Single-site catalysts for electrocatalytic nitrogen activation
Carsten Streb a, Rongji Liu a
a Johannes Gutenberg University Mainz, Staudingerweg 7, Mainz, 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
Oral, Carsten Streb, presentation 036
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.036
Publication date: 16th December 2024

Ammonium nitrate is a key chemical feedstock which is produced by two energy intense processes, that is nitrogen reduction (Haber-Bosch Process) and catalytic ammonia oxidation (Ostwald Process). To-date, in industry, both processes use fossil fuels as energy input and raw materials. In this presentation, we propose the development of (photo-)electrochemically driven reactors capable of coupling the nitrogen-to-ammonium reduction reaction (NRR) and the nitrogen-to nitrate oxidation reaction (NOR), leading to autonomous flow photoreactors for ammonium nitrate production from nitrogen, water, sunlight, and sustainable electricity.

Specifically, we weill report on the development of noble-metal-free single atom catalysts (SACs, 1 metal reaction center) and single-site catalysts (SSCs 2 metal reaction centers) anchored to electrically conductive carbon supports.[1,2] Variation of the SAC/SSC metal sites will allow control of NRR/NOR performance, while metal stabilization in a well-defined all-oxo coordination environment will allow us to tune reactivity. Deposition of these molecular precursors on high-porosity is used to facilitate stable mechanical and electrical linkage between catalyst and electrode. In situ/operando (photo-)electrochemical studies and theoretical modelling will be reported to gain insights into the system performance, selectivity and stability. This will provide insights from the atomic to the reactor-level on the catalytic performance, its limitations, and enable us to identify key optimization parameters.

 

Funding by the Deutsche Forschungsgemeinschaft DFG via Priority Program PP2370 "Nitroconversion" is gratefully acknowledged.

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