Electroreduction of nitrogen with almost 100% current-to-ammonia efficiency

Hoang-Long Du, Manjunath Chatti, Rebecca Y. Hodgetts, Pavel V. Cherepanov, Cuong K. Nguyen, Karolina Matuszek, Douglas R. MacFarlane () and Alexandr N. Simonov ()
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Hoang-Long Du: Monash University
Manjunath Chatti: Monash University
Rebecca Y. Hodgetts: Monash University
Pavel V. Cherepanov: Monash University
Cuong K. Nguyen: Monash University
Karolina Matuszek: Monash University
Douglas R. MacFarlane: Monash University
Alexandr N. Simonov: Monash University

Nature, 2022, vol. 609, issue 7928, 722-727

Abstract: Abstract In addition to its use in the fertilizer and chemical industries1, ammonia is currently seen as a potential replacement for carbon-based fuels and as a carrier for worldwide transportation of renewable energy2. Implementation of this vision requires transformation of the existing fossil-fuel-based technology for NH3 production3 to a simpler, scale-flexible technology, such as the electrochemical lithium-mediated nitrogen-reduction reaction3,4. This provides a genuine pathway from N2 to ammonia, but it is currently hampered by limited yield rates and low efficiencies4–12. Here we investigate the role of the electrolyte in this reaction and present a high-efficiency, robust process that is enabled by compact ionic layering in the electrode–electrolyte interface region. The interface is generated by a high-concentration imide-based lithium-salt electrolyte, providing stabilized ammonia yield rates of 150 ± 20 nmol s−1 cm−2 and a current-to-ammonia efficiency that is close to 100%. The ionic assembly formed at the electrode surface suppresses the electrolyte decomposition and supports stable N2 reduction. Our study highlights the interrelation between the performance of the lithium-mediated nitrogen-reduction reaction and the physicochemical properties of the electrode–electrolyte interface. We anticipate that these findings will guide the development of a robust, high-performance process for sustainable ammonia production.

Date: 2022
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DOI: 10.1038/s41586-022-05108-y

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