TY - INPR ID - discovery10205809 N2 - 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. SN - 0002-7863 PB - American Chemical Society UR - https://doi.org/10.1021/jacs.4c17380 JF - Journal of the American Chemical Society A1 - Li, Xin A1 - Hai, Guangtong A1 - Wan, Daniel HC A1 - Liao, Yiwen A1 - Yao, Zhangyi A1 - Zhao, Fenglin A1 - Huang, Lingzhi A1 - Zhou, Jinsong A1 - Li, Gang A1 - Chen, Gao-Feng A1 - Wang, Feng Ryan A1 - Leung, Michael KH A1 - Wang, Haihui TI - Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion Y1 - 2025/02/27/ AV - restricted N1 - This version is the author accepted manuscript. For information on re-use, please refer to the publisher?s terms and conditions. ER -