Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.106
Publication date: 18th July 2023
Over only few years of intense research, the lithium redox-mediated nitrogen reduction reaction (NRR) has proven to enable electrosynthesis of ammonia at practical yield rates and faradaic efficiencies approaching 100 %. Today, it remains the one and only practical approach towards sustainable electrosynthesis of ammonia. However, further significant research and development efforts are required to translate the redox-mediated NRR into a technology of applied significance, in the first place by addressing the two current major challenges: (i) insufficient stability in operation, and (ii) energy efficiency that is thermodynamically limited to approximately 33% (under standard conditions).
Both of these limitations stem from the need for the operation under strongly reductive conditions defined by the reversible potential of the Li+ + N2 / Li3N redox couple. Under unoptimised conditions, continuous and uncontrollable degradation of the electrolyte solution components results in progressive poisoning of the N2-reducing cathode surface, rapid loss in the performance, and impossibility of passing charge more than few hundred C cm-2 in typically reported experiments. Our research aims to resolve this through understanding the mechanism of operation of the NRR cathodes and design of the electrolyte solutions that prevent reductive degradation pathways while sustaining high rates and faradaic efficiencies of the ammonia production.
The talk will present some of our recent findings in this domain, in particular outcomes of the studies exploring the effects of the chemical nature of the electrolyte, proton carriers and mass-transport on the NRR performance. Feasibility of increasing the energy efficiency of the process will be briefly highlighted.
The financial support from the Australian Research Council (projects FT200100317 and DP200101878) is gratefully acknowledged. Parts of the work were undertaken at the Platypus beamline of the Australian Centre for Neutron Scattering, ANSTO, Monash Centre for Electron Microscopy and Monash X-ray platform.
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