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

Li, Xin; Hai, Guangtong; Wan, Daniel HC; Liao, Yiwen; Yao, Zhangyi; Zhao, Fenglin; Huang, Lingzhi; ... Wang, Haihui; + view all (2025) Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion. Journal of the American Chemical Society 10.1021/jacs.4c17380. (In press).

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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.

Type: Article
Title: Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion
Location: United States
DOI: 10.1021/jacs.4c17380
Publisher version: https://doi.org/10.1021/jacs.4c17380
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10205809
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