducation - Académie de Grenoble (ESPE Grenoble), Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry]), Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), and École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Electrolysis process, Materials science, Nanoparticle, chemistry.chemical_element, Proton exchange membrane fuel cell, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, law.invention, Catalysis, law, porous catalysts, General Materials Science, Iridium, Electrolytic process, Anodes, Electrolysis, Renewable Energy, Sustainability and the Environment, Oxygen evolution, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Evaporation (deposition), 0104 chemical sciences, chemistry, Chemical engineering, nanoneedles, 0210 nano-technology, Hydrogen
Abstract

International audience; Iridium oxide is the gold‐standard catalyst for the oxygen evolution reaction (OER) in acidic media due to its unmatched activity and stability. Here, a new catalyst architecture comprising a nanoneedle network of iridium‐containing oxides assembled into macroporous micrometric particles with ≈75% of porosity is reported. The rationally designed porous hierarchical structure optimizes the accessibility of reactants and products to the surface of the nanoparticles and maximizes catalyst activity. The materials are easily prepared from aqueous solutions by an industrially viable spray‐drying route through an evaporation self‐assembly mechanism. The versatility of the process enables the preparation of mixed oxides with low iridium content, particles with tunable crystallinity, and various iridium surface species with high electrochemical activity. Highly porous Ir0.7Ru0.3O2 outperforms commercial iridium oxide. These materials also represent an ideal platform to assess the reactivity of the iridium and oxygen species involved in the oxygen evolution reaction. Furthermore, it is demonstrated that these highly porous particles are optimal building blocks to be integrated into catalyst layers, without the drawbacks associated with the use of discrete nanoparticles. Fresh‐ and end‐of‐test membrane–electrode assemblies' characterization shows that their particular architecture is preserved upon catalyst layer preparation and after operation in a proton‐exchange membrane electrolysis cell.

Published
2019

35. A pure aqueous route to mesoporous silica thin films via dip-coating of prefabricated hybrid micelles

Author

Heiko Zschiedrich, Cédric Boissière, Patricia J. Kooyman, Eric Prouzet, Institut Européen des membranes (IEM), Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM), DelftChemTech/NCH REM, Delft University of Technology (TU Delft), Institute for Nanotechnology [Waterloo], University of Waterloo [Waterloo], Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Dip-coating, Nanostructure, Materials science, Evaporation-induced self-assembly, Mesoporous, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Micelle, Biomaterials, Materials Chemistry, Composite material, Aqueous solution, Ellipsoporosimetry, Silica, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, Mesoporous silica, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Evaporation (deposition), 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Mesoporous organosilica, Thin film, Ceramics and Composites, 0210 nano-technology, Mesoporous material
Abstract

Mesoporous thin films were prepared by dip-coating with a purely aqueous method, as a substitute for the alcohol-based evaporation-induced self-assembly route. Unlike other aqueous routes that require a very slow pulling rate possible only using high performance dip-coaters, as a result of the high surface tension of water, this new process works with standard dip-coaters and at similar pulling rates as are used for the evaporation-induced self-assembly route. This unique asset is the result of the synthesis of prefabricated self-assembled silicate/organic hybrid micelles. These building blocks are concentrated before use, which provides a gelling edge after moderate evaporation. As a result, defect-free continuous mesoporous films with well-organized hexagonally packed pores were prepared after optimization of both the evaporation rate of the solution of hybrid micelles and the dip-coater pulling rate. The transmission electron microscopy observation reveals the hexagonally packed structure of mesoporous silica film. This nanostructure has already been observed on films prepared with the evaporation-induced self-assembly process, but it is the first time it is obtained with a pure aqueous method, based on prefabricated hybrid micelles, not on controlled evaporation of mesophases.

Published
2016

36. Multifunctional core–shell hybrid nano-composites made using Pickering emulsions: a new design for therapeutic vectors

Author

Thomas Fontecave, Clément Sanchez, Cédric Boissière, Marc-André Fortin, Manon Bourbousson, Ana Espinosa, Claire Wilhelm, Corinne Chanéac, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Nanomatériaux (MHN), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Centre National de la Recherche Scientifique (CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Centre National de la Recherche Scientifique (CNRS), Matière et Systèmes Complexes (MSC (UMR_7057)), Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), and Matière et Systèmes Complexes (MSC)

Subjects
Chemistry, Nanoparticle, Nanotechnology, 02 engineering and technology, General Chemistry, Prodrug, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Catalysis, Pickering emulsion, 0104 chemical sciences, Ouzo effect, Covalent bond, Drug delivery, Emulsion, Materials Chemistry, [CHIM]Chemical Sciences, Molecule, 0210 nano-technology
Abstract

International audience; In this manuscript, we present a new strategy for the direct synthesis of functional nano-composite hybrid therapeutic vectors. The smart coupling of soft-chemistry and “ouzo effect” based emulsification processing allows us to create in a very simple way a Pickering stabilized emulsion from various prodrug modelling molecules used as a core, and subsequently embedded into a mesostructured silica shell. The resulting prodrug/Fe2O3/silica architecture offers a very good functionality/complexity ratio, realistic from a pharmaceutical development point of view at the industrial scale. While usual magnetic resonance imaging (MRI) contrast agent properties of maghemite nanoparticles are maintained, we proved for the first time that their smart localization at the organic/silica interface allows us to isolate them from phosphate anions of the surrounding environment, and thus to use their surface as a heterogeneous catalyst for controlled hydrolysis-mediated model drug delivery. This original hydrolysis-mediated release mechanism was investigated by grafting a model drug molecule via various covalent bonds. The release time can be tuned by this approach in between one hour and three days. In addition, magnetic radio frequency stimulation commonly used for hyperthermia treatment was able to accelerate the catalytic hydrolysis and release of the model drug by one order of magnitude, proving that drug release can be triggered on demand.

Published
2016

37. Injectable Anisotropic Materials: Self‐Assembled Collagen Microparticles by Aerosol as a Versatile Platform for Injectable Anisotropic Materials (Small 4/2020)

Author

Jean-Jacques Lataillade, Clément Sanchez, M. Grosbot, Marina Trouillas, Bernard Coulomb, Alba Marcellan, Milena Lama, Francisco M. Fernandes, Marie-Madeleine Giraud-Guille, Cédric Boissière, J. Peltzer, Nadine Nassif, and Sébastien Banzet

Subjects
Biomaterials, Materials science, Spray drying, General Materials Science, Nanotechnology, General Chemistry, Self-assembly, Anisotropy, Biotechnology, Aerosol, Self assembled
Published
2020

38. Self‐Assembled Collagen Microparticles by Aerosol as a Versatile Platform for Injectable Anisotropic Materials

Author

Cédric Boissière, Nadine Nassif, Sébastien Banzet, Marie-Madeleine Giraud-Guille, Francisco M. Fernandes, Jean-Jacques Lataillade, Alba Marcellan, Bernard Coulomb, Clément Sanchez, M. Grosbot, Marina Trouillas, Milena Lama, J. Peltzer, Matériaux et Biologie (LCMCP-MATBIO), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Sciences et Ingénierie de la Matière Molle (UMR 7615) (SIMM), Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Composantes innées de la réponse immunitaire et différenciation (CIRID), Université Bordeaux Segalen - Bordeaux 2-Centre National de la Recherche Scientifique (CNRS), Département des Facteurs Humains, Service de Santé des Armées-Ministère de la Défense, Chaire Chimie des matériaux hybrides, Paris-Centre de Recherche Cardiovasculaire (PARCC - UMR-S U970), Hôpital Européen Georges Pompidou [APHP] (HEGP), Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP)-Hôpitaux Universitaires Paris Ouest - Hôpitaux Universitaires Île de France Ouest (HUPO)-Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP)-Hôpitaux Universitaires Paris Ouest - Hôpitaux Universitaires Île de France Ouest (HUPO)-Université Paris Descartes - Paris 5 (UPD5)-Institut National de la Santé et de la Recherche Médicale (INSERM), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Sciences et Ingénierie de la Matière Molle (SIMM), ESPCI ParisTech-PSL Research University (PSL)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Université Paris Descartes - Paris 5 (UPD5)-Hôpital Européen Georges Pompidou [APHP] (HEGP), Hôpitaux Universitaires Paris Ouest - Hôpitaux Universitaires Île de France Ouest (HUPO)-Assistance publique - Hôpitaux de Paris (AP-HP) (APHP)-Hôpitaux Universitaires Paris Ouest - Hôpitaux Universitaires Île de France Ouest (HUPO)-Assistance publique - Hôpitaux de Paris (AP-HP) (APHP)-Institut National de la Santé et de la Recherche Médicale (INSERM), and Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP)

Subjects
[SDV.BIO]Life Sciences [q-bio]/Biotechnology, [SDV]Life Sciences [q-bio], Gingiva, 02 engineering and technology, 010402 general chemistry, Fibril, 01 natural sciences, Self assembled, Biomaterials, Humans, [CHIM]Chemical Sciences, General Materials Science, Cells, Cultured, Aerosols, Tissue Scaffolds, Chemistry, Regeneration (biology), Mesenchymal stem cell, Mesenchymal Stem Cells, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, 021001 nanoscience & nanotechnology, Extracellular Matrix, 0104 chemical sciences, [CHIM.POLY]Chemical Sciences/Polymers, Cell culture, Collagen molecule, Biophysics, [SDV.IB]Life Sciences [q-bio]/Bioengineering, Collagen, Self-assembly, 0210 nano-technology, Type I collagen, Biotechnology
Abstract

Extracellular matrices (ECM) rich in type I collagen exhibit characteristic anisotropic ultrastructures. Nevertheless, working in vitro with this biomacromolecule remains challenging. When processed, denaturation of the collagen molecule is easily induced in vitro avoiding proper fibril self-assembly and further hierarchical order. Here, an innovative approach enables the production of highly concentrated injectable collagen microparticles, based on collagen molecules self-assembly, thanks to the use of spray-drying process. The versatility of the process is shown by performing encapsulation of secretion products of gingival mesenchymal stem cells (gMSCs), which are chosen as a bioactive therapeutic product for their potential efficiency in stimulating the regeneration of a damaged ECM. The injection of collagen microparticles in a cell culture medium results in a locally organized fibrillar matrix. The efficiency of this approach for making easily handleable collagen microparticles for encapsulation and injection opens perspectives in active tissue regeneration and 3D bioprinted scaffolds.

Published
2019

39. Stabilization of Mesoporous Iron Oxide Films against Sintering and Phase Transformations via Atomic Layer Deposition of Alumina and Silica

Author

Guylhaine Clavel, Nicola Pinna, Cédric Boissière, Roman Schmack, Katrin Kraffert, Thomas Wirth, Ralph Kraehnert, Matthias Karg, Stranski Laboratorium für Physikalische und Theoretische Chemie, Technische Universität Berlin (TU), CICECO, Universidade de Aveiro, Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Humboldt-Universität zu Berlin

Subjects
Materials science, Iron oxide, Sintering, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 01 natural sciences, Ferrihydrite, chemistry.chemical_compound, Atomic layer deposition, Thin layers, mesoporous oxides, Mechanical Engineering, [CHIM.MATE]Chemical Sciences/Material chemistry, Hematite, 021001 nanoscience & nanotechnology, 0104 chemical sciences, stabilization, chemistry, Chemical engineering, Mechanics of Materials, visual_art, atomic layer deposition, visual_art.visual_art_medium, Crystallite, 0210 nano-technology, Mesoporous material
Abstract

International audience; The stabilization of crystal phases and nanostructured morphologies is an essential topic in application-driven design of mesoporous materials. Many applications, e.g. catalysis, require high temperature and humidity. Typical metal oxides transform under such conditions from a metastable, low crystal-line material into a thermodynamically more favorable form, i.e. from ferrihy-drite into hematite in the case of iron oxide. The harsh conditions induce also a growth of the crystallites constituting pore walls, which results in sintering and finally collapse of the porous network. Herein, a new method to stabi-lize mesoporous templated metal oxides against sintering and pore collapse is reported. The method employs atomic layer deposition (ALD) to coat the internal mesopore surface with thin layers of either alumina or silica. The authors demonstrate that silica exerts a very strong influence: It shifts hematite formation from 400 to 600 °C and sintering of hematite from 600 to 900 °C. Differences between the stabilization via alumina and silica are rationalized by a different interaction strength between the ALD material and the ferrihydrite film. The presented approach allows to stabilize mesoporous thin films that require a high crystallization temperature, with submonolayer quantity of an ALD mate-rial, and to apply mesoporous materials for high temperature applications.

Published
2018

40. Dynamic Shaping of Femtoliter Dew Droplets

Author

Philippe Steyer, Andrea Cattoni, Marco Faustini, Annie Malchere, Cédric Boissière, David Grosso, Jennifer Peron, Paul Ebrard, Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre de Nanosciences et de Nanotechnologies [Marcoussis] (C2N), Université Paris-Sud - Paris 11 (UP11)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Matériaux, ingénierie et science [Villeurbanne] (MATEIS), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Institut des Matériaux, de Microélectronique et des Nanosciences de Provence (IM2NP), Aix Marseille Université (AMU)-Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Université de Lyon-Université de Lyon-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), and Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU)

Subjects
Materials science, Evaporation, General Physics and Astronomy, dew, hydrophilic, 02 engineering and technology, anisotropy, 010402 general chemistry, 01 natural sciences, law.invention, Physics::Fluid Dynamics, Optical microscope, law, [CHIM]Chemical Sciences, General Materials Science, Anisotropy, Lithography, Condensation, General Engineering, technology, industry, and agriculture, Femtoliter, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, eye diseases, 0104 chemical sciences, condensation, Chemical physics, nanoimprinting, shaping, Dew, Wetting, 0210 nano-technology
Abstract

International audience; Herein, we show that wetting properties such as giant wetting anisotropy and dynamic shaping can be observed when femtoliter (submicron scale) dew droplets are condensed on nanopatterned mildly hydrophilic surfaces. Large-scale, optically transparent, nanopatterned TiO2 surfaces were fabricated by direct nanoimprinting lithography of sol–gel-derived films. Square, infinitely elongated, or circular droplets were obtained with square, line, or concentric patterns, respectively, and were visualized in situ during formation and recession using optical microscopy and environmental scanning electronic microscopy. We first describe how extremely elongated droplets could form on mildly hydrophilic surfaces, naturally contaminated in real environmental conditions. In this configuration, the dew droplet shape can be dynamically and reversibly varied by controlling the out-of-equilibrium conditions associated with condensation/evaporation kinetics. As an example of the application, we propose a “morphological” sensor that exploits the shape of the dew droplets as a transduction mode for detecting organic vapors in the outer atmosphere. Importantly, this study is underlining that environmentally stable, purely hydrophilic surfaces can be smartly engineered to induce wetting phenomena at very small scale never observed so far for hydrophobic or heterogeneous surfaces. Our versatile approach based on nanoimprinted, transparent sol–gel films could open great perspectives for the implementation of environmentally stable, mildly hydrophilic materials for “dew engineering” applications such as open microfluidics, fuming for fingerprints, vapor sensing, or water harvesting on glass windows, for instance.

Published
2018

41. Gold–silica quantum rattles for multimodal imaging and therapy

Author

Ciro Chiappini, Sergio Bertazzo, Olumide Ogunlade, Challa S. S. R. Kumar, Glenna L. Drisko, Mark F. Lythgoe, Molly M. Stevens, Katla Sai Krishna, Mathew Hembury, Paul C. Beard, Coline Jumeaux, Cédric Boissière, Clément Sanchez, Alexandra E. Porter, Tammy L. Kalber, Simon Walker-Samuel, The Royal Society, Commission of the European Communities, Engineering & Physical Science Research Council (EPSRC), Department of Materials, Imperial College London, Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Engineering and Physical Sciences Research Council (EPSRC), Rosetrees Trust, Medical Research Council (MRC), Department of Health (DoH) (United Kingdom), UK Regenerative Medicine Platform Safety Hub [MRC: MR/K026739/1], European Union Project Functional Anatomical Molecular Optical Screening (FAMOS) (FP7 ICT) [317744], College de France, CNRS, EPSRC [EP/K020641/1], European Research Council starting grant [257182], US Department of Energy [DE-SC0001058, LEQSF (2008-10)-ENH-TR-07], EPSRC Early Career fellowship [EP/L006472/1], Wellcome Trust Senior Research fellowship [WT100247MA], King's College London, University College London (UCL) Comprehensive Cancer Imaging Centre Cancer Research UK (CR-UK), and EPSRC

Subjects
Physics::Optics, Nanoparticle, 02 engineering and technology, MAGNETISM, Multimodal Imaging, 01 natural sciences, chemistry.chemical_compound, NANOPARTICLES, Multidisciplinary, [CHIM.MATE]Chemical Sciences/Material chemistry, Silicon Dioxide, 021001 nanoscience & nanotechnology, nanomedicine, CANCER, TUMORS, 3. Good health, Multidisciplinary Sciences, Colloidal gold, Physical Sciences, Science & Technology - Other Topics, Nanomedicine, gold quantum dots, 0210 nano-technology, Materials science, Silicon dioxide, cancer nanotechnology, Nanotechnology, 010402 general chemistry, Nanoclusters, Microscopy, Electron, Transmission, Quantum Dots, MD Multidisciplinary, Humans, mesoporous silica, STRATEGY, FLUORESCENCE, Science & Technology, NANOCLUSTERS, hybrid nanoparticle, Phototherapy, Photothermal therapy, Mesoporous silica, equipment and supplies, 0104 chemical sciences, MODEL, chemistry, Quantum dot, Hela Cells, CELLS, Gold, CLUSTERS
Abstract

International audience; Gold quantum dots exhibit distinctive optical and magnetic behaviors compared with larger gold nanoparticles. However, their unfavorable interaction with living systems and lack of stability in aqueous solvents has so far prevented their adoption in biology and medicine. Here, a simple synthetic pathway integrates gold quantum dots within a mesoporous silica shell, alongside larger gold nanoparticles within the shell's central cavity. This ``quantum rattle'' structure is stable in aqueous solutions, does not elicit cell toxicity, preserves the attractive near-infrared photonics and paramagnetism of gold quantum dots, and enhances the drug-carrier performance of the silica shell. In vivo, the quantum rattles reduced tumor burden in a single course of photothermal therapy while coupling three complementary imaging modalities: near-infrared fluorescence, photoacoustic, and magnetic resonance imaging. The incorporation of gold within the quantum rattles significantly enhanced the drug-carrier performance of the silica shell. This innovative material design based on the mutually beneficial interaction of gold and silica introduces the use of gold quantum dots for imaging and therapeutic applications.

Published
2015

42. First acidic macro-mesocellular aluminosilicate monolithic foams 'SiAl(HIPE)' and their catalytic properties

Author

Cédric Boissière, Rénal Backov, Damien P. Debecker, Philippe Eliaers, Clément Sanchez, Guillaume Laurent, Stéphanie Huet, Institute of Condensed Matter and Nanosciences (ICMN), Université Catholique de Louvain = Catholic University of Louvain (UCL), Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre de recherches Paul Pascal (CRPP), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Centre de Ressources Technologiques en Chimie (Certech), The French Région Ile de France SESAME program is acknowledged for financial support (700 MHz spectrometer)., and UCL - SST/IMCN/MOST - Molecules, Solids and Reactivity

Subjects
geography, geography.geographical_feature_category, Materials science, education, technology, industry, and agriculture, Metals and Alloys, Nanotechnology, [CHIM.CATA]Chemical Sciences/Catalysis, General Chemistry, Catalysis, Sial, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, High surface, Chemical engineering, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Aluminosilicate, Emulsion, Materials Chemistry, Ceramics and Composites, Mixed oxide, Monolith, Mesoporous material
Abstract

International audience; A new type of acidic macrocellular and mesoporous silica-alumina foam is obtained via a one pot alkaline sol-gel route coupled with a concentrated emulsion-based templating technique. The mixed oxide monolith exhibits high surface acidity, translating in excellent performance in the acid-catalyzed dehydration of bioethanol to ethene.

Published
2015

43. Rendre les populations locales actrices de la surveillance de leur environnement. Cas de capteurs de suivi de la qualité de l’eau

Author

Ollivier Tamarin, Jean-Luc Lachaud, Hamida Hallil, Vincent Raimbault, Cédric Boissière, Marie-Paule Bonnet, Dominique Rebiere, Corinne Dejous, Laboratoire de l'intégration, du matériau au système (IMS), Université Sciences et Technologies - Bordeaux 1 (UB)-Institut Polytechnique de Bordeaux-Centre National de la Recherche Scientifique (CNRS), Université de Guyane (UG), Équipe MICrosystèmes d'Analyse (LAAS-MICA), Laboratoire d'analyse et d'architecture des systèmes (LAAS), Université Toulouse Capitole (UT Capitole), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université Toulouse - Jean Jaurès (UT2J), Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université Toulouse Capitole (UT Capitole), Université de Toulouse (UT), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), UMR 228 Espace-Dev, Espace pour le développement, Institut de Recherche pour le Développement (IRD)-Université de Perpignan Via Domitia (UPVD)-Avignon Université (AU)-Université de La Réunion (UR)-Université de Montpellier (UM)-Université de Guyane (UG)-Université des Antilles (UA), Centre National de la Recherche Scientifique (CNRS)-Institut Polytechnique de Bordeaux-Université Sciences et Technologies - Bordeaux 1, Université Toulouse - Jean Jaurès (UT2J)-Université Toulouse 1 Capitole (UT1), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse - Jean Jaurès (UT2J)-Université Toulouse 1 Capitole (UT1), Université Fédérale Toulouse Midi-Pyrénées, Université de Guyane (UG)-Université des Antilles (UA)-Institut de Recherche pour le Développement (IRD)-Université de Perpignan Via Domitia (UPVD)-Avignon Université (AU)-Université de La Réunion (UR)-Université de Montpellier (UM), and Université Sciences et Technologies - Bordeaux 1-Institut Polytechnique de Bordeaux-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS.PHYS.PHYS-INS-DET]Physics [physics]/Physics [physics]/Instrumentation and Detectors [physics.ins-det], [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, ComputingMilieux_MISCELLANEOUS
Abstract

National audience

Published
2017

44. Love wave devices coated with TiO2 porous sensitive layer for direct detection of small molecules

Author

Ollivier Tamarin, Wassim Ouelhazi, Jean-Luc Lachaud, Ingrid Bazin, Hamida Hallil, Vincent Raimbault, Cédric Boissière, Dominique Rebière, Corinne Dejous, Laboratoire de l'intégration, du matériau au système (IMS), Centre National de la Recherche Scientifique (CNRS)-Institut Polytechnique de Bordeaux-Université Sciences et Technologies - Bordeaux 1, Laboratoire de Génie de l'Environnement Industriel (LGEI), IMT - MINES ALES (IMT - MINES ALES), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Université Sciences et Technologies - Bordeaux 1-Institut Polytechnique de Bordeaux-Centre National de la Recherche Scientifique (CNRS)

Subjects
[SPI]Engineering Sciences [physics], [PHYS.PHYS.PHYS-INS-DET]Physics [physics]/Physics [physics]/Instrumentation and Detectors [physics.ins-det], [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2017

45. Flyscan opportunities in medicine: the case of quantum rattle based on gold quantum dots

Author

Julien Berthault, Chantal Jouanneau, Dominique Thiaudière, Corinne Chanéac, Nicolas Leclercq, Jean-François Greisch, Emmanuel Esteve, Bernard Leyh, Dominique Bazin, Solenn Reguer, Pierre Ronco, Michel Daudon, Cédric Boissière, Cristian Mocuta, Gustavo Lugo, Des Maladies Rénales Rares aux Maladies Fréquentes, Remodelage et Réparation, Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut National de la Santé et de la Recherche Médicale (INSERM), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Department of Chemistry [Liège], Université de Liège, Institute of Nanotechnology [Karlsruhe] (INT), Karlsruhe Institute of Technology (KIT), CHU Tenon [AP-HP], Sorbonne Université (SU)-Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Matériaux Hybrides et Procédés (LCMCP-MHP ), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP)-Sorbonne Université (SU)

Subjects
Nuclear and High Energy Physics, Materials science, X-ray fluorescence, Nanotechnology, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 01 natural sciences, law.invention, Data acquisition, law, gold-cluster-enriched mesoporous silica nanospheres, Absorption (electromagnetic radiation), xanes, Instrumentation, Quantum, Radiation, business.industry, [CHIM.MATE]Chemical Sciences/Material chemistry, Mesoporous silica, 021001 nanoscience & nanotechnology, [SDE.ES]Environmental Sciences/Environmental and Society, Synchrotron, Flyscan method, 0104 chemical sciences, 3. Good health, Beamline, Quantum dot, Optoelectronics, 0210 nano-technology, business, theranostic vectors
Abstract

International audience; The new rapid scan method, Flyscan mode, implemented on the DiffAbs beamline at Synchrotron SOLEIL, allows fast micro-X-ray fluorescence data acquisition. It paves the way for applications in the biomedical field where a large amount of data is needed to generate meaningful information for the clinician. This study presents a complete set of data acquired after injection of gold-cluster-enriched mesoporous silica nanospheres, used as potential theranostic vectors, into rats. While classical X-ray fluorescence investigations (using step-by-step acquisitions) are based on a limited number of samples (approximately one per day at the DiffAbs beamline), the Flyscan mode has enabled gathering information on the interaction of nanometer-scale vectors in different organs such as liver, spleen and kidney at the micrometer scale, for five rats, in only a single five-day synchrotron shift. Moreover, numerous X-ray absorption near-edge structure spectra, which are beam-time-consuming taking into account the low concentration of these theranostic vectors, were collected

Published
2017

47. The Critical Role of the Atmosphere in Dip-Coating Process

Author

David Grosso, Elisa Bindini, Guillaume Naudin, Marco Faustini, Cédric Boissière, Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux, de Microélectronique et des Nanosciences de Provence (IM2NP), Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Matériaux Hybrides et Procédés (LCMCP-MHP ), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and Aix Marseille Université (AMU)-Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Nanotechnology, dip-coating, 02 engineering and technology, Substrate (electronics), engineering.material, 010402 general chemistry, 01 natural sciences, Dip-coating, Atmosphere, Coating, Deposition (phase transition), Physical and Theoretical Chemistry, Composite material, chemistry.chemical_classification, Thin layers, relative pressure, Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, General Energy, Optical coating, chemistry, thin films, 13. Climate action, engineering, 0210 nano-technology
Abstract

International audience; Dip-coating is a common liquid deposition technique employed in research, but also for industrial production, to obtain polymer, hybrid and inorganic thin layers of controlled thickness. During liquid deposition, the substrate withdrawal speed allows in principle an easy tuning of deposited film thickness (first modeled by Landau and Levich). Yet, experimentally, unexplained thickness irreproducibility or strong fluctuations of the sol-gel films are often observed when coating large substrates, which is a critical issue for optical coatings such as anti-reflective/reflective coatings. In this study, we pointed out for the first time that uncontrolled solvent relative pressure gradients (coming from solvent evaporation) are responsible for these thickness fluctuation issues. We investigated and quantified their impact for various solutions (of sol-gel or polymer), and pointed out that the solvent evaporation rate is not constant but strongly depends on the geometric configuration of the dip-coating experiment. From this understanding, we demonstrated how an accurate tuning of processing atmosphere can provide a very good control on layer thickness in the practical case of the deposition of anti-reflective water repellent coating. In a second example, we used this phenomenon for developing a very easy synthesis strategy leading to giant and controlled thickness gradient profiles.

Published
2017

48. Water-Induced Phase Separation Forming Macrostructured Epitaxial Quartz Films on Silicon

Author

Adrian Carretero-Genevrier, Cédric Boissière, Djawhar Ferrah, Jaume Gazquez, Clément Sanchez, David Grosso, Glenna L. Drisko, Juan Rodríguez-Carvajal, Martí Gich, INL - Hétéroepitaxie et Nanostructures (INL - H&N), Institut des Nanotechnologies de Lyon (INL), École Centrale de Lyon (ECL), Université de Lyon-Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École Supérieure de Chimie Physique Électronique de Lyon (CPE)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-École Centrale de Lyon (ECL), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), College de France foundation, Marie Curie Reintegration Grant [PCIG09-GA-2011-294168], [RyC-2012-11709], Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Institut National des Sciences Appliquées (INSA)-Université de Lyon-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-École Centrale de Lyon (ECL), Institut National des Sciences Appliquées (INSA)-Université de Lyon-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay

Subjects
Materials science, Silicon, business.industry, Doping, chemistry.chemical_element, Nanotechnology, [CHIM.MATE]Chemical Sciences/Material chemistry, Condensed Matter Physics, Epitaxy, Piezoelectricity, Electronic, Optical and Magnetic Materials, law.invention, Biomaterials, Metal, Semiconductor, chemistry, Chemical engineering, law, visual_art, Electrochemistry, visual_art.visual_art_medium, Crystallization, business, Quartz
Abstract

International audience; Quartz has been widely used as a bulk material in optics, the microelectronic industry, and sensors. The nanostructuring and direct integration of oriented quartz crystals onto a semiconductor platform has proven to be challenging. However, here, a new approach is presented to integrate epitaxial quartz films with macroperforations within the range of 500 nm and 1 mu m using chemical solution deposition. This method constitutes an appealing approach to develop piezoelectric mass sensors with enhanced resonance frequencies due to the thickness reduction. Perforated quartz films on (100)-silicon are prepared from amorphous silica films deposited via dip-coating and doped with metal cations that catalyze quartz crystallization. The metal cations are also active in the formation of the macroperforations, which arise due to a phase separation mechanism. Cationic surfactant-anion-metal cation assemblies stabilize droplets of water, creating an indentation in the hydrophilic silica matrix which remains after solvent evaporation. Many cations induce phase separation, including Li+, Na+, Sr2+, Mn2+, Fe2+/Fe3+, Ca2+, Ce3+ and La3+ but only the Sr2+ and Ca2+ cations in this series induce the epitaxial growth of alpha-quartz films under the conditions studied. The combination of sol-gel chemistry and epitaxial growth opens new opportunities for the integration of patterned quartz on silicon.

Published
2014

49. High sensitive mesoporous TiO2-coated love wave device for heavy metal detection

Author

Touria Cohen-Bouhacina, Fabien Moroté, Corinne Dejous, Rafik Kalfat, Ibtissem Gammoudi, Dominique Rebière, Cédric Boissière, Christine Grauby-Heywang, Laurianne Blanc, Laboratoire de l'intégration, du matériau au système (IMS), Université Sciences et Technologies - Bordeaux 1-Institut Polytechnique de Bordeaux-Centre National de la Recherche Scientifique (CNRS), Laboratoire Ondes et Matière d'Aquitaine (LOMA), Université de Bordeaux (UB)-Centre National de la Recherche Scientifique (CNRS), Institut National de Recherche et d'Analyse Physico-Chimique (INRAP), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Projet CMCU - PHC Utique n° 10G1103, ANR-06-ECOT-0004,ENSEIRB,Immunocapteur à ondes de Love ultra-sensible pour la détection rapide de micro-organismes dans l'eau, visant la réalisation d'un dispositif d'alerte(2006), and Université Sciences et Technologies - Bordeaux 1 (UB)-Institut Polytechnique de Bordeaux-Centre National de la Recherche Scientifique (CNRS)

Subjects
Escherichia, Materials science, Transducers, Biomedical Engineering, Biophysics, Nanotechnology, Biosensing Techniques, 02 engineering and technology, Sensitivity and Specificity, 01 natural sciences, Metal, Metals, Heavy, Specific surface area, Escherichia coli, Electrochemistry, [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, Deposition (law), Titanium, TiO2 mesoporous, 010401 analytical chemistry, Acoustics, Equipment Design, General Medicine, Polyelectrolyte, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Love-waves, Heavy metals, Chemical engineering, Biofilms, visual_art, visual_art.visual_art_medium, Degradation (geology), AFM, 0210 nano-technology, Mesoporous material, Porosity, Biosensor, Layer (electronics), Cadmium, Biotechnology
Abstract

International audience; This work deals with the design of a highly sensitive whole cell-based biosensor for heavy metal detection in liquid medium. The biosensor is constituted of a Love wave sensor coated with a polyelectrolyte multilayer (PEM). Escherichia Coli bacteria are used as bioreceptors as their viscoelastic properties are influenced by toxic heavy metals. The acoustic sensor is constituted of a quartz substrate with interdigitated transducers and a SiO2 guiding layer. However, SiO2 shows some degradation when used in a saline medium. Mesoporous TiO2 presents good mechanical and chemical stability and offers a high active surface area. Then, the addition of a thin titania layer dip-coated onto the acoustic path of the sensor is proposed to overcome the silica degradation and to improve the mass effect sensitivity of the acoustic device. \{PEM\} and bacteria deposition, and heavy metal influence, are real time monitored through the resonance frequency variations of the acoustic device. The first polyelectrolyte layer is inserted through the titania mesoporosity, favouring rigid link of the \{PEM\} on the sensor and improving the device sensitivity. Also, the mesoporosity of surface increases the specific surface area which can be occupied and favors the formation of homogeneous PEM. It was found a frequency shift near 20±1kHz for bacteria immobilization with titania film instead of 7±3kHz with bare silica surface. The sensitivity is highlighted towards cadmium detection. Moreover, in this paper, particular attention is given to the immobilization of bacteria and to biosensor lifetime. Atomic Force Microscopy characterizations of the biosurface have been done for several weeks. They showed significant morphological differences depending on the bacterial life time. We noticed that the lifetime of the biosensor is longer in the case of using a mesoporous TiO2 layer.

Published
2014

50. Liquid deposition approaches to self-assembled periodic nanomasks

Author

Glenna L. Drisko, Marco Faustini, Cédric Boissière, David Grosso, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Nanostructure, Fabrication, Materials science, Silicon, Nanomask, business.industry, Mechanical Engineering, Liquid deposition, Metals and Alloys, Nanopattern, chemistry.chemical_element, Nanotechnology, Self-assembly, [CHIM.MATE]Chemical Sciences/Material chemistry, Condensed Matter Physics, Etching, chemistry, Mechanics of Materials, Etching (microfabrication), Deposition (phase transition), Microelectronics, General Materials Science, Fluidics, Photonics, business
Abstract

International audience; The fabrication of two-dimensional high-aspect-ratio nanostructures is becoming an important area of research for its technological implications, for example in photonics, fluidics and microelectronics. Nanopatterned layers prepared by liquid deposition methods and bottom-up approaches are emerging as good candidates due to the diversity of their structures and the fact that they can be applied to large surfaces. We discuss the recent developments of self-assembled nanomasks and how they can be exploited for efficient pattern transfer on silicon. (C) 2013 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Published
2014

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