Modification of the electrode-electrolyte interfaces of molecular carbon materials for adsorption and electrochemical conversion of dinitrogen and other small molecules
Martin Oschatz a, Konstantin Schutjajew a
a Friedrich Schiller University Jena, Germany, Jena, Germany
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Interlinking heterogeneous catalysts, mechanisms, and reactor concepts for dinitrogen reduction - #Nitroconversion
Sevilla, Spain, 2025 March 3rd - 7th
Organizers: Roland Marschall, Jennifer Strunk and Dirk Ziegenbalg
Invited Speaker, Martin Oschatz, presentation 061
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.061
Publication date: 16th December 2024

The catalytic activation of small molecules/ions such as N2, CO2 or nitrate on the surface of porous electrocatalysts at their interface with electrolytes belongs to the most fundamental phenomena on the way to a more sustainable and decentralized production of commodity chemicals such as ammonia or methanol. Nanoporous carbon materials play an ever increasing role in this regards because adsorption phenomena on the carbon surface are crucial for the working principles of the respective devices. It is well known that the adsorption properties of such materials are a function of their pore architecture. Pore size, pore geometry, pore connectivity, and pore hierarchy determine important factors like mass transport and the strength of interaction with different guest species. Another (and possibly even more powerful) “regulation screw” to control the adsorption properties of nanoporous carbon materials is their atomic construction. The controlled integration of heteroatoms (most often nonmetallic group III or group V and VI elements with nitrogen being the most widely studied heteroatom) into porous sp2-based carbon networks can significantly change their physicochemical properties [1]. This includes but is not limited to their acidity/basicity, oxidation resistance, electric conductivity, and surface polarity. In order to make use of these effects it is important that the heteroatoms are significant in number, that they are uniformly distributed over the bulk of the material, and that the local atomic construction motives are as defined as possible. The synthesis of nitrogen-rich carbon materials by controlled condensation of well-defined nitrogen-rich molecular precursors is a particularly elegant way to synthesize porous carbon materials with large concentrations and precisely incorporated heteroatoms [2].

My presentation will give an overview of current attempts to develop synthetic methods for the precise tailoring of the chemical architecture and pore structure of functional nanoporous carbon materials [2],[3]. Special focus will be on the fabrication of all-carbon hybrid materials which combine a rather heteroatom-rich carbon phase and a pristine porous carbon on the nanoscale to combine, for instance, a demanded chemical property with high electrical conductivity. The structure-property-relationships of these materials in the electrochemical conversion of N2 and nitrate will also be presented [3],[4]. In addition, attempts to modify the adsorption properties of the carbon pores by immobilization of ionic liquids will be presented.

M.O. acknowledges funding by the European Union (ERC, CILCat, project number 101040394). The views and opinions presented are solely those of the author(s) and do not necessarily represent those of the European Union or the European Research Council Executive Agency. The European Union and the granting authority are not liable for any statements made.

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