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Herein, we propose a single\u2010atom interlayer bridge strategy by introducing Au single atoms into layered Bi\n                    <jats:sub>4<\/jats:sub>\n                    O\n                    <jats:sub>5<\/jats:sub>\n                    Br\n                    <jats:sub>2<\/jats:sub>\n                    (AuIB\u2010BOB) to address the above limitations. The incorporated Au atoms substitute Bi sites and are stabilized by a mixed O\/Br coordination environment with an average local structure of Au\n                    <jats:sub>1<\/jats:sub>\n                    O\n                    <jats:sub>3<\/jats:sub>\n                    Br\n                    <jats:sub>2<\/jats:sub>\n                    , forming a covalent bridge between the Br\n                    <jats:sup>\u2212<\/jats:sup>\n                    and [Bi\n                    <jats:sub>4<\/jats:sub>\n                    O\n                    <jats:sub>5<\/jats:sub>\n                    ]\n                    <jats:sup>2+<\/jats:sup>\n                    layers to provide an excellent pathway for cross\u2010layer charge transport. Thus, holes that would otherwise remain confined in the Br\n                    <jats:sup>\u2212<\/jats:sup>\n                    layer are extracted and delivered to the surface O\u2010oxidation sites, while photogenerated electrons are retained and utilized at the surface Bi\u2010reduction sites. This directional charge redistribution considerably suppresses charge recombination, prolonging the average carrier lifetime from 19.5 to 109.7\u00a0ps. Meanwhile, the bridge\u2010mediated charge transport activates the intrinsic Bi reduction sites and O oxidation sites synchronously, promoting CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption\/activation and H\n                    <jats:sub>2<\/jats:sub>\n                    O oxidation\u2010related processes. Without sacrificial agents or photosensitizers, AuIB\u2010BOB achieves a CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010CO evolution rate of 58.21\u00a0\u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    in pure water. This work provides an atomic\u2010level paradigm for regulating cross\u2010layer charge transfer and unlocking intrinsic redox sites in layered photocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.2142051","type":"journal-article","created":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T12:40:03Z","timestamp":1785933603000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Au Single\u2010Atom Interlayer Bridge Promotes Cross\u2010Layer Charge Transport and Intrinsic Catalytic Dual\u2010Sites Activation for Efficient CO\n                    <sub>2<\/sub>\n                    Photoreduction"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-4879-8706","authenticated-orcid":false,"given":"Yutang","family":"Yu","sequence":"first","affiliation":[{"name":"Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral Materials School of Materials Science and Technology China University of Geosciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jingcong","family":"Hu","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Microstructure and Properties of Solids Faculty of Materials and Manufacturing Beijing University of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1579-3264","authenticated-orcid":false,"given":"Fang","family":"Chen","sequence":"additional","affiliation":[{"name":"Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral Materials School of Materials Science and Technology China University of Geosciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-0562-5407","authenticated-orcid":false,"given":"Zijian","family":"Zhu","sequence":"additional","affiliation":[{"name":"Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral Materials School of Materials Science and Technology China University of Geosciences  Beijing China"},{"name":"School of Materials Science and Engineering Peking University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yue","family":"Lu","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Microstructure and Properties of Solids Faculty of Materials and Manufacturing Beijing University of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6105-0851","authenticated-orcid":false,"given":"Jun","family":"Li","sequence":"additional","affiliation":[{"name":"Henan Institute of Advanced Technology School of Chemical Engineering Zhengzhou University  Zhengzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0271-1079","authenticated-orcid":false,"given":"Hongwei","family":"Huang","sequence":"additional","affiliation":[{"name":"Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral Materials School of Materials Science and Technology China University of Geosciences  Beijing 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