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However, their assembly through weak van der Waals interactions often results in inefficient charge migration and rapid electron\u2013hole recombination. Hydrogen\u2010bonded organic frameworks (HOFs) offer an alternative strategy to integrate functional clusters into ordered crystalline materials while preserving molecular isolation. Herein, we report the first example of coinage\u2010metal\u2010cluster\u2010based donor\u2013acceptor (D\u2013A) heterojunction engineered into a HOF. A tailored\n                    <jats:bold>\n                      Ag\n                      <jats:sub>6<\/jats:sub>\n                    <\/jats:bold>\n                    cluster serves as the electron\u2010rich donor, and 4,4\u2032\u2010bipyridine (BPY) acts as the electron\u2010deficient acceptor. Directional N\u2500H\u00b7\u00b7\u00b7N hydrogen bonds guide the assembly into a crystalline\n                    <jats:bold>\n                      Ag\n                      <jats:sub>6<\/jats:sub>\n                      \u2010HOF\n                    <\/jats:bold>\n                    , which retains the intrinsic structure of the\n                    <jats:bold>\n                      Ag\n                      <jats:sub>6<\/jats:sub>\n                    <\/jats:bold>\n                    clusters while creating hydrogen\u2010bonded channels for enhanced inter\u2010cluster charge transport. Photoelectrochemical studies and density functional theory calculations reveal an S\u2010scheme heterojunction, with the highest occupied molecular orbital (HOMO) localized on the\n                    <jats:bold>\n                      Ag\n                      <jats:sub>6<\/jats:sub>\n                    <\/jats:bold>\n                    cluster and the lowest unoccupied molecular orbital (LUMO) on the BPY linker. This electronic configuration promotes spatial charge separation, extends visible\u2010light absorption, and significantly boosts photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production compared to the individual components. The work demonstrates hydrogen\u2010bond\u2010directed assembly as a precise and versatile approach to design cluster\u2010based heterojunctional materials with tunable electronic structures and enhanced photocatalytic performance.\n                  <\/jats:p>","DOI":"10.1002\/anie.5527054","type":"journal-article","created":{"date-parts":[[2026,4,24]],"date-time":"2026-04-24T07:23:11Z","timestamp":1777015391000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Engineering Ag\n                    <sub>6<\/sub>\n                    Cluster\u2010Based Donor\u2013Acceptor Heterojunctions Into Hydrogen\u2010Bonded Organic Frameworks for Photocatalytic H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Production"],"prefix":"10.1002","volume":"65","author":[{"given":"Furong","family":"Yuan","sequence":"first","affiliation":[{"name":"Fujian Key Laboratory of Polymer Materials College of Chemistry and Materials Science Fujian Normal University  Fuzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yujuan","family":"Zhuo","sequence":"additional","affiliation":[{"name":"Fujian Key Laboratory of Polymer Materials College of Chemistry and Materials Science Fujian Normal University  Fuzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuai","family":"Chen","sequence":"additional","affiliation":[{"name":"Institute of Inorganic Chemistry University of Bonn  Bonn Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weihua","family":"Deng","sequence":"additional","affiliation":[{"name":"Fujian Key Laboratory of Polymer Materials College of Chemistry and Materials Science Fujian Normal University  Fuzhou P. R. 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China"},{"name":"Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science Zhejiang Normal University  Jinhua P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1264-7648","authenticated-orcid":false,"given":"Zhangjing","family":"Zhang","sequence":"additional","affiliation":[{"name":"Fujian Key Laboratory of Polymer Materials College of Chemistry and Materials Science Fujian Normal University  Fuzhou P. R. 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