Lithium-mediated nitrogen reduction to ammonia via the catalytic solid–electrolyte interphase
Abstract
The lithium-mediated nitrogen reduction reaction (LiNRR) produces ammonia in ambient conditions. This electrochemical pathway is dependent on a catalytic solid–electrolyte interphase—a nanoscale passivation layer formed from reductive electrolyte decomposition on the surface of lithium metal. The catalytic solid–electrolyte interphase is a unique nanostructured environment that exists on reactive metal surfaces and intimately influences product selectivity. Here we explore recent progress made in the field of lithium-mediated nitrogen reduction to ammonia, especially in light of growing knowledge about the nature of the catalytic solid–electrolyte interphase. We systematically analyse the observed chemical species and reactions that occur within the solid–electrolyte interphase. We also summarize key developments in kinetic and transport models, as well as highlight the cathodic and complementary anodic reactions. Trends in ammonia selectivities and rates with varying electrolyte compositions, cell designs and operating conditions are extracted and used to articulate a path forward for continued development of lithium-mediated nitrogen reduction to ammonia.
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Acknowledgement
This material is based on work supported by the National Science Foundation (grant no. 2204756). We gratefully acknowledge support from the Resnick Sustainability Institute. K.M. gratefully acknowledges support from the Sloan Foundation. W.C. acknowledges funding support from the Arnold and Mabel Beckman Foundation via a 2022 Arnold O. Beckman Postdoctoral Fellowship in Chemical Sciences. F.R. acknowledges funding support from the Independent Research Fund Denmark (DFF), case no. 0217-00234B. We also thank M. Yusov, C. Klein and G. Lee for productive and helpful feedback and discussions.
Contributions
These authors contributed equally: Wesley Chang, Anukta Jain.
W.C. conducted the initial meta-analysis from literature sources, analysed the data and generated the figures. A.J. brought the manuscript to submission-ready completion with detailed edits. W.C. and A.J. led the majority of the work, with input from the whole group. F.R. helped decide our cell-naming convention. K.M. mentored, edited and financed the work. All authors contributed to manuscript proofreading.
Conflict of Interest
The authors declare no competing interests.
Additional details
- National Science Foundation
- CBET-2204756
- Resnick Sustainability Institute
- Alfred P. Sloan Foundation
- Arnold and Mabel Beckman Foundation
- Danmarks Frie Forskningsfond
- 0217-00234B
- Caltech groups
- Resnick Sustainability Institute