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However, establishing strong molecular\u2010level connections between these interfaces to achieve superior interfacial quality presents significant challenges. This study introduces an innovative electrochemical etching method that generates a high concentration of oxygen vacancy sites on BiVO\n                    <jats:sub>4<\/jats:sub>\n                    surfaces (Ov\u2010BiVO\n                    <jats:sub>4<\/jats:sub>\n                    ), enabling interactions with the oxygen\u2010rich ligands of MIL\u2010101. This reduces the formation energy and promotes conformal growth on BiVO\n                    <jats:sub>4<\/jats:sub>\n                    . The Ov\u2010BiVO\n                    <jats:sub>4<\/jats:sub>\n                    \/MIL\u2010101 composite exhibits an ideal semiconductor\/cocatalyst interface, achieving an impressive photocurrent density of 5.91 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at 1.23 V\n                    <jats:sub>RHE<\/jats:sub>\n                    , along with excellent stability. This high\u2010performing photoanode enables an unbiased tandem device with an Ov\u2010BiVO\n                    <jats:sub>4<\/jats:sub>\n                    \/MIL\u2010101\u2010Si solar cell system, achieving a solar\u2010to\u2010hydrogen efficiency of 4.33%. The molecular\u2010level integration mitigates surface states and enhances the internal electric field, facilitating the migration of photogenerated holes into the MIL\u2010101 overlayer. This process activates highly efficient Fe catalytic sites, which effectively adsorb water molecules, lowering the energy barrier for water oxidation and improving interfacial kinetics. Further studies confirm the broad applicability of oxygen vacancy\u2010induced molecular epitaxial growth in various MOFs, offering valuable insights into defect engineering for optimizing interfaces and enhancing photocatalytic activity.\n                  <\/jats:p>","DOI":"10.1002\/adma.202417589","type":"journal-article","created":{"date-parts":[[2025,1,19]],"date-time":"2025-01-19T22:36:36Z","timestamp":1737326196000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":81,"title":["Enhanced Photocatalytic Efficiency Through Oxygen Vacancy\u2010Driven Molecular Epitaxial Growth of Metal\u2013Organic Frameworks on BiVO\n                    <sub>4<\/sub>"],"prefix":"10.1002","volume":"37","author":[{"given":"Yulei","family":"Xin","sequence":"first","affiliation":[{"name":"School of Pharmaceutical and Chemical Engineering Taizhou University  Jiaojiang 318000 P. R. China"}]},{"given":"Jian","family":"Tian","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Shandong University of Science and Technology  Qingdao 266590 P. R. China"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9337-4500","authenticated-orcid":false,"given":"Xianqiang","family":"Xiong","sequence":"additional","affiliation":[{"name":"School of Pharmaceutical and Chemical Engineering Taizhou University  Jiaojiang 318000 P. R. China"}]},{"given":"Chenglin","family":"Wu","sequence":"additional","affiliation":[{"name":"School of Pharmaceutical and Chemical Engineering Taizhou University  Jiaojiang 318000 P. R. China"}]},{"given":"S\u00f3nia A.C.","family":"Carabineiro","sequence":"additional","affiliation":[{"name":"LAQV\u2010REQUIMTE Department of Chemistry NOVA School of Science and Technology Universidade NOVA de Lisboa  Caparica 2829\u2010516 Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1142-3100","authenticated-orcid":false,"given":"Xiaogang","family":"Yang","sequence":"additional","affiliation":[{"name":"Institute of Materials Science and Devices Suzhou University of Science and Technology  Suzhou 215011 P. R. China"}]},{"given":"Zhangxing","family":"Chen","sequence":"additional","affiliation":[{"name":"School of Pharmaceutical and Chemical Engineering Taizhou University  Jiaojiang 318000 P. R. China"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9627-4898","authenticated-orcid":false,"given":"Yang","family":"Xia","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Zhejiang University of Technology  Hangzhou 313200 P. R. 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