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. 2022 Sep;609(7928):722-727.
doi: 10.1038/s41586-022-05108-y. Epub 2022 Jul 22.

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

Hoang-Long Du  1   2 , Manjunath Chatti  1   2 , Rebecca Y Hodgetts  1   2 , Pavel V Cherepanov  2 , Cuong K Nguyen  1   2 , Karolina Matuszek  2 , Douglas R MacFarlane  3   4 , Alexandr N Simonov  5   6
Affiliations

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

Hoang-Long Du et al. Nature. 2022 Sep.

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.

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References

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