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Here we report the synthesis of a robust, efficient, and reusable MOF catalyst, MOF\u2010NiH, by adaptively generating and stabilizing dinickel active sites using the bipyridine groups in MOF\u2010253 with the formula of Al(OH)(2,2\u2032\u2010bipyridine\u20105,5\u2032\u2010dicarboxylate) for<jats:italic>Z<\/jats:italic>\u2010selective semihydrogenation of alkynes and selective hydrogenation of C=C bonds in \u03b1,\u03b2\u2010unsaturated aldehydes and ketones. Spectroscopic studies established the dinickel complex (bpy\u22c5<jats:sup>\u2212<\/jats:sup>)Ni<jats:sup>II<\/jats:sup>(<jats:italic>\u03bc<\/jats:italic><jats:sub>2<\/jats:sub>\u2010H)<jats:sub>2<\/jats:sub>Ni<jats:sup>II<\/jats:sup>(bpy\u22c5<jats:sup>\u2212<\/jats:sup>) as the active catalyst. MOF\u2010NiH efficiently catalyzed selective hydrogenation reactions with turnover numbers of up to 192 and could be used in five cycles of hydrogenation reactions without catalyst leaching or significant decrease of catalytic activities. The present work uncovers a synthetic strategy toward solution\u2010inaccessible Earth\u2010abundant bimetallic MOF catalysts for sustainable catalysis.<\/jats:p>","DOI":"10.1002\/anie.202306905","type":"journal-article","created":{"date-parts":[[2023,7,7]],"date-time":"2023-07-07T16:32:19Z","timestamp":1688747539000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":38,"title":["Generation and Stabilization of a Dinickel Catalyst in a Metal\u2010Organic Framework for Selective Hydrogenation Reactions"],"prefix":"10.1002","volume":"62","author":[{"given":"Qing\u2010Yun","family":"Guo","sequence":"first","affiliation":[{"name":"Department of Chemistry The University of Chicago Chicago IL 60637 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zitong","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Chemistry The University of Chicago Chicago IL 60637 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