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Here, we propose a precatalyst engineering strategy wherein the crystallographic structure dictates the reconstruction pathway toward targeted active sites. Using bismuth oxyiodide as a model system, we demonstrate that layered BiOI transforms into metallic Bi favorable for the hydrogen evolution reaction. In contrast, the robust three\u2010dimensional framework of non\u2010stoichiometric Bi\n                    <jats:sub>5<\/jats:sub>\n                    O\n                    <jats:sub>7<\/jats:sub>\n                    I structurally preserves iodine, directing its reconstruction into a surface rich in coupled bismuth vacancies and iodine dopants. This uniquely defective configuration achieves a formate Faradaic efficiency of 96.8% at a high current density of 400\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , while demonstrating stable operation for over 100\u00a0h with negligible activity loss at 200\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . Combining in situ characterization with theoretical calculations, we elucidate the structure\u2010dependent evolution mechanism. This work establishes a design principle for bismuth oxyhalide precatalysts to program reconstruction pathways for efficient CO\n                    <jats:sub>2<\/jats:sub>\n                    electroreduction.\n                  <\/jats:p>","DOI":"10.1002\/anie.5655942","type":"journal-article","created":{"date-parts":[[2026,7,6]],"date-time":"2026-07-06T08:16:18Z","timestamp":1783325778000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Precatalyst Engineering Directs Reconstruction Into Coupled Defective Sites for Selective CO\n                    <sub>2<\/sub>\n                    \u2011to\u2011Formate Electroreduction"],"prefix":"10.1002","volume":"65","author":[{"given":"Yi","family":"Cheng","sequence":"first","affiliation":[{"name":"Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoli","family":"Zhao","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Xihua University  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lulu","family":"Li","sequence":"additional","affiliation":[{"name":"Institute of Chemical Research of Catalonia (ICIQ\u2010CERCA) The Barcelona Institute of Science and Technology (BIST)  Tarragona Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lijuan","family":"Yang","sequence":"additional","affiliation":[{"name":"Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruizhe","family":"Yang","sequence":"additional","affiliation":[{"name":"Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu 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