eprintid: 10205809 rev_number: 9 eprint_status: archive userid: 699 dir: disk0/10/20/58/09 datestamp: 2025-03-10 14:55:00 lastmod: 2025-03-10 14:55:00 status_changed: 2025-03-10 14:55:00 type: article metadata_visibility: show sword_depositor: 699 creators_name: Li, Xin creators_name: Hai, Guangtong creators_name: Wan, Daniel HC creators_name: Liao, Yiwen creators_name: Yao, Zhangyi creators_name: Zhao, Fenglin creators_name: Huang, Lingzhi creators_name: Zhou, Jinsong creators_name: Li, Gang creators_name: Chen, Gao-Feng creators_name: Wang, Feng Ryan creators_name: Leung, Michael KH creators_name: Wang, Haihui title: Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion ispublished: inpress divisions: UCL divisions: B04 divisions: F43 note: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. 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. date: 2025-02-27 date_type: published publisher: American Chemical Society official_url: https://doi.org/10.1021/jacs.4c17380 full_text_type: other language: eng verified: verified_manual elements_id: 2365427 doi: 10.1021/jacs.4c17380 lyricists_name: Wang, Feng lyricists_id: FWANG76 actors_name: Wang, Feng actors_id: FWANG76 actors_role: owner full_text_status: restricted publication: Journal of the American Chemical Society event_location: United States issn: 0002-7863 citation: Li, Xin; Hai, Guangtong; Wan, Daniel HC; Liao, Yiwen; Yao, Zhangyi; Zhao, Fenglin; Huang, Lingzhi; ... Wang, Haihui; + view all <#> Li, Xin; Hai, Guangtong; Wan, Daniel HC; Liao, Yiwen; Yao, Zhangyi; Zhao, Fenglin; Huang, Lingzhi; Zhou, Jinsong; Li, Gang; Chen, Gao-Feng; Wang, Feng Ryan; Leung, Michael KH; Wang, Haihui; - view fewer <#> (2025) Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion. Journal of the American Chemical Society 10.1021/jacs.4c17380 <https://doi.org/10.1021/jacs.4c17380>. (In press). document_url: https://discovery.ucl.ac.uk/id/eprint/10205809/1/Wang_Revised_manuscript.pdf