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De l’élaboration de matériaux graphéniques tridimensionnels dopés à l’azote : vers des catalyseurs pour l’électroréduction de l’oxygène sans platine

Abstract : The storage of energy in the form of dihydrogen is attracting growing interest in the scientific community as well as in the energy and transport industries. Proton exchange membrane fuel cells (PEMFC) convert this gas into electricity without harmful emission, at relatively low temperatures. Nowadays, catalysts are mainly made up of platinum nanoparticles, deposited on a microporous carbon material. However, this noble metal is a source of environmental and societal problems, and its supply is subject to geopolitical tensions and vagaries. This thesis work explores the possibility of using alternative materials without metals. Widely studied in the literature, carbon materials doped with nitrogen atoms have a catalytic activity for the oxygen reduction reaction (ORR), this reaction being the most limiting in PEMFCs. An elaboration method based on a solvothermal reaction between an alcohol and sodium, followed by a pyrolysis treatment, has been developed, yielding N-doped graphenic materials with a pronounced three-dimensional aspect and a very developed porosity. The study of the solvothermal reaction between 1-(2-hydroxyethyl)piperidine and sodium allowed to give a description of the reaction mechanism, by focusing on the analysis of the atmosphere composition within the solvothermal reactor during the reaction, and on the characterization of the solid solvothermal product. In addition, the influence of the pyrolysis conditions on the final material was studied using complementary and multi-scale characterization techniques, permitting to elaborate materials with good structural qualities and high specific surfaces. The catalytic activity of doped graphenic materials has been proven inside a PEMFC. Electrical power densities greater than 3 mW.cm-2 have been reached. Several parameters contributing to the improvement of the catalytic activity towards the ORR were identified, allowing to better target the future aspects on which to progress.
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Lilian Moumaneix. De l’élaboration de matériaux graphéniques tridimensionnels dopés à l’azote : vers des catalyseurs pour l’électroréduction de l’oxygène sans platine. Matériaux. Université de Lorraine, 2020. Français. ⟨NNT : 2020LORR0081⟩. ⟨tel-02962872⟩

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