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Herein, for the first time, we demonstrate that TiO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010engineered NH\n                    <jats:sub>2<\/jats:sub>\n                    \u2010MIL\u2010101(Cr) enables strong electronic metal\u2013support interaction (EMSI) to generate confined electron\u2010rich Ni active sites with an ultrafine size of 3.2\u2009nm, thereby markedly accelerating the rate\u2010determining N\u2013H bond activation. As a result, the Ni\/TiO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010NH\n                    <jats:sub>2<\/jats:sub>\n                    \u2010MIL\u2010101 delivers a turnover frequency (TOF) of 422\u2009h\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 343\u2009K for N\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    \u00b7H\n                    <jats:sub>2<\/jats:sub>\n                    O dehydrogenation, 28, 10, and 4 times higher than unsupported Ni NPs (15\u2009h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), Ni\/MIL\u2010101 (42\u2009h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), and Ni\/NH\n                    <jats:sub>2<\/jats:sub>\n                    \u2010MIL\u2010101 (98\u2009h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), respectively, while maintaining 100% H\n                    <jats:sub>2<\/jats:sub>\n                    selectivity and exceptional stability over 20 cycles, outperforming the state\u2010of\u2010the\u2010art nonprecious metal catalysts reported for this reaction. It also exhibits superior catalytic activity and robust durability toward hydrazine borane (N\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    BH\n                    <jats:sub>3<\/jats:sub>\n                    , 15.4 wt%) dehydrogenation, achieving a TOF up to 881\u2009h\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 343\u2009K. These findings demonstrate that TiO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010driven electronic activation of Ni sites in MOFs offers a generalizable support\u2010engineering strategy for efficient and durable hydrogen production from liquid hydrogen\u2010storage materials.\n                  <\/jats:p>","DOI":"10.1002\/cssc.70524","type":"journal-article","created":{"date-parts":[[2026,3,12]],"date-time":"2026-03-12T23:59:53Z","timestamp":1773359993000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["TiO\n                    <sub>2<\/sub>\n                    \u2010Engineered MOFs Activate Electron\u2010Rich Ni Sites for Efficient and Durable Hydrogen Production"],"prefix":"10.1002","volume":"19","author":[{"given":"Tao","family":"Liang","sequence":"first","affiliation":[{"name":"Key Laboratory of Green Catalysis of Jiangxi Education Institutes Key Laboratory of Green Hydrogen and Advanced Catalysis of Jiangxi Province Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education College of Chemistry and Materials Jiangxi Normal University  Nanchang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhengling","family":"Gao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Green Catalysis of Jiangxi Education Institutes Key Laboratory of Green Hydrogen and Advanced Catalysis of Jiangxi Province Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education College of Chemistry and Materials Jiangxi Normal University  Nanchang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7751-5596","authenticated-orcid":false,"given":"Qilu","family":"Yao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Green Catalysis of Jiangxi Education Institutes Key Laboratory of Green Hydrogen and Advanced Catalysis of Jiangxi Province Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education College of Chemistry and Materials Jiangxi Normal University  Nanchang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kun","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Green Catalysis of Jiangxi Education Institutes Key Laboratory of Green Hydrogen and Advanced Catalysis of Jiangxi Province Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education College of Chemistry and Materials Jiangxi Normal University  Nanchang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4828-5108","authenticated-orcid":false,"given":"Gang","family":"Feng","sequence":"additional","affiliation":[{"name":"Key Laboratory for Environment and Energy Catalysis of Jiangxi Province College of Chemistry and Chemical Engineering Nanchang University  Nanchang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6342-0879","authenticated-orcid":false,"given":"Zhang\u2010Hui","family":"Lu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Green Catalysis of Jiangxi Education Institutes Key Laboratory of Green Hydrogen and Advanced Catalysis of Jiangxi Province Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education College of Chemistry and Materials Jiangxi Normal University  Nanchang P. R. 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