Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion

Xin Li, Guangtong Hai, Daniel H.C. Wan, Yiwen Liao, Zhangyi Yao, Fenglin Zhao, Lingzhi Huang, Jinsong Zhou, Gang Li, Gao Feng Chen*, Feng Ryan Wang*, Michael K.H. Leung*, Haihui Wang*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Current nitrate production involves a two-step thermochemical process that is energy-intensive and generates substantial CO2 emissions. Sustainable NO3- production via the nitrogen electrooxidation reaction powered by renewable electricity is highly desirable, but the Faradaic efficiency (FE) at high production rates is unsatisfactory due to competition from the oxygen evolution reaction (OER). In this study, we propose reengineering the catalyst’s microstructure-to-macroenvironment interface by particularly utilizing the previously considered unfavored oxygen from the OER. We demonstrate that the re-engineered interface facilitates a record-breaking FE of 35.52% under 8 atm air, with an impressive increase in FE (41.56%) observed during a continuous electrochemical process lasting for 60 h due to the in situ formation of the O2-rich macro-interface environment. The revelation is anticipated to furnish groundbreaking perspectives for the reaction systems design in electrochemical nitrate production and other electrocatalytic fields.

Original languageEnglish
Pages (from-to)8587-8596
Number of pages10
JournalJournal of the American Chemical Society
Volume147
Issue number10
DOIs
Publication statusPublished - 12 Mar 2025
Externally publishedYes

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Li, X., Hai, G., Wan, D. H. C., Liao, Y., Yao, Z., Zhao, F., Huang, L., Zhou, J., Li, G., Chen, G. F., Wang, F. R., Leung, M. K. H., & Wang, H. (2025). Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion. Journal of the American Chemical Society, 147(10), 8587-8596. https://doi.org/10.1021/jacs.4c17380