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However, the near 100\u2009% Faradaic efficiency (FE) has yet to be achieved due to the complicated reduction route with several intermediates. Here, we report that carbon dioxide (CO<jats:sub>2<\/jats:sub>) can enhance the nitrite electroreduction to ammonia on copper nanowire (Cu NW) catalysts. In a broad potential range (\u22120.7\u223c\u22121.3\u2005V vs. RHE), the FE of nitrite to ammonia is close to 100\u2009% with a 3.5\u2010fold increase in activity compared to that obtained without CO<jats:sub>2.<\/jats:sub> In situ Raman spectroscopy and density functional theory (DFT) calculations indicate that CO<jats:sub>2<\/jats:sub> acts as a catalyst to facilitate the *NO to *N step, which is the rate determining step for ammonia synthesis. The promotion effect of CO<jats:sub>2<\/jats:sub> can be expanded to electroreduction of other nitro\u2010compounds, such as nitrate to ammonia and nitrobenzene to aniline.<\/jats:p>","DOI":"10.1002\/anie.202213711","type":"journal-article","created":{"date-parts":[[2022,11,24]],"date-time":"2022-11-24T12:42:39Z","timestamp":1669293759000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":90,"title":["Nitrite Electroreduction to Ammonia Promoted by Molecular Carbon Dioxide with Near\u2010unity Faradaic Efficiency"],"prefix":"10.1002","volume":"62","author":[{"given":"Yangyang","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Lab of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing P. R. 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