@article{discovery10205809, journal = {Journal of the American Chemical Society}, year = {2025}, publisher = {American Chemical Society}, title = {Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion}, note = {This version is the author accepted manuscript. For information on re-use, please refer to the publisher's terms and conditions.}, month = {February}, 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.}, issn = {0002-7863}, url = {https://doi.org/10.1021/jacs.4c17380}, author = {Li, Xin and Hai, Guangtong and Wan, Daniel HC and Liao, Yiwen and Yao, Zhangyi and Zhao, Fenglin and Huang, Lingzhi and Zhou, Jinsong and Li, Gang and Chen, Gao-Feng and Wang, Feng Ryan and Leung, Michael KH and Wang, Haihui} }