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Here, a structure\u2013selectivity relationship of catalysts is pivotal for the control of a highly selective and active CO\n                    <jats:sub>2<\/jats:sub>\n                    RR pathway. We report the fabrication of an oxygen\u2010substituted C\n                    <jats:sub>2<\/jats:sub>\n                    N as metal\u2010free catalyst (O\u2500C\n                    <jats:sub>2<\/jats:sub>\n                    N) for electrochemical CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2500to\u2500CO conversion with tunable O microenvironment. Combined spectroscopic analysis reveals a fine tailored N\u2500C\u2500O moiety in O\u2500C\n                    <jats:sub>2<\/jats:sub>\n                    N, where C\u2500O\u2500C species (e.g., ring in\u2010plane ether) become the dominant oxygen configurations at higher pyrolysis temperatures. Based on experimental observations, a correlation between the exocyclic O\u2010substituted N\u2500C\u2500O\u2500C moieties and CO selectivity is established, giving clear chemical tools for active structure design. The optimized O\u2500C\n                    <jats:sub>2<\/jats:sub>\n                    N electrocatalysts with the dominant appearance of C\u2500O\u2500C moieties exhibit an outstanding 2e\n                    <jats:sup>\u2212<\/jats:sup>\n                    CO\n                    <jats:sub>2<\/jats:sub>\n                    RR performance with a CO selectivity up to 94.8%, which can be well maintained in a practical flow\u2010cell reactor with an adjustable syngas feature.\n                  <\/jats:p>","DOI":"10.1002\/anie.202501896","type":"journal-article","created":{"date-parts":[[2025,3,29]],"date-time":"2025-03-29T04:43:12Z","timestamp":1743223392000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Oxygen\u2010Substituted Porous C\n                    <sub>2<\/sub>\n                    N Frameworks as Efficient Electrocatalysts for Carbon Dioxide Electroreduction"],"prefix":"10.1002","volume":"64","author":[{"given":"Shuai","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Pollution Control and Resources Reuse School of Environmental Science and Engineering Tongji University  1239 Siping Road Shanghai 200092 P.R. 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