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Although clusters with a high hydride content are particularly intriguing, they present considerable synthetic challenges. Herein, we report two copper hydride clusters,\n                    <jats:bold>\n                      Cu\n                      <jats:sub>18<\/jats:sub>\n                      H\n                      <jats:sub>16<\/jats:sub>\n                    <\/jats:bold>\n                    and\n                    <jats:bold>\n                      Cu\n                      <jats:sub>40<\/jats:sub>\n                      H\n                      <jats:sub>38<\/jats:sub>\n                    <\/jats:bold>\n                    , which exhibit similar layered structures and components, albeit differing in size. The larger\u2010sized\n                    <jats:bold>\n                      Cu\n                      <jats:sub>40<\/jats:sub>\n                      H\n                      <jats:sub>38<\/jats:sub>\n                    <\/jats:bold>\n                    with more hydrides was achieved through ligand\u2010length modulation by replacing 1,2\u2010bis(diphenylphosphino)ethane (dppe) in the synthesis of\n                    <jats:bold>\n                      Cu\n                      <jats:sub>18<\/jats:sub>\n                      H\n                      <jats:sub>16<\/jats:sub>\n                    <\/jats:bold>\n                    with 1,5\u2010bis(diphenylphosphino)pentane (dpppe).\n                    <jats:bold>\n                      Cu\n                      <jats:sub>40<\/jats:sub>\n                      H\n                      <jats:sub>38<\/jats:sub>\n                    <\/jats:bold>\n                    is remarkable for i) the highest number of hydrides among known molecular compounds, ii) the highest number of unligated copper atoms and the highest metal\u2010to\u2010ligand ratio in copper hydride clusters. Moreover, catalytic studies on the selective hydrogenation of \u03b1,\u03b2\u2010unsaturated carbonyl compounds demonstrate that\n                    <jats:bold>\n                      Cu\n                      <jats:sub>40<\/jats:sub>\n                      H\n                      <jats:sub>38<\/jats:sub>\n                    <\/jats:bold>\n                    is a promising catalyst and provide clear structural evidence that a less sterically hindered cluster surface, with a high metal\u2010to\u2010ligand ratio, is beneficial for high\u2010performance catalysis. The findings highlight the importance of surface composition and ligand coverage in catalytic efficiency and offer new avenues for designing high\u2010performance copper hydride cluster catalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.202504671","type":"journal-article","created":{"date-parts":[[2025,4,14]],"date-time":"2025-04-14T23:39:03Z","timestamp":1744673943000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Hydride\u2010Richest Molecular Complex: Ligand\u2010Length Facilitated Cu\n                    <sub>40<\/sub>\n                    H\n                    <sub>38<\/sub>\n                    Nanoclusters Exhibiting High Catalytic Performance for Selective Hydrogenation"],"prefix":"10.1002","volume":"64","author":[{"given":"Jie","family":"Zhou","sequence":"first","affiliation":[{"name":"Department of Chemistry School of Chemistry and Materials Science Jiangsu Normal University  Xuzhou 221116 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wen\u2010Wen","family":"Zhan","sequence":"additional","affiliation":[{"name":"Department of Chemistry School of Chemistry and Materials Science Jiangsu Normal University  Xuzhou 221116 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yan","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemistry School of Chemistry and Materials Science Jiangsu Normal University  Xuzhou 221116 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin\u2010Rui","family":"Gao","sequence":"additional","affiliation":[{"name":"Department of Chemistry School of Chemistry and Materials Science Jiangsu Normal University  Xuzhou 221116 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chengkai","family":"Zhang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Colloid and Interface Chemistry Ministry of Education School of Chemistry and Chemical Engineering State Key Laboratory of Crystal Materials Shandong University  Jinan 250100 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Di","family":"Sun","sequence":"additional","affiliation":[{"name":"Key Laboratory of Colloid and Interface Chemistry Ministry of Education School of Chemistry and Chemical Engineering State Key Laboratory of Crystal Materials Shandong University  Jinan 250100 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yang","family":"Yang","sequence":"additional","affiliation":[{"name":"Department of Chemistry School of Chemistry and Materials Science Jiangsu Normal University  Xuzhou 221116 P.R. 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