464 results on '"Alain Celzard"'
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2. Investigation of membranes-electrodes assemblies in anion exchange membrane fuel cells (AEMFCs): Influence of ionomer ratio in catalyst layers
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Zarina Turtayeva, Feina Xu, Jérôme Dillet, Kévin Mozet, Régis Peignier, Alain Celzard, and Gaël Maranzana
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AEMFCs (Anion exchange membrane fuel cells) ,Catalyst inks ,CCMs (Catalyst-coated membranes) ,GDEs (Gas-diffusion electrodes) ,Polarization curves ,Water management ,Science (General) ,Q1-390 ,Social sciences (General) ,H1-99 - Abstract
Anion exchange membrane fuel cells (AEMFCs) have recently attracted significant attention as low-cost alternative fuel cells to traditional proton exchange membrane fuel cells because of the possible use of platinum-group metal-free electrocatalysts. Over the past decade, new materials dedicated to the alkaline medium, such as anion exchange membranes (AEMs) and anion exchange ionomers (AEIs), have been developed and studied in AEMFCs. However, only a few AEMs and AEIs are commercially available, and there are no ready-to-use membrane electrodes assemblies (MEAs) with the desired AEMs and AEIs. Consequently, the need to manufacture in-house CCMs or GDEs becomes a reality that we must face.This work deals with the influence of ionomer content on the prepared MEAs with the commercial anion exchange membrane and ionomer from Aemion™ Ionomr Innovations AF1–HNN8–2 and AP1–ENN8/HNN8 respectively and by varying the support (gas diffusion layer or membrane). The prepared MEAs were characterized morphologically by SEM and profilometry, as well as electrochemically by AEMFC polarization curves and cyclic voltammetry. In addition, an attempt to investigate water management was made with and without a reference electrode in the cell to understand the behavior of water in an operating AEMFC. Our results show that CCM-based MEAs can undergo deformation during the anion conversion step, leading to weakening of the membrane and hence faster degradation in the fuel cell. On the contrary, no deformation was observed for the GDEs during the anionic conversion, although the results are poorer due to (i) poor interface contact between membrane and GDE that depends on ionomer ratio in the ink and (ii) a high overpotential at the anode due to the production of water that cannot be effectively evacuated.
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- 2024
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3. Dielectric and Ultrasonic Properties of PDMS/TiO2 Nanocomposites
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Ieva Vanskeviče, Martynas Kinka, Jūras Banys, Jan Macutkevič, Sebastien Schaefer, Algirdas Selskis, Vanessa Fierro, and Alain Celzard
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dielectric permittivity ,Vogel–Fulcher law ,titanium dioxide ,Organic chemistry ,QD241-441 - Abstract
This work presents the dielectric and ultrasonic properties of polydimethylsiloxane (PDMS) nanocomposites filled with titanium dioxide nanoparticles. The dielectric study was performed over a very broad range of frequencies (20 Hz–3 THz). The dielectric permittivity was almost frequency-independent in all the composites at room temperature over the whole range of measurement frequencies, and the dielectric losses were very low under these conditions (less than 2). The dielectric permittivity strongly increases with the nanoparticle concentration according to the Maxwell–Garnet model. Therefore, the investigated composites are suitable for various flexible electronic applications, particularly in the microwave and terahertz frequency ranges. Dielectric dispersion and increased attenuation of ultrasonic waves were observed at lower temperatures (below 280 K) due to the relaxation of polymer molecules at the PDMS/TiO2 interface and in the polymer matrix. The relaxation time followed the Vogel–Vulcher law, while the freezing temperature increased with the titanium dioxide concentration due to interactions between the polymer molecules and nanoparticles. The significant hysteresis in the ultrasonic properties indicated that titanium dioxide acts as a crystallization center. This is confirmed by the correlation between the hysteresis in the ultrasonic properties and the structure of the composites. The small difference in the activation energy values obtained from the ultrasonic and dielectric investigations is related to the fact that the dielectric dispersion is slightly broader than the Debye-type dielectric dispersion.
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- 2024
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4. The Influence of Ink Formulation and Preparation on the Performance of Proton-Exchange Membrane Fuel Cell
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Zarina Turtayeva, Feina Xu, Jérôme Dillet, Kévin Mozet, Régis Peignier, Alain Celzard, and Gaël Maranzana
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catalyst-coated membranes (CCMs) ,catalyst layers (CLs) ,ink formulation and preparation ,physicochemical and electrochemical characterizations ,proton-exchange membrane fuel cells (PEMFCs) ,Technology - Abstract
The fabrication step of the catalyst layer (CL) is important to master in order to achieve good performance in fuel cells. Nevertheless, the final structure of a CL depends on many factors, such as the ink composition and preparation, as well as the order of its preparation steps. However, it is not easy for neophytes to understand the relationship between the composition of the ink with the obtained structure of the catalyst layer and its performance in fuel cells. In this work, a systemic experimental study was carried out in order to qualitatively correlate the performance of the PEMFC with the structure of the catalyst layer by playing on different parameters such as the composition and preparation of the ink and the operating conditions. All of the prepared samples were characterized by electron microscopy and profilometry, as well as by electrochemical tests at a single-cell level. The main results show that (i) the chosen ratio and ingredients result in a catalyst layer structure that can affect the PEMFC performance in different ways, and (ii) the reproducibility of the results requires particular care in the choice of catalyst and carbon support.
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- 2023
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5. Biomass Derived High Porous Carbon via CO2 Activation for Supercapacitor Electrodes
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Azamat Taurbekov, Alisher Abdisattar, Meiram Atamanov, Mukhtar Yeleuov, Chingis Daulbayev, Kydyr Askaruly, Bayan Kaidar, Zulkhair Mansurov, Jimena Castro-Gutierrez, Alain Celzard, Vanessa Fierro, and Tolganay Atamanova
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activated carbon ,supercapacitors ,biowaste derived ,physical activation ,chemical activation ,Technology ,Science - Abstract
In this study, we systematically study the efficient production method and electrochemical characteristics of activated carbons (AC) derived from rice husk (RH) and walnut shell (WS). In particular, the effectiveness of physical activation using carbon dioxide (CO2) was investigated and compared with the more common chemical activation method using potassium hydroxide (KOH). The results show that the KOH–activated samples have remarkable specific capacities, reaching 157.8 F g−1 for RH and 152 F g−1 for WS at 1 A g−1. However, the rate capability of AC obtained via KOH decreases significantly as the scanning rate increases, retaining only 51.5% and 68% of their original capacities for RH–KOH and WS–KOH, respectively, at 20 A g–1. In contrast, CO2–activated samples show a superior rate performance with a capacity retention of 75.6% for WS and 80% for RH at the same current density. In addition, electrochemical impedance spectroscopy (EIS) analysis shows that AC obtained via CO2 has a lower charge transfer resistance compared to its KOH counterparts. CO2–activated RH and WS electrodes show Rct values of 0.1 Ω and 0.24 Ω, respectively, indicating improved ion transport kinetics and surface area utilization. These results highlight the importance of activation techniques in tailoring the electrochemical behavior of biomass–derived carbon. This study not only expands the understanding of the interaction between activation, morphology, and performance but also indicates the potential of CO2 activation as an environmentally friendly and efficient alternative. As the field of sustainable energy storage advances, this work provides valuable guidance for the development of high–performance supercapacitor electrodes with less environmental impact.
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- 2023
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6. Zinc Doping Enhances the Electrocatalytic Properties of Cobalt Borides for the Hydrogen Evolution Reaction
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Javier Quílez-Bermejo, Sergio García-Dalí, Raj Karthik, Rafael Canevesi, María T. Izquierdo, Mélanie Emo, Alain Celzard, and Vanessa Fierro
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Zn doping ,cobalt borides ,HER ,water splitting ,electrolyzer ,General Works - Abstract
Electrochemical water splitting requires new, low-cost cathode electrodes for the hydrogen evolution reaction to enable the worldwide implementation of electrolyzers. Cobalt borides are proposed as one of the most promising materials to overcome the limitations of the commercial electrocatalysts, but the catalytic activity still needs to be improved to be competitive. Here, we report that the introduction of zinc into cobalt boride to produce a ternary cobalt boride is an efficient route to further improve the catalytic activity towards the hydrogen evolution reaction (HER) of cobalt boride. The ternary Co-Zn-B was prepared by an easy chemical reduction method to achieve superior HER electrocatalytic performance with a lower overpotential than the homologous Co-B. The larger surface area, structural order, crystallization degree and, in particular, the different surface chemistry seem to be key factors for this improvement.
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- 2022
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7. Electrocatalytic hydrogen evolution on the noble metal-free MoS2/carbon nanotube heterostructure: a theoretical study
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Farhad Keivanimehr, Sajjad Habibzadeh, Alireza Baghban, Amin Esmaeili, Ahmad Mohaddespour, Amin Hamed Mashhadzadeh, Mohammad Reza Ganjali, Mohammad Reza Saeb, Vanessa Fierro, and Alain Celzard
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Medicine ,Science - Abstract
Abstract Molybdenum disulfide (MoS2) is considered as a promising noble-metal-free electrocatalyst for the Hydrogen Evolution Reaction (HER). However, to effectively employ such material in the HER process, the corresponding electrocatalytic activity should be comparable or even higher than that of Pt-based materials. Thus, efforts in structural design of MoS2 electrocatalyst should be taken to enhance the respective physico-chemical properties, particularly, the electronic properties. Indeed, no report has yet appeared about the possibility of an HER electrocatalytic association between the MoS2 and carbon nanotubes (CNT). Hence, this paper investigates the synergistic electrocatalytic activity of MoS2/ CNT heterostructure for HER by Density Functional Theory simulations. The characteristics of the heterostructure, including density of states, binding energies, charge transfer, bandgap structure and minimum-energy path for the HER process were discussed. It was found that regardless of its configuration, CNT is bound to MoS2 with an atomic interlayer gap of 3.37 Å and binding energy of 0.467 eV per carbon atom, suggesting a weak interaction between CNT and MoS2. In addition, the energy barrier of HER process was calculated lower in MoS2/CNT, 0.024 eV, than in the MoS2 monolayer, 0.067 eV. Thus, the study elaborately predicts that the proposed heterostructure improves the intrinsic electrocatalytic activity of MoS2.
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- 2021
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8. Progress in the Use of Biosourced Phenolic Molecules for Electrode Manufacturing
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Javier Quílez-Bermejo, Sara Pérez-Rodríguez, Alain Celzard, and Vanessa Fierro
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biosourced ,phenolic molecules ,electrodes ,carbon ,energy storage ,Technology - Abstract
In the era of renewable technologies and clean processes, carbon science must adapt to this new model of a green society. Carbon materials are often obtained from petroleum precursors through polluting processes that do not meet the requirements of sustainable and green chemistry. Biomass is considered the only renewable source for the production of carbon materials, as the carbon in biomass comes from the consumption of carbon dioxide from the atmosphere, resulting in zero net carbon dioxide emissions. In addition to being a green source of carbon materials, biomass has many advantages such as being a readily available, large and cheap feedstock, as well as the ability to create unique carbon-derived structures with well-developed porosity and heteroatom doping. All these positive aspects position biomass-derived carbon materials as attractive alternatives in multiple applications, from energy storage to electrocatalysis, via adsorption and biosensors, among others. This review focuses on the application of phenolic resins to the production of electrodes for energy storage and the slow but inexorable movement from petroleum-derived phenolic compounds to biosourced molecules (i.e., lignins, tannins, etc.) as precursors for these carbon materials. Important perspectives and challenges for the design of these biosourced electrodes are discussed.
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- 2022
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9. Structure and electrochemical properties of carbon nanostructures derived from nickel(II) and iron(II) phthalocyanines
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Angela Sanchez-Sanchez, Maria Teresa Izquierdo, Sandrine Mathieu, Jaafar Ghanbaja, Alain Celzard, and Vanessa Fierro
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Medicine (General) ,R5-920 ,Science (General) ,Q1-390 - Abstract
Mesoporous carbons containing up to 3.6 at.% N and 4.4 at.% O and exhibiting graphitic character have been prepared from Ni(II) and Fe(II) phthalocyanines by direct pyrolysis or by HTC + pyrolysis, and subsequently applied as supercapacitor materials. No mesoporous templates or doping post-treatments were used, and the catalytic effect of Ni(II) and Fe(II), naturally present in the precursor molecules, allowed obtaining graphitic carbons at temperatures ≤ 900 °C. Metals were encapsulated in the core of onion–like structures with no contact with the electrolyte, so that electrodes were prevented from degradation during device operation. The materials exhibited high rate capabilities up to 1 V s−1, higher interfacial capacitances than a wide variety of materials possessing higher surface areas, and high capacitance retentions up to 99% at 5 A g−1 current density throughout 10 000 charge–discharge cycles. The electrochemical performances of the phthalocyanine-derived carbons are due to their graphitic character and to the pseudocapacitance contribution of the surface groups through Faradaic reactions. This work opens a new way to obtain carbon materials from a great family of metal phthalocyanines, since the central metal and the radicals of the latter can be varied to tune the carbon properties for specific applications. Keywords: Metal phthalocyanines, Hydrothermal carbonisation, Catalytic graphitisation, Supercapacitors
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- 2020
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10. Electrical Resistivity and Microwave Properties of Carbon Fiber Felt Composites
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Marina Tretjak, Sandra Pralgauskaitė, Jonas Matukas, Artyom Plyushch, Jan Macutkevič, Jūras Banys, Blagoj Karakashov, Vanessa Fierro, and Alain Celzard
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carbon fibers ,electrical resistivity ,electromagnetic shielding ,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
We present studies on the microwave properties, electrical resistivity, and low-frequency (10 Hz–20 kHz) noise characteristics in the temperature range of 78 K to 380 K of composite materials made from bisphenol A-based epoxy resin and carbon fiber felts. Two types of carbon fibers were used, derived from polyacrylonitrile or regenerated cellulose. We show that these structures are suitable for electromagnetic shielding applications, especially in the direction parallel to the carbon fibers. The low-frequency voltage fluctuations observed in these materials are of the 1/fα, and the noise intensity is proportional to the square of the voltage. The characteristics of the investigated materials show an instability in the temperature range from 307 K to 332 K. This effect is followed by an increase in resistivity and noise intensity, but it does not change the character of the noise, and this instability vanishes after a few repeated heating and cooling cycles.
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- 2022
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11. A Review of Rigid Polymeric Cellular Foams and Their Greener Tannin-Based Alternatives
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Antonio M. Borrero-López, Vincent Nicolas, Zelie Marie, Alain Celzard, and Vanessa Fierro
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rigid foams ,tannin-based foams ,polyurethane foams ,phenolic foams ,Organic chemistry ,QD241-441 - Abstract
This review focuses on the description of the main processes and materials used for the formulation of rigid polymer foams. Polyurethanes and their derivatives, as well as phenolic systems, are described, and their main components, foaming routes, end of life, and recycling are considered. Due to environmental concerns and the need to find bio-based alternatives for these products, special attention is given to a recent class of polymeric foams: tannin-based foams. In addition to their formulation and foaming procedures, their main structural, thermal, mechanical, and fire resistance properties are described in detail, with emphasis on their advanced applications and recycling routes. These systems have been shown to possess very interesting properties that allow them to be considered as potential substitutes for non-renewable rigid polymeric cellular foams.
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- 2022
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12. Experimental Design Optimization of Acrylate—Tannin Photocurable Resins for 3D Printing of Bio-Based Porous Carbon Architectures
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Pauline Blyweert, Vincent Nicolas, Vanessa Fierro, and Alain Celzard
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tannin ,porous carbon ,stereolithography ,additive manufacturing ,experimental design ,Organic chemistry ,QD241-441 - Abstract
In this work, porous carbons were prepared by 3D printing formulations based on acrylate–tannin resins. As the properties of these carbons are highly dependent on the composition of the precursor, it is essential to understand this effect to optimise them for a given application. Thus, experimental design was applied, for the first time, to carbon 3D printing. Using a rationalised number of experiments suggested by a Scheffé mixture design, the experimental responses (the carbon yield, compressive strength, and Young’s modulus) were modelled and predicted as a function of the relative proportions of the three main resin ingredients (HDDA, PETA, and CN154CG). The results revealed that formulations containing a low proportion of HDDA and moderate amounts of PETA and CN154CG gave the best properties. Thereby, the optimised carbon structures had a compressive strength of over 5.2 MPa and a Young’s modulus of about 215 MPa. The reliability of the model was successfully validated through optimisation tests, proving the value of experimental design in developing customisable tannin-based porous carbons manufactured by stereolithography.
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- 2022
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13. Energy Storage in Supercapacitors: Focus on Tannin-Derived Carbon Electrodes
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Jimena Castro-Gutiérrez, Alain Celzard, and Vanessa Fierro
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supercapacitors ,energy storage ,porous carbons ,OMCs ,tannins ,Technology - Abstract
Supercapacitors (SCs) are energy storage devices that bridge the gap between batteries and conventional capacitors. They can store more energy than capacitors and supply it at higher power outputs than batteries. These features, combined with high cyclability and long-term stability, make SCs attractive devices for energy storage. SCs are already present in many applications, either in combination with other energy storage devices (mainly batteries), or as autonomous energy sources. Porous carbons are presently used in the electrodes of commercial SCs due to their high surface area and their good conductivity. However, new porous materials are continuously being developed. Herein, an outline of the principles of the energy storage mechanism in SCs is presented as a guide to illustrate the research on porous carbons materials for SC applications. Indeed, an overview of these carbons and their synthesis methods is also presented. In the context of an urgent need to progress toward the development of environmentally friendly technologies and methods, the final part of this review focuses on the studies carried out using biosourced carbon precursors, such as tannins, which are natural polyphenolic molecules. In particular, mimosa tannin-derived carbon materials with controlled micro- and mesoporosity can be produced by methods with lower environmental impact and lower health and safety risks because crosslinkers are not needed to produce resins.
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- 2020
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14. Carbon Monoliths with Hierarchical Porous Structure for All-Vanadium Redox Flow Batteries
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Jose Francisco Vivo-Vilches, Blagoj Karakashov, Alain Celzard, Vanessa Fierro, Ranine El Hage, Nicolas Brosse, Anthony Dufour, and Mathieu Etienne
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vanadium redox flow battery ,hierarchical carbon ,carbon electrode ,porosity ,sucrose-based carbon monolith ,Production of electric energy or power. Powerplants. Central stations ,TK1001-1841 ,Industrial electrochemistry ,TP250-261 - Abstract
Carbon monoliths were tested as electrodes for vanadium redox batteries. The materials were synthesised by a hard-templating route, employing sucrose as carbon precursor and sodium chloride crystals as the hard template. For the preparation process, both sucrose and sodium chloride were ball-milled together and molten into a paste which was hot-pressed to achieve polycondensation of sucrose into a hard monolith. The resultant material was pyrolysed in nitrogen at 750 °C, and then washed to remove the salt by dissolving it in water. Once the porosity was opened, a second pyrolysis step at 900 °C was performed for the complete conversion of the materials into carbon. The products were next characterised in terms of textural properties and composition. Changes in porosity, obtained by varying the proportions of sucrose to sodium chloride in the initial mixture, were correlated with the electrochemical performances of the samples, and a good agreement between capacitive response and microporosity was indeed observed highlighted by an increase in the cyclic voltammetry curve area when the SBET increased. In contrast, the reversibility of vanadium redox reactions measured as a function of the difference between reduction and oxidation potentials was correlated with the accessibility of the active vanadium species to the carbon surface, i.e., was correlated with the macroporosity. The latter was a critical parameter for understanding the differences of energy and voltage efficiencies among the materials, those with larger macropore volumes having the higher efficiencies.
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- 2021
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15. Mechanical and Thermal Behavior of Fibrous Carbon Materials
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Blagoj Karakashov, M’Barek Taghite, Richard Kouitat, Vanessa Fierro, and Alain Celzard
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nonwoven ,carbon felt ,carbon fiber ,compression ,hyperelasticity ,thermal conductivity ,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
The ability of various commercial fibrous carbon materials to withstand stress and conduct heat has been evaluated through experimental and analytical studies. The combined effects of different micro/macro-structural characteristics were discussed and compared. Large differences in mechanical behavior were observed between the different groups or subgroups of fibrous materials, due to the different types of fibers and the mechanical and/or chemical bonds between them. The application of the Mooney–Rivlin model made it possible to determine the elastic modulus of soft felts, with a few exceptions, which were studied in-depth. The possible use of two different mechanical test methods allowed a comparison of the results in terms of elastic modulus obtained under different deformation regimes. The effective thermal conductivity of the same fibrous materials was also studied and found to be much lower than that of a single carbon fiber due to the high porosity, and varied with the bulk density and the fiber organization involving more or less thermal contact resistances. The thermal conductivity of most materials is highly anisotropic, with higher values in the direction of preferential fiber orientation. Finally, the combination of compression and transient thermal conductivity measurement techniques allowed the heat conduction properties of the commercial fibrous carbons to be investigated experimentally when compressed. It was observed that thermal conductivity is strongly affected under compression, especially perpendicular to the main fiber orientation.
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- 2021
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16. An Evaluation of the Impact of the Amount of Potassium Hydroxide on the Porous Structure Development of Activated Carbons
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Mirosław Kwiatkowski, Elżbieta Broniek, Vanessa Fierro, and Alain Celzard
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activated carbons ,adsorption ,porous structure ,biomass-based materials ,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 paper presents the results of an evaluation of the impact of the amount of potassium hydroxide on the obtained porous structure of the activated carbons derived from the shells of pistachios, hazelnuts, and pecans by carbonization and subsequent chemical activation with potassium hydroxide by different adsorption methods: Brunauer–Emmett–Teller, Dubinin–Raduskevich, the new numerical clustering-based adsorption analysis, Quenched Solid Density Functional Theory, and 2D-Non-linear Density Functional Theory for Heterogeneous Surfaces, applied to nitrogen adsorption isotherms at −196 °C. Based on the conducted research, a significant potential for the production of activated carbons from waste materials, such as nut shells, has been demonstrated. All the activated carbons obtained in the present study at the activator/char mass ratio R = 4 exhibited the most developed porous structure, and thus very good adsorption properties. However, activated carbons obtained from pecan shells deserve special attention, as they were characterized by the most homogeneous surface among all the samples analyzed, i.e., by a very desirable feature in most adsorption processes. The paper demonstrates the necessity of using different methods to analyze the porous structure of activated carbons in order to obtain a complete picture of the studied texture. This is because only a full spectrum of information allows for correctly selecting the appropriate technology and conditions for the production of activated carbons dedicated to specific industrial applications. As shown in this work, relying only on the simplest methods of adsorption isotherm analysis can lead to erroneous conclusions due to lack of complete information on the analyzed porous structure. This work thus also explains how and why the usual characterizations of the porous structure of activated carbons derived from lignocellulosic biomass should not be taken at face value. On the contrary, it is advisable to cross reference several models to get a precise idea of the adsorbent properties of these materials, and therefore to propose the most suitable production technology, as well as the conditions of the preparation process.
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- 2021
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17. Noise and Electrical Characteristics of Composites Filled with Onion-Like Carbon Nanoparticles
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Marina Tretjak, Edita Palaimiene, Sandra Pralgauskaitė, Jonas Matukas, Jūras Banys, Jan Macutkevič, Vanessa Fierro, Sébastien Schaefer, and Alain Celzard
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charge carrier transfer ,composite ,electrical conductivity ,fluctuation ,noise ,onion-like carbon ,Organic chemistry ,QD241-441 - Abstract
Polymer matrix composites filled with carbon nanoparticles are promising materials for many applications, but their properties strongly depend on the particle features, concentration and distribution within the matrix. Here we present a study of the electrical resistivity and the low-frequency voltage fluctuation of composites based on epoxy resin filled with onion-like carbon (OLC) of different sizes (40–250 nm) above the percolation threshold, which should clarify the electrical transport characteristics in these materials. Electrical measurements were performed in the temperature range of 78 to 380 K, and voltage noise analysis was carried out from 10 Hz to 20 kHz. At low temperatures (below 250 K), thermally activated tunneling, variable-range hopping and generation–recombination of charge carriers take place. Above 250 K, the rapid expansion of the matrix with the temperature increases the resistivity, but above ~330 K, the conductivity of the matrix becomes significant. Quasi one-dimensional electrical transport is observed in composites with the smallest particles (40 nm), while in composites with the largest particles (220–250 nm), the dimensionality of the electrical transport is higher. The temperature dependence of the electrical conductivity of composites with smaller particles is more sensitive to matrix expansion.
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- 2021
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18. Control of Light Transmission in a Plasmonic Liquid Metacrystal
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Alexander Zharov, Zacharias Viskadourakis, George Kenanakis, Vanessa Fierro, and Alain Celzard
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liquid metamaterials ,liquid metacrystals ,plasmonic metamaterials ,Chemistry ,QD1-999 - Abstract
In this study, we experimentally demonstrated the control of light transmission through a slab of plasmonic liquid metacrystal by an external electric field. By applying the external static field, we were able to induce macroscopic anisotropy, which caused the polarization-dependent suppression of transmission at resonant frequencies. Such behavior indicates the selective plasmon excitation governed by the orientation of the meta-atoms with respect to the polarization of the electromagnetic wave. The problem of light transmission through a plasmonic liquid metacrystal was analyzed theoretically from first principles, and the obtained results were compared with the experimental data.
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- 2021
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19. New Insights into H2S Adsorption on Graphene and Graphene-Like Structures: A Comparative DFT Study
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Azam Salmankhani, Zohre Karami, Amin Hamed Mashhadzadeh, Mohammad Reza Ganjali, Vahid Vatanpour, Amin Esmaeili, Sajjad Habibzadeh, Mohammad Reza Saeb, Vanessa Fierro, and Alain Celzard
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H2S adsorption ,metal oxide ,graphene-like structures ,Ni-decorated graphene ,DFT ,Organic chemistry ,QD241-441 - Abstract
The efficient removal of pollutants from different environments has been one of the great challenges for scientists in recent years. However, the understanding of the mechanisms underlying this phenomenon is still the subject of passionate debates, mainly due to the lack of experimental tools capable of detecting events at the atomic scale. Herein, a comparative theoretical study was carried out to capture the adsorption of H2S on metal oxide surfaces such as zinc oxide (ZnO) and beryllium oxide (BeO), as well as graphene and Ni-decorated graphene. A simulation based on density-functional theory (DFT) was carried out by adopting General Gradient Approximation (GGA) under the Perdew–Burke–Ernzerhof (PBE) function. The calculations quantified H2S adsorption on the considered metal oxide sheets as well as on the non-decorated graphene having a physical nature. In contrast, H2S adsorbed on Ni-decorated graphene sheet gave an adsorption energy of −1.64 eV due to the interaction of S and Ni atoms through the formation of a covalent bond, proof of chemisorption. It seems that the graphene sheet decorated with Ni atoms is a more suitable adsorbent for H2S molecules than BeO, ZnO, or non-decorated graphene, providing a theoretical basis for future studies.
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- 2020
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20. Improving Water Repellence and Friability of Tannin-Furanic Foams by Oil-Grafted Flavonoid Tannins
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Géraldine Rangel, Hubert Chapuis, Maria-Cecilia Basso, Antonio Pizzi, Clara Delgado-Sanchez, Vanessa Fierro, Alain Celzard, and Christine Gerardin-Charbonnier
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Foam ,Oil-grafted tannin ,Flavonoids ,Water repellency ,Biotechnology ,TP248.13-248.65 - Abstract
Tannin-furanic biobased foams, based on the co-reaction of bark-derived condensed tannins and thermoset furanic polymers, have low thermal conductivity, are self-extinguishing, and have high fire resistance, which allows their development for several industrial uses. One of their main drawbacks, however, is the absorption of water within the foam itself. Another problem is the rather friable surface, which is a definite drawback for some potential applications. In this work, these two problems are minimized or eliminated by introducing a component of oil-grafted tannin in the foam formulation. The incorporation of fatty chains markedly decreased foam friability and increased water repellency in the body of the foams. These properties and the compounds formed by fatty acids grafting onto the tannin flavonoids were extensively tested.
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- 2016
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21. Characterization of Carbon Materials for Hydrogen Storage and Compression
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Giuseppe Sdanghi, Rafael L. S. Canevesi, Alain Celzard, Matthias Thommes, and Vanessa Fierro
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physical adsorption ,characterization ,hydrogen storage ,hydrogen compression ,Organic chemistry ,QD241-441 - Abstract
Carbon materials have proven to be a suitable choice for hydrogen storage and, recently, for hydrogen compression. Their developed textural properties, such as large surface area and high microporosity, are essential features for hydrogen adsorption. In this work, we first review recent advances in the physisorption characterization of nanoporous carbon materials. Among them, approaches based on the density functional theory are considered now standard methods for obtaining a reliable assessment of the pore size distribution (PSD) over the whole range from narrow micropores to mesopores. Both a high surface area and ultramicropores (pore width < 0.7 nm) are needed to achieve significant hydrogen adsorption at pressures below 1 MPa and 77 K. However, due to the wide PSD typical of activated carbons, it follows from an extensive literature review that pressures above 3 MP are needed to reach maximum excess uptakes in the range of ca. 7 wt.%. Finally, we present the adsorption–desorption compression technology, allowing hydrogen to be compressed at 70 MPa by cooling/heating cycles between 77 and 298 K, and being an alternative to mechanical compressors. The cyclic, thermally driven hydrogen compression might open a new scenario within the vast field of hydrogen applications.
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- 2020
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22. Towards Non-Mechanical Hybrid Hydrogen Compression for Decentralized Hydrogen Facilities
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Giuseppe Sdanghi, Gaël Maranzana, Alain Celzard, and Vanessa Fierro
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hydrogen storage ,hydrogen compression ,non-mechanical compressors ,electrochemical compressors ,activated carbons ,Technology - Abstract
The cost of the hydrogen value chain needs to be reduced to allow the widespread development of hydrogen applications. Mechanical compressors, widely used for compressing hydrogen to date, account for more than 50% of the CAPEX (capital expenditure) in a hydrogen refueling station. Moreover, mechanical compressors have several disadvantages, such as the presence of many moving parts, hydrogen embrittlement, and high consumption of energy. Non-mechanical hydrogen compressors have proven to be a valid alternative to mechanical compressors. Among these, electrochemical compressors allow isothermal, and therefore highly efficient, compression of hydrogen. On the other hand, adsorption-desorption compressors allow hydrogen to be compressed through cooling/heating cycles using highly microporous materials as hydrogen adsorbents. A non-mechanical hybrid hydrogen compressor, consisting of a first electrochemical stage followed by a second stage driven by adsorption-desorption of hydrogen on activated carbons, allows hydrogen to be produced at 70 MPa, a value currently required for the development of hydrogen automotive applications. This system has several advantages over mechanical compressors, such as the absence of moving parts and high compactness. Its use in decentralized hydrogen facilities, such as hydrogen refueling stations, can be considered.
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- 2020
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23. Mechanical Properties of C3N Nanotubes from Molecular Dynamics Simulation Studies
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Azam Salmankhani, Zohre Karami, Amin Hamed Mashhadzadeh, Mohammad Reza Saeb, Vanessa Fierro, and Alain Celzard
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C3N nanotubes ,molecular dynamics ,mechanical properties ,nanobuds ,defects ,Chemistry ,QD1-999 - Abstract
Although the properties of carbon nanotubes (CNTs) are very well-known and are still extensively studied, a thorough understanding of other carbon-based nanomaterials such as C3N nanotubes (C3NNTs) is still missing. In this article, we used molecular dynamics simulation to investigate the effects of parameters such as chirality, diameter, number of walls, and temperature on the mechanical properties of C3N nanotubes, C3N nanobuds, and C3NNTs with various kinds of defects. We also modeled and tested the corresponding CNTs to validate the results and understand how replacing one C atom of CNT by one N atom affects the properties. Our results demonstrate that the Young’s modulus of single-walled C3NNTs (SWC3NNTs) increased with diameter, irrespective of the chirality, and was higher in armchair SWC3NNTs than in zigzag ones, unlike double-walled C3NNTs. Besides, adding a second and then a third wall to SWC3NNTs significantly improved their properties. In contrast, the properties of C3N nanobuds produced by attaching an increasing number of C60 fullerenes gradually decreased. Moreover, considering C3NNTs with different types of defects revealed that two-atom vacancies resulted in the greatest reduction of all the properties studied, while Stone–Wales defects had the lowest effect on them.
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- 2020
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24. First Tools for Tannin-Furanic Foams Design
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María Cecilia Basso, Marie-Christine Lagel, Antonio Pizzi, Alain Celzard, and Soliman Abdalla
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Quebracho tannin foams ,Formulation design ,Without formaldehyde ,Reactive effects ,Expansion-hardening processes ,Specific properties ,Biotechnology ,TP248.13-248.65 - Abstract
Formaldehyde-free quebracho tannin foams were prepared for the first time. Several simple formulations have been presented in order to study the capital influence of each component on foaming and therefore on the characteristics of the obtained foams. Incorporation of a non-ionic surfactant leads to smaller cells and a more homogeneous cell size distribution. Cross-linking agents improve the mechanical properties of foams. A combination of different catalysts allows control of the ratio between the expansion/hardening processes. The understanding of the roles and interactions of the different components of formulation make possible the design of tannin foams having specific properties.
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- 2015
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25. MALDI-TOF and 13C NMR Analysis of Tannin–Furanic–Polyurethane Foams Adapted for Industrial Continuous Lines Application
- Author
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Maria Cecilia Basso, Antonio Pizzi, Clement Lacoste, Luc Delmotte, Fahad M. Al-Marzouki, Soliman Abdalla, and Alain Celzard
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polyurethane foams ,phenolic foams ,furan foams ,tannin foams ,copolymerization ,formulations ,Organic chemistry ,QD241-441 - Abstract
Mixed phenolic-polyurethane-type rigid foams were developed using tannin-furfuryl alcohol natural materials co-reacted with polymeric isocyanate in the proportions imposed by the limitations inherent to continuous industrial plants for polyurethane foams. A variety of different copolymerization oligomers formed. Urethanes appeared to have been formed with two flavonoid tannin sites, mainly at the flavonoid hydroxyl group at C3, but also, although less, on the phenolic hydroxyl groups of the flavonoid oligomers. Urethanes are also formed with (i) glyoxal in the formulation, be it pre-reacted or not with the tannin; (ii) with phenolsulfonic acid and (iii) with furfural. This latter one, however, greatly favors reaction with the A-ring of the flavonoids through a methylene bridge rather than reaction with the isocyanate groups to form urethanes. All of the materials appeared to have co-reacted in a manner to form urethane and methylene bridges between all of the main components used. Thus, the tannin, the furfuryl alcohol, the isocyanate, the glyoxal and even the phenol sulfonic acid hardener formed a number of mixed species linked by the two bridge types. Several mixed species comprised of 2, 3 and even 4 co-reacted different components have been observed.
- Published
- 2014
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26. An Enhanced Carbon Capture and Storage Process (e-CCS) Applied to Shallow Reservoirs Using Nanofluids Based on Nitrogen-Rich Carbon Nanospheres
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Elizabeth Rodriguez Acevedo, Farid B. Cortés, Camilo A. Franco, Francisco Carrasco-Marín, Agustín F. Pérez-Cadenas, Vanessa Fierro, Alain Celzard, Sébastien Schaefer, and Agustin Cardona Molina
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adsorption ,carbon capture and storage process (CCS) ,carbon dioxide ,nanofluids ,nanoparticles and shallow reservoirs ,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
The implementation of carbon capture and storage process (CCS) has been unsuccessful to date, mainly due to the technical issues and high costs associated with two main stages: (1) CO2 separation from flue gas and (2) CO2 injection in deep geological deposits, more than 300 m, where CO2 is in supercritical conditions. This study proposes, for the first time, an enhanced CCS process (e-CCS), in which the stage of CO2 separation is removed and the flue gas is injected directly in shallow reservoirs located at less than 300 m, where the adsorptive phenomena control CO2 storage. Nitrogen-rich carbon nanospheres were used as modifying agents of the reservoir porous texture to improve both the CO2 adsorption capacity and selectivity. For this purpose, sandstone was impregnated with a nanofluid and CO2 adsorption was evaluated at different pressures (atmospheric pressure and from 3 × 10−3 MPa to 3.0 MPa) and temperatures (0, 25, and 50 °C). As a main result, a mass fraction of only 20% of nanomaterials increased both the surface area and the molecular interactions, so that the increase of adsorption capacity at shallow reservoir conditions (50 °C and 3.0 MPa) was more than 677 times (from 0.00125 to 0.9 mmol g−1).
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- 2019
- Full Text
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27. Lignin-Based Carbon Nanofibers as Electrodes for Vanadium Redox Couple Electrochemistry
- Author
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Jose Francisco Vivo-Vilches, Alain Celzard, Vanessa Fierro, Isabelle Devin-Ziegler, Nicolas Brosse, Anthony Dufour, and Mathieu Etienne
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electrospinning ,lignin ,carbon nanofibers ,vanadium electrochemistry ,Chemistry ,QD1-999 - Abstract
Three different types of lignin (kraft, organosolv and phosphoric acid lignin) were characterized and tested as precursors of electrospun nanofibers. Polyethylene oxide (PEO) was added as a plasticizer and dimethyl formamide (DMF) employed as a solvent. It was found that the molecular weight of lignin was the key parameter to understand the differences of the mechanical stability of the resultant fiber mats. In the case of kraft lignin (KL), the influence of some changes in the synthetic process was also tested: applied voltage, pretreatment in air or not, and the addition of a small amount of Ketjen black. After pyrolysis in nitrogen flow, the obtained carbon nanofibers (CNFs) were characterized by different techniques to analyze their differences in morphology and surface chemistry. Vanadium electrochemistry in 3M sulfuric acid was used to evaluate the different CNFs. All fibers allowed electrochemical reactions, but we observed that the oxidation of V(II) to V(III) was very sensitive to the nature of the raw material. Materials prepared from kraft and phosphorus lignin showed the best performances. Nevertheless, when 1 wt.% of Ketjen black was added to KL during the electrospinning, the electrochemical performance of the sample was significantly improved and all targeted reactions for an all-vanadium redox flow battery were observed. Therefore, in this work, we demonstrated that CNFs obtained by the electrospinning of lignin can be employed as electrodes for vanadium electrochemistry, and their properties can be tuned to improve their electrochemical properties.
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- 2019
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28. Physical properties of tannin/furanic resin foamed with different blowing agents
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Xinjun Li, Antonio Pizzi, Clément Lacoste, Vanessa Fierro, and Alain Celzard
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Tannin/furanic rigid foam ,Different blowing agents ,Cell size ,Thermal conductivity ,Mechanical property ,Biotechnology ,TP248.13-248.65 - Abstract
Tannin/furanic rigid foam made from raw materials of natural origin could be used to replace polyurethane and phenolic foams in many future applications. In this study, diethyl ether, pentane, and a mixture of the two were used to prepare tannin/furanic foams having different microstructures. It was found that the bulk density of the foam could be significantly extended, up to 180 kg/m3. The cell size of the pentane foam was larger than that of diethyl ether foam with comparable density; however, both presented a sudden increase in cell size when the density decreased. The thermal conductivity and mechanical properties were determined for the two foam types at the same density but different cell size. The minimum thermal conductivity for diethyl ether and pentane foams were presented, along with a suggested method for lowering the thermal conductivity of such foam. Additionally, the results of mechanical tests indicate that cell size does not play a role in compressive strength.
- Published
- 2013
29. Structure and Electromagnetic Properties of Cellular Glassy Carbon Monoliths with Controlled Cell Size
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Andrzej Szczurek, Vanessa Fierro, Artyom Plyushch, Jan Macutkevic, Polina Kuzhir, and Alain Celzard
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cellular monoliths ,glasslike carbon ,porosity ,electrical conductivity ,permittivity ,electromagnetic properties ,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
Electromagnetic shielding is a topic of high importance for which lightweight materials are highly sought. Porous carbon materials can meet this goal, but their structure needs to be controlled as much as possible. In this work, cellular carbon monoliths of well-defined porosity and cell size were prepared by a template method, using sacrificial paraffin spheres as the porogen and resorcinol-formaldehyde (RF) resin as the carbon precursor. Physicochemical studies were carried out for investigating the conversion of RF resin into carbon, and the final cellular monoliths were investigated in terms of elemental composition, total porosity, surface area, micropore volumes, and micro/macropore size distributions. Electrical and electromagnetic (EM) properties were investigated in the static regime and in the Ka-band, respectively. Due to the phenolic nature of the resin, the resultant carbon was glasslike, and the special preparation protocol that was used led to cellular materials whose cell size increased with density. The materials were shown to be relevant for EM shielding, and the relationships between those properties and the density/cell size of those cellular monoliths were elucidated.
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- 2018
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30. Hydrothermal Treatment of Tannin: A Route to Porous Metal Oxides and Metal/Carbon Hybrid Materials
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Flavia L. Braghiroli, Vanessa Fierro, Andrzej Szczurek, Philippe Gadonneix, Jaafar Ghanbaja, Julien Parmentier, Ghouti Medjahdi, and Alain Celzard
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hydrothermal treatment ,tannin ,metal oxide nanoparticles ,hollow microspheres ,iron/carbon hybrid materials ,Inorganic chemistry ,QD146-197 - Abstract
In the present paper, porous materials were prepared from the hydrothermal treatment of aqueous solutions of tannin, a renewable phenolic resource extracted from tree barks, containing dissolved salts of transition metals: V, Cr, Ni and Fe. Hydrothermal treatment produced carbonaceous particles doped with the aforementioned metals, and such materials were treated according to two different routes: (i) calcination in air in order to burn the carbon and to recover porous oxides; (ii) pyrolysis in inert atmosphere so as to recover porous metal/carbon hybrid materials. The nature of the metal salt was found to have a dramatic impact on the structure of the materials recovered by the first route, leading either to nano-powders (V, Cr) or to hollow microspheres (Ni, Fe). The second route was only investigated with iron, leading to magnetic Fe-loaded micro/mesoporous carbons whose texture, pore volumes and surface areas gradually changed with the iron content.
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- 2017
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31. Polycondensation Resins by Flavonoid Tannins Reaction with Amines
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Francisco-Jose Santiago-Medina, Antonio Pizzi, Maria Cecilia Basso, Luc Delmotte, and Alain Celzard
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flavonoid tannin amines reactions ,oligomers distribution ,resins ,MALDI-ToF ,CP-MAS 13C NMR ,Organic chemistry ,QD241-441 - Abstract
Reaction of a condensed flavonoid tannin, namely mimosa tannin extract with a hexamethylene diamine, has been investigated. For that purpose, catechin was also used as a flavonoid model compound and treated in similar conditions. Solid-state cross-polarisation/magic-angle spinning (CP-MAS) carbon 13 nuclear magnetic resonance (13C NMR) and matrix assisted laser desorption ionisation time of flight (MALDI-ToF) mass spectroscopy studies revealed that polycondensation compounds leading to resins were obtained by the reaction of the amines with the phenolic hydroxy groups of the tannin. Simultaneously, a second reaction leading to the formation of ionic bonds between the two groups occurred. These new reactions have been shown to clearly lead to the reaction of several phenolic hydroxyl groups, and flavonoid unit oligomerisation, to form hardened resins.
- Published
- 2017
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32. PLA with Intumescent System Containing Lignin and Ammonium Polyphosphate for Flame Retardant Textile
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Aurélie Cayla, François Rault, Stéphane Giraud, Fabien Salaün, Vanessa Fierro, and Alain Celzard
- Subjects
PLA ,lignin ,ammonium polyphosphate ,flame retardant ,melt spinning ,Organic chemistry ,QD241-441 - Abstract
Using bio-based polymers to replace of polymers from petrochemicals in the manufacture of textile fibers is a possible way to improve sustainable development for the textile industry. Polylactic acid (PLA) is one of the available bio-based polymers. One way to improve the fire behavior of this bio-based polymer is to add an intumescent formulation mainly composed of acid and carbon sources. In order to optimize the amount of bio-based product in the final material composition, lignin from wood waste was selected as the carbon source. Different formulations of and/or ammonium polyphosphate (AP) were prepared by melt extrusion and then hot-pressed into sheets. The thermal properties (thermogravimetric analyses (TGA) and differential scanning calorimetry (DSC)) and fire properties (UL-94) were measured. The spinnability of the various composites was evaluated. The mechanical properties and physical aspect (microscopy) of PLA multifilaments with lignin (LK) were checked. A PLA multifilament with up to 10 wt % of intumescent formulation was processed, and the fire behavior of PLA fabrics with lignin/AP formulation was studied by cone calorimeter.
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- 2016
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33. 3D-Printed Carbons with Improved Properties and Oxidation Resistance
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Pauline Blyweert, Vincent Nicolas, Vanessa Fierro, and Alain Celzard
- Subjects
Renewable Energy, Sustainability and the Environment ,General Chemical Engineering ,Environmental Chemistry ,General Chemistry - Published
- 2023
34. Easy and Support-Free Synthesis of Bimetallic Borates for Boosting the Oxygen Evolution Reaction
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Sergio García-Dalí, Javier Quílez-Bermejo, Raj Karthik, Rafael Luan Sehn Canevesi, María T. Izquierdo, Mélanie Emo, Alain Celzard, Vanessa Fierro, Agence Nationale de la Recherche (France), European Commission, Ministerio de Universidades (España), Universidad de Oviedo, Universidad de Alicante, García Dalí, Sergio, Quílez Bermejo, J., Karthik, Raj, Canevesi, Rafael L. S., Izquierdo Pantoja, María Teresa, Emo, Mélanie, Celzard, Alain, Fierro, Vanessa, Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, and Materiales Carbonosos y Medio Ambiente
- Subjects
Oxygen evolution reaction ,Ensure access to affordable, reliable, sustainable and modern energy for all ,Materials Chemistry ,Electrochemistry ,Energy Engineering and Power Technology ,Chemical Engineering (miscellaneous) ,Electrocatalysts ,Cobalt borates ,Bimetallic borates ,Electrical and Electronic Engineering ,Transition-metal doping - Abstract
5 figures.-- Supporting information available., The sluggish kinetics of the oxygen evolution reaction (OER) is one of the most limiting factors for the development of many “green” electrochemical devices. Expensive ruthenium and iridium oxide electrodes are often used as advanced electrocatalysts to overcome this limitation. However, these materials are rare in nature, which further limit the implementation of this kind of electrochemical device on a global scale. Compounds based on transition metals and boron have proven to be promising alternatives to commercial electrocatalysts due to their high catalytic properties and robust stability under working conditions. However, such compounds are often obtained through expensive synthetic routes that often involve the use of supports, which increases the cost of electrocatalysts. Here, we present an easy and support-free synthesis of bimetallic borates based on the introduction of transition metals into cobalt borates. Depending on the metal, different morphologies, structural order, surface chemistry, and, most importantly, electrocatalytic properties toward the OER have been obtained. Among all the transition metals, nickel is the one that most improves the catalytic activity of cobalt borate for the OER in an alkaline electrolyte. An overpotential of 230 mV, similar to that of commercial and state-of-the-art electrocatalysts, was obtained by using a support-free synthesis route for the preparation of this catalyst., This study was partly supported by the French PIA project “Lorraine Université d’Excellence”, reference ANR-15-IDEX-04-LUE, and the TALiSMAN project funded by ERDF (2019-000214). SGD thanks the Ministerio de Universidades, the European Union, and the University of Oviedo for the financial support (MU-21-UP2021-030 30267158). JQB thanks the Ministerio de Universidades, the European Union, and the University of Alicante for the financial support (MARSALAS21-21).
- Published
- 2023
35. Hydration Mechanisms of Tungsten Trioxide Revealed by Water Adsorption Isotherms and First-Principles Molecular Dynamics Simulations
- Author
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Yann Foucaud, Azza Ben Jannet, Stefano Caramori, Rafael Canevesi, Moncef Said, Alain Celzard, Vanessa Fierro, Michael Badawi, and Mariachiara Pastore
- Subjects
General Energy ,Physical and Theoretical Chemistry ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials - Published
- 2023
36. Green and easy synthesis of P-doped carbon-based hydrogen evolution reaction electrocatalysts
- Author
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Sergio García-Dalí, Javier Quílez-Bermejo, Jimena Castro-Gutiérrez, Niki Baccile, María T. Izquierdo, Alain Celzard, Vanessa Fierro, Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, Materiales Carbonosos y Medio Ambiente, Agence Nationale de la Recherche (France), Université de Lorraine (France), European Commission, Ministerio de Universidades (España), Universidad de Oviedo, Universidad de Alicante, García Dalí, Sergio, Quílez Bermejo, J., Castro Gutiérrez, Jimena, Baccile, Niki, Izquierdo Pantoja, María Teresa, Celzard, Alain, and Fierro, Vanessa
- Subjects
Carbon doping ,Ensure access to affordable, reliable, sustainable and modern energy for all ,General Materials Science ,General Chemistry ,Phosphorus-doped carbon ,Hydrogen evolution reaction - Abstract
7 figures, 1 table.-- Supplementary information available. © 2023. This manuscript version is made available under the CC-BY-NC-ND 4.0 license https://creativecommons.org/licenses/by-nc-nd/4.0/, In this study, efficient electrodes for the hydrogen evolution reaction (HER) based on low-cost and metal-free carbon catalysts are presented. Phytic acid, a biosourced molecule containing carbon (C) and phosphorus (P), was found to be an excellent precursor for producing carbon materials with high P content, depending on the carbonization temperature, from 27.9 wt% at 700 °C to 7.3 wt% at 1000 °C. A green and easy route to produce P-doped carbon materials by heat treatment of this biosourced precursor without the need for additional reagents is thus proposed. We show that the conversion of P-O-type groups into P-C-type species is of paramount importance for improving the catalytic activity in HER of P-doped carbon materials. P-C-type groups appear to be the key factor in the electrocatalytic activity, reaching an onset potential of - 0.27 V. This study sheds light on the origin of the catalytic activity of P-doped carbons, in which P is expected to modify the homogenous distribution of the electron density of undoped carbons and increase their catalytic performance., This study was partially supported by the French PIA project “Lorraine Université d’Excellence”, reference ANR-15-IDEX-04-LUE, and the TALiSMAN and TALisMAN2 projects funded by ERDF. SGD thanks the Ministerio de Universidades, the European Union, and the University of Oviedo for the financial support (MU-21-UP2021-030 30267158). JQB thanks the Ministerio de Universidades, the European Union, and the University of Alicante for the financial support (MARSALAS21-21).
- Published
- 2023
37. Pyrolysis temperature dependence of sodium storage mechanism in non-graphitizing carbons
- Author
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Hélène Tonnoir, Da Huo, Carine Davoisne, Alain Celzard, Vanessa Fierro, Damien Saurel, Mimoun El Marssi, Manal Benyoussef, Philippe Meunier, Raphaël Janot, Laboratoire réactivité et chimie des solides - UMR CNRS 7314 (LRCS), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie et des Matériaux Paris-Est (ICMPE), Institut de Chimie du CNRS (INC)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Advanced Lithium Energy Storage Systems - ALISTORE-ERI (ALISTORE-ERI), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Réseau sur le stockage électrochimique de l'énergie (RS2E), Aix Marseille Université (AMU)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Nantes Université (Nantes Univ)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), CIC ENERGIGUNE - Parque Tecnol Alava, Laboratoire de Physique de la Matière Condensée - UR UPJV 2081 (LPMC), and Université de Picardie Jules Verne (UPJV)
- Subjects
In situ Raman spectroscopy ,Sodium-ion battery ,Hard carbon ,General Materials Science ,General Chemistry ,SAXS ,[CHIM.MATE]Chemical Sciences/Material chemistry ,Porosity - Abstract
International audience; Hard carbons are the most investigated materials as negative electrode for Na-ion batteries, although the exact mechanism of sodium storage remains under debate. This work is focused on the study of the sodiation mechanism of non-graphitizing carbons (NGC) prepared in a wide range of pyrolysis temperatures (1000 °C–2500 °C), thus covering the whole range from hard carbons (HC) to glassy carbons (GC). Structural and textural characterizations show that increasing the pyrolysis temperature leads to NGCs with a more ordered structure, containing fewer heteroatoms and structural defects, and particularly leads to a developed closed microporosity. In this work, in situ Raman spectroscopy at different excitation wavelengths is used to clarify the mechanism of electrochemical sodiation: it is revealed that the intercalation of Na+ between the graphene layers occurs mainly during the sloping part of the galvanostatic profile, whereas the plateau at low voltage (below 0.1 V vs. Na+/Na) can be associated with the filling of micropores with sodium.
- Published
- 2023
38. Tannin-Based Resins for 3D printing of Porous Carbon Architectures
- Author
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Pauline Blyweert, Vincent Nicolas, Jan Macutkevic, Vanessa Fierro, and Alain Celzard
- Subjects
Renewable Energy, Sustainability and the Environment ,General Chemical Engineering ,Environmental Chemistry ,General Chemistry - Published
- 2022
39. Piezoelectric Nanogenerators Based On BaTiO3 /PDMS Composites for High-Frequency Applications
- Author
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Darya Meisak, Martynas Kinka, Artyom Plyushch, Jan Macutkevič, Aleksej Zarkov, Sébastien Schaefer, Algirdas Selskis, Vytautas Samulionis, Polina Kuzhir, Ju̅ras Banys, Vanessa Fierro, Alain Celzard, Vilnius University [Vilnius], Institut Jean Lamour (IJL), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Center for Physical Sciences and Technology [Vilnius] (FTMC), University of Eastern Finland, NATO Science for Peace and Security Program (Grant G5697 CERTAIN 'Globular carbon-based structures and metamaterials for enhanced electromagnetic protection'), Research Council of Lithuania (LMTLT), agreement no S-PD-22-90, Academy of Finland via the Flagship Programme Photonics Research and Innovation (PREIN), decision 320166, and European Project: 823728 ,DiSeTCom
- Subjects
[PHYS]Physics [physics] ,General Chemical Engineering ,Nanoparticles ,Piezoelectrics ,[CHIM]Chemical Sciences ,General Chemistry ,Insulators ,Glass transition ,Composites - Abstract
International audience; A series of highly flexible and environmentally friendly composites based on polydimethylsiloxane (PDMS) filled with 200 nm size ferroelectric BaTiO3 (BTO) particles at different concentrations (from 7 to 23 vol %) have been fabricated by a simple dispersion method. The dielectric, piezoelectric, and ultrasonic properties have been studied. The ferroelectric state of BTO was confirmed by differential scanning calorimetry and ultrasonic spectroscopy. The addition of BTO into PDMS strongly affects the dielectric properties of the composites. At low temperatures close to 160 K, the PDMS matrix exhibits a dielectric anomaly related to a dynamic glass transition, which shifts to higher temperatures as the BTO content increases due to the strong interaction between polymer chains and nanoparticles. Ultrasonic measurements demonstrate the appearance of a piezoelectricvoltage signal on a thin plate of the composite with the highest available filler concentration (23 vol %) under longitudinal stress applied by a 10 MHz ultrasonic wave. As a result, at room temperature, the detected signal is characterized by output voltage and specific stored energy values of 10 mV and 367.3 MeV/m2, respectively, followed by a further increase with cooling to 35 mV at 150K. The proposed BTO/PDMS composite system is thus a potential candidate for nanogenerators, namely, a simple, flexible, and lead-free device converting high-frequency (10 MHz) mechanical vibrations into electrical voltage.
- Published
- 2023
40. Advanced design of metal nanoclusters and single atoms embedded in C1N1-derived carbon materials for ORR, HER, and OER
- Author
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Javier Quílez‐Bermejo, Sergio García‐Dalí, Ayoub Daouli, Andrea Zitolo, Rafael L.S. Canevesi, Mélanie Emo, María T. Izquierdo, Michael Badawi, Alain Celzard, Vanessa Fierro, European Commission, Ministerio de Universidades (España), Universidad de Alicante, Universidad de Oviedo, Quílez Bermejo, J., García Dalí, Sergio, Zitolo, Andrea, Canevesi, Rafael L. S., Emo, Mélanie, Izquierdo Pantoja, María Teresa, Badawi, Michael, Celzard, Alain, Fierro, Vanessa, Institut Jean Lamour (IJL), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Departamento de Quimica Organica, (ORFEO-CINQA), Universidad de Alicante, Universidad de Oviedo [Oviedo], Laboratoire de Physique et Chimie Théoriques (LPCT), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Instituto de Carboquimica, Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), Ministerio de Universidades, European Union, and University of Alicante for the financial support (MARSALAS21-21), Ministerio de Universidades, European Union, and University of Oviedo for the financial support (MU-21-UP2021-03030267158)., ANR-15-IDEX-0004,LUE,Isite LUE(2015), and European Project: 323300,EC:FP7:Fission,FP7-Fission-2012,TALISMAN(2013)
- Subjects
[PHYS]Physics [physics] ,Metal nanoclusters ,Carbon materials ,Ensure access to affordable, reliable, sustainable and modern energy for all ,Electrocatalysts ,C1N1 ,Condensed Matter Physics ,Electronic, Optical and Magnetic Materials ,Biomaterials ,C 1 N 1 Metal Nanoclusters Single Atoms Electrocatalysts Carbon Materials ,Electrochemistry ,[CHIM]Chemical Sciences ,C 1 N 1 ,Single atoms - Abstract
5 figures.-- Supplementary information available., Single atoms and nanoclusters of Fe, Ni, Co, Cu, and Mn are systematically designed and embedded in a well-defined C1N1-type material that has internal cavities of ≈0.6 nm based on four N atoms. These N atoms serve as perfect anchoring points for the nucleation of small nanoclusters of different metal natures through the creation of metal-nitrogen (TM-N4) bonds. After pyrolysis at 800 °C, TM@CNx-type structures are obtained, where TM is the transition metal and x < 1. Fe@CNx and Co@CNx are the most promising for oxygen reduction reaction and hydrogen evolution reaction, respectively, with a Pt-like performance, and Ni@CNx is the most active for oxygen evolution reaction (OER) with an EOER of 1.59 V versus RHE, far outperforming the commercial IrO2 (EOER = 1.72 V). This systematic and benchmarking study can serve as a basis for the future design of advanced multi-functional electrocatalysts by modulating and combining the metallic nature of nanoclusters and single atoms., ANR-15-IDEX-04-LUE and the TALiSMAN and TALiSMAN2 projects, financed by the European Regional Development Fund (ERDF), are gratefully acknowledged. J.Q.B. thanks the Ministerio de Universidades, the European Union, and the University of Alicante for the financial support (MARSALAS21-21). S.G.D. thanks the Ministerio de Universidades, the European Union, and the University of Oviedo for the financial support (MU-21-UP2021-030 30267158).
- Published
- 2023
41. Manufacturing catalyst-coated membranes by ultrasonic spray deposition for PEMFC: Identification of key parameters and their impact on PEMFC performance
- Author
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Zarina Turtayeva, Feina Xu, Jérôme Dillet, Kévin Mozet, Régis Peignier, Alain Celzard, and Gael Maranzana
- Subjects
Fuel Technology ,Renewable Energy, Sustainability and the Environment ,Energy Engineering and Power Technology ,Condensed Matter Physics - Published
- 2022
42. Modeling High-Pressure Hydrogen Uptake by Nanoporous Metal–Organic Frameworks: Implications for Hydrogen Storage and Delivery
- Author
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Vanessa Fierro, Alain CELZARD, Pamela Ramirez Vidal, and Rafael Canevesi
- Subjects
General Materials Science - Published
- 2022
43. New, 3d Binder-Jetted Carbons with Minimal Periodic Surface Structures
- Author
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Marco Pelanconi, Pauline Blyweert, Giovanni Bianchi, Vincent Nicolas, Davide Viganò, Samuele Bottacin, Vanessa Fierro, Alain Celzard, and Alberto Ortona
- Published
- 2023
44. Recent progress in the development of efficient biomass-based ORR electrocatalysts
- Author
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Anthony Dessalle, Javier Quílez-Bermejo, Vanessa Fierro, Feina Xu, Alain Celzard, Institut Jean Lamour (IJL), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Énergies et Mécanique Théorique et Appliquée (LEMTA ), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Universidad de Alicante, Ministerio de Universidades, the European Union and the University of Alicante for the financial support of his Margarita Salas fellowship (MARSALAS21-21), ANR-15-IDEX-0004,LUE,Isite LUE(2015), European Project: 323300,EC:FP7:Fission,FP7-Fission-2012,TALISMAN(2013), Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, and Materiales Carbonosos y Medio Ambiente
- Subjects
Metal-free catalysts ,Non-precious metal catalysts ,Pt-free electrocatalysts ,General Materials Science ,General Chemistry ,[CHIM.CATA]Chemical Sciences/Catalysis ,Biomass-derived carbon-based electrocatalysts ,Oxygen reduction reaction - Abstract
Platinum is considered the reference catalyst in many electrochemical devices such as electrolyzers or fuel cells. Nevertheless, the large-scale commercialization of these Pt-based devices is limited by the prohibitive cost of platinum as well as its quantity and availability. Regardless of its price and scarcity, it is well known that the oxygen reduction reaction (ORR) with Pt in acidic media is slow compared to that in alkaline media. Due to the lower overpotentials in the latter case, the possibility of using Pt-free catalysts opens the door to new catalyst research. Among them, the development of carbon-based catalysts, either metal-free or with non-precious metals, from the conversion of biomass precursors by various synthetic processes has recently become a challenging goal, as biomass represents an eco-friendly source of carbon. The surface chemistry, textural properties and structure of carbonaceous materials make it complex to identify the origin of ORR catalytic activities. This review provides a critical discussion of the influence of the physicochemical and electrochemical properties of biomass-derived, carbon-based electrocatalysts for the ORR reported over the past decade. This study was partly supported by the French PIA project “Lorraine Université d’Excellence”, reference ANR-15-IDEX-04-LUE and the TALiSMAN project funded by ERDF (2019–000214). JQB thanks the Ministerio de Universidades, the European Union and the University of Alicante for the financial support of his Margarita Salas fellowship (MARSALAS21-21).
- Published
- 2023
45. Eco-Friendly Production of Hyper-Cross-Linked Polymers Using Mechanosynthesis and Bioresources: A Critical Review
- Author
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Antonio María Borrero-López, Vanessa Fierro, Alain CELZARD, Institut Jean Lamour (IJL), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Pro2TecS-Chemical Product and Process Technology Research Centre (Pro2TecS), Universidad de Huelva, Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), European Regional Development Fund (ERDF) projects TALiSMAN and TALiSMAN 2. A.M.B.-L., Margarita Salas grant (SOL-RPU-59), and European Project: 101033964,RFCS
- Subjects
bioresources ,Renewable Energy, Sustainability and the Environment ,green chemistry ,General Chemical Engineering ,Environmental Chemistry ,[CHIM]Chemical Sciences ,General Chemistry ,hyper-cross-linked polymers ,porous materials ,Mechanosynthesis - Abstract
International audience; Hyper-crosslinked polymers (HCPs) are receiving great attention due to their high specific surface area, allowing them to offer high performance in many different applications. However, most of the time, their synthesis requires hazardous and time-consuming protocols, making their implementation and scaling up difficult. To overcome this problem, a relatively old technology such as mechanosynthesis (MS) has gained renewed interest as a greener and faster technology to produce HCPs, which involves much lower energy consumption during the reaction process. In this review, the latest advances on the performance of HCPs based on MS protocols are compiled and analysed, subdivided into those based on Friedel-Crafts alkylation, Scholl coupling reactions and other less common procedures. An analysis of MS versus solvent-based protocols regarding the twelve principles of green chemistry is also reported, as well as a section including a summary of the most recent applications of HCPs. Finally, the use of bio-based precursors for the formulation of HCPs is discussed, thus pooling knowledge for a greener, faster and more widely applicable future development of HCPs.
- Published
- 2022
46. Review on the preparation of carbon membranes derived from phenolic resins for gas separation: From petrochemical precursors to bioresources
- Author
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Vanessa Fierro, Eric Favre, D. Torres, Christophe Castel, Alain Celzard, Laëtitia Cesari, and S. Pérez-Rodríguez
- Subjects
Air separation ,business.industry ,chemistry.chemical_element ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,7. Clean energy ,0104 chemical sciences ,Pressure swing adsorption ,Membrane ,Petrochemical ,chemistry ,Chemical engineering ,13. Climate action ,Natural gas ,General Materials Science ,Amine gas treating ,Gas separation ,0210 nano-technology ,business ,Carbon - Abstract
Membrane processes, whose low energy and operating costs make them competitive for gas separation compared to other conventional methods such as pressure swing adsorption, cryogenic distillation or amine absorption, allows high-purity gas to be obtained in a sustainable and continuous manner. Similarly, resin-derived carbon membranes with molecular sieving properties have improved the selectivity and permeability of conventional dense membranes, as well as having high chemical and thermal resistance. In this review, an overview of the preparation of phenolic resin-based carbon membranes and their performance in gas separation is presented, particularly in processes involving permanent gases such as hydrogen purification, air separation, natural gas/biogas sweetening or carbon dioxide capture. Moreover, bioresources already proven for the synthesis of “greener” phenolic resins and the separation performance of some carbon membranes based on bioresource-derived phenolic resins are also reported and discussed in this work. This review will summarise the development and gas separation performance of phenolic resin-based carbon membranes and will provide a clear future direction in “green” carbon membranes research.
- Published
- 2021
47. 3D printing of carbon-based materials: A review
- Author
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Alain Celzard, Vanessa Fierro, V. Nicolas, and P. Blyweert
- Subjects
Rapid prototyping ,Subtractive color ,Process (engineering) ,Computer science ,business.industry ,3D printing ,chemistry.chemical_element ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Personalization ,chemistry ,On demand ,General Materials Science ,0210 nano-technology ,business ,Process engineering ,Carbon - Abstract
Unlike conventional subtractive methods, 3D printing allows rapid prototyping and customization on demand. However, as a process recently applied to carbon-based materials, 3D printing faces many challenges, including the precise tailoring of the printed material and the control of its porosity, as well as obtaining directly printed (pure) carbon. The present review focuses on the latest advances in carbonaceous materials in 3D printing to address these challenges. A brief introduction to additive manufacturing processes is given, followed by a summary and many recent examples of manufacturing processes, structural characteristics, and applications of various carbon-based composites and carbonaceous materials. Finally, viewpoints and prospects for this emerging field are presented.
- Published
- 2021
48. Resonant absorption in an inhomogeneous disordered metamaterial: First-principles simulation
- Author
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Alexander Zharov, Vanessa Fierro, and Alain Celzard
- Published
- 2022
49. Microwave absorption by carbon-based materials and structures
- Author
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Polina Kuzhir, Alain Celzard, Xiaobo Chen, University of Eastern Finland, Institut Jean Lamour (IJL), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), University of Missouri [Kansas City] (UMKC), University of Missouri System, Academy of Finland via Flagship Program Photonics Research and Innovation (PREIN), Decision No. 32016, Campus France and Lithuanian Science Council through the joint program PHC Gilibert No. 46414VC 'Hybrid gels for electromagnetic applications,', NATO Science for Peace and Security Program [Grant No. G5697 CERTAIN, 'Globular carbon-based structures and metamaterials for enhanced electromagnetic protection']., European Project: 823728 ,DiSeTCom, and European Project: 823878,TERASSE
- Subjects
[PHYS]Physics [physics] ,Microwave absorptions ,microwave ,nanocarbon ,graphene ,Carbohydrates ,General Physics and Astronomy ,Composite materials ,3D printing ,metasurface ,Carbon based materials ,Chemical engineering ,Electromagnetic spectrum ,Electromagnetic compatibility ,carbon nanotube ,absorption ,Mechanosynthesis - Abstract
'Microwave absorption by carbon-based materials and structures' special topic Editorial 
- Published
- 2022
50. Easy enrichment of graphitic nitrogen to prepare highly catalytic carbons for oxygen reduction reaction
- Author
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Javier Quílez-Bermejo, Sara Pérez-Rodríguez, Rafael Canevesi, Daniel Torres, Emilia Morallón, Diego Cazorla-Amorós, Alain Celzard, Vanessa Fierro, Universidad de Alicante. Departamento de Química Física, Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, Electrocatálisis y Electroquímica de Polímeros, and Materiales Carbonosos y Medio Ambiente
- Subjects
Química Inorgánica ,Porous carbons ,Nitrogen ,Graphitic enrichment ,General Materials Science ,Electrocatalysts ,General Chemistry ,Química Física ,Functionalization ,Oxygen reduction reaction - Abstract
One of the biggest challenges in producing fuel cells at affordable prices is to synthesize carbon materials selectively doped with graphitic nitrogen, as it is considered the most active nitrogen species for the oxygen reduction reaction (ORR). So far, all strategies focus on the use of nitrogen-containing carbon precursors, which limits the functionalization of commercially available carbon materials. Here, we present a post-functionalization method to boost the catalytic properties of carbon materials for the ORR by selectively enriching activated carbons with nitrogen graphitic species. A commercial high-surface area activated carbon was post-functionalized by a two-step procedure. First, the commercial carbon was mixed with different carbon/urea weight ratios and heated in air at 350 °C. Then, the functionalized materials were heat-treated at high temperature (from 700 to 1300 °C) to tailor the amount and distribution of the different nitrogen species in the resulting carbon structure. Nitrogen functionalization using a carbon to urea weight ratio of 1:2 and heat-treatment at 1100 °C led to highly selective doping in graphitic nitrogen species, which provided the tools to individually asses the catalytic activity of these nitrogen species. In addition, this study presents a low-cost and easily feasible synthesis route to improve the catalytic activity of carbon materials, leading to an onset potential of almost 0.9 V compared to reversible hydrogen electrode for ORR in an alkaline electrolyte. Moreover, this study provides significant evidence for the key role of graphitic nitrogen. The French research team thanks ANR-15-IDEX-04-LUE and the TALiSMAN project (2019-000215), financed by the European Regional Development Fund (ERDF). The authors from UA thank MICINN and ERDF (project RTI2018-095291-B-I00) for financial support.
- Published
- 2022
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