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However, their low stability hinders the in‐depth study of their intrinsic reactivity and catalytic property accompanying their redox processes. Herein, we demonstrate that a molecular hybrid of an atomically precise {Ag<jats:sub>27</jats:sub>}<jats:sup>17+</jats:sup> nanocluster and polyoxometalates (POMs) can efficiently cleave H<jats:sub>2</jats:sub> into protons and electrons. The Ag nanocluster accommodates electrons through the redox reaction from {Ag<jats:sub>27</jats:sub>}<jats:sup>17+</jats:sup> to {Ag<jats:sub>27</jats:sub>}<jats:sup>13+</jats:sup>, and the POM ligands play the following important roles: (i) a significant stabilization of the typically unstable Ag nanocluster to preserve its structure during the redox reaction with H<jats:sub>2</jats:sub>, (ii) formation of a unique interface between the Ag nanocluster and metal oxides for efficient H<jats:sub>2</jats:sub> cleavage, and (iii) storage of the generated protons on the negatively charged basic surface.</jats:p>"}]}],"creator":[{"@id":"https://cir.nii.ac.jp/crid/1380017288465407236","@type":"Researcher","foaf:name":[{"@value":"Kentaro Yonesato"}],"jpcoar:affiliationName":[{"@value":"Department of Applied Chemistry School of Engineering The University of Tokyo  7-3-1 Hongo, Bunkyo-ku Tokyo 113-8656 Japan"}]},{"@id":"https://cir.nii.ac.jp/crid/1420564276174093568","@type":"Researcher","personIdentifier":[{"@type":"KAKEN_RESEARCHERS","@value":"40510243"},{"@type":"NRID","@value":"1000040510243"},{"@type":"NRID","@value":"9000283618500"},{"@type":"NRID","@value":"9000001732199"},{"@type":"NRID","@value":"9000391904376"},{"@type":"NRID","@value":"9000401809937"},{"@type":"NRID","@value":"9000025065809"},{"@type":"NRID","@value":"9000391891880"},{"@type":"NRID","@value":"9000283618494"},{"@type":"NRID","@value":"9000399497666"},{"@type":"NRID","@value":"9000024940736"},{"@type":"NRID","@value":"9000019143351"},{"@type":"NRID","@value":"9000006877268"},{"@type":"NRID","@value":"9000020135990"},{"@type":"NRID","@value":"9000391883304"},{"@type":"NRID","@value":"9000391879114"},{"@type":"NRID","@value":"9000402010840"},{"@type":"NRID","@value":"9000401808644"},{"@type":"NRID","@value":"9000402010796"},{"@type":"NRID","@value":"9000402010800"},{"@type":"NRID","@value":"9000401800818"},{"@type":"NRID","@value":"9000398139592"},{"@type":"NRID","@value":"9000255703482"},{"@type":"NRID","@value":"9000010667449"},{"@type":"NRID","@value":"9000025106497"},{"@type":"NRID","@value":"9000411249361"},{"@type":"NRID","@value":"9000391872021"},{"@type":"NRID","@value":"9000401809981"},{"@type":"NRID","@value":"9000248964602"},{"@type":"NRID","@value":"9000381959457"},{"@type":"NRID","@value":"9000024968123"},{"@type":"NRID","@value":"9000024967553"},{"@type":"NRID","@value":"9000326638065"},{"@type":"NRID","@value":"9000402445933"},{"@type":"NRID","@value":"9000412110409"},{"@type":"NRID","@value":"9000398270460"},{"@type":"NRID","@value":"9000025123459"},{"@type":"NRID","@value":"9000397820753"},{"@type":"NRID","@value":"9000263064506"},{"@type":"NRID","@value":"9000258731201"},{"@type":"NRID","@value":"9000411249353"},{"@type":"NRID","@value":"9000391856630"},{"@type":"NRID","@value":"9000401809941"},{"@type":"NRID","@value":"9000401975545"},{"@type":"NRID","@value":"9000024967435"},{"@type":"NRID","@value":"9000020394849"},{"@type":"NRID","@value":"9000402009503"},{"@type":"NRID","@value":"9000402023389"},{"@type":"NRID","@value":"9000402001684"},{"@type":"NRID","@value":"9000279889096"},{"@type":"NRID","@value":"9000024961309"},{"@type":"NRID","@value":"9000023260969"},{"@type":"NRID","@value":"9000401791482"},{"@type":"RESEARCHMAP","@value":"https://researchmap.jp/read0154245"}],"foaf:name":[{"@value":"Seiji Yamazoe"}],"jpcoar:affiliationName":[{"@value":"Department of Chemistry Graduate School of Science Tokyo Metropolitan University  1-1 Minami Osawa, Hachioji Tokyo 192-0397 Japan"},{"@value":"Precursory Research for Embryonic Science and Technology (PRESTO) Japan Science and Technology Agency (JST)  4-1-8 Honcho Kawaguchi Saitama 332-0012 Japan"}]},{"@id":"https://cir.nii.ac.jp/crid/1380017288465407235","@type":"Researcher","foaf:name":[{"@value":"Daisuke Yokogawa"}],"jpcoar:affiliationName":[{"@value":"Graduate School of Arts and Science The University of Tokyo  3-8-1 Komaba, Meguro-ku Tokyo 153-8902 Japan"}]},{"@id":"https://cir.nii.ac.jp/crid/1380017288465407234","@type":"Researcher","foaf:name":[{"@value":"Kazuya Yamaguchi"}],"jpcoar:affiliationName":[{"@value":"Department of Applied Chemistry School of Engineering The University of Tokyo  7-3-1 Hongo, Bunkyo-ku Tokyo 113-8656 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Agency (JST)  4-1-8 Honcho Kawaguchi Saitama 332-0012 Japan"}]}],"publication":{"publicationIdentifier":[{"@type":"PISSN","@value":"00448249"},{"@type":"EISSN","@value":"15213757"},{"@type":"PISSN","@value":"14337851"},{"@type":"EISSN","@value":"15213773"}],"prism:publicationName":[{"@value":"Angewandte Chemie"}],"dc:publisher":[{"@value":"Wiley"}],"prism:publicationDate":"2021-06-26","prism:volume":"133","prism:number":"31","prism:startingPage":"17131","prism:endingPage":"17135"},"reviewed":"false","dc:rights":["http://onlinelibrary.wiley.com/termsAndConditions#am","http://onlinelibrary.wiley.com/termsAndConditions#vor"],"url":[{"@id":"https://onlinelibrary.wiley.com/doi/pdf/10.1002/ange.202106786"},{"@id":"https://onlinelibrary.wiley.com/doi/full-xml/10.1002/ange.202106786"},{"@id":"https://onlinelibrary.wiley.com/doi/am-pdf/10.1002/ange.202106786"},{"@id":"https://onlinelibrary.wiley.com/doi/pdf/10.1002/anie.202106786"},{"@id":"https://onlinelibrary.wiley.com/doi/full-xml/10.1002/anie.202106786"},{"@id":"https://onlinelibrary.wiley.com/doi/am-pdf/10.1002/anie.202106786"}],"createdAt":"2021-06-03","modifiedAt":"2023-08-30","project":[{"@id":"https://cir.nii.ac.jp/crid/1040566775672420224","@type":"Project","projectIdentifier":[{"@type":"KAKEN","@value":"20H02749"},{"@type":"JGN","@value":"JP20H02749"},{"@type":"URI","@value":"https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-20H02749/"}],"notation":[{"@language":"ja","@value":"金属ナノクラスター／酸化物ナノ複合体の精密設計と機能開拓"},{"@language":"en","@value":"Precise Design of nano-hybrids of metal nanocluster and oxides"}]},{"@id":"https://cir.nii.ac.jp/crid/1040566775673476352","@type":"Project","projectIdentifier":[{"@type":"KAKEN","@value":"20H04659"},{"@type":"JGN","@value":"JP20H04659"},{"@type":"URI","@value":"https://kaken.nii.ac.jp/grant/KAKENHI-PUBLICLY-20H04659/"}],"notation":[{"@language":"ja","@value":"金属酸化物ソフトクリスタルの精密設計と新展開"}]}],"relatedProduct":[{"@id":"https://cir.nii.ac.jp/crid/1360002214423606016","@type":"Article","resourceType":"学術雑誌論文(journal article)","relationType":["references"],"jpcoar:relatedTitle":[{"@value":"Design of a Silver–Cerium Dioxide Core–Shell Nanocomposite Catalyst for Chemoselective Reduction Reactions"}]},{"@id":"https://cir.nii.ac.jp/crid/1360004229909101952","@type":"Article","resourceType":"学術雑誌論文(journal article)","relationType":["references"],"jpcoar:relatedTitle":[{"@value":"Three‐Dimensional Ordered Arrays of 58×58×58 Å<sup>3</sup> Hollow Frameworks in Ionic Crystals of 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Framework"}]},{"@id":"https://cir.nii.ac.jp/crid/1360572092576768512","@type":"Article","resourceType":"学術雑誌論文(journal article)","relationType":["references"],"jpcoar:relatedTitle":[{"@value":"A protecting group strategy to access stable lacunary polyoxomolybdates for introducing multinuclear metal clusters"}]},{"@id":"https://cir.nii.ac.jp/crid/1360576120813396864","@type":"Article","relationType":["references"],"jpcoar:relatedTitle":[{"@value":"Current State of [FeFe]-Hydrogenase Research: Biodiversity and Spectroscopic Investigations"}]},{"@id":"https://cir.nii.ac.jp/crid/1360576121150287872","@type":"Article","relationType":["references"],"jpcoar:relatedTitle":[{"@value":"[Ag<sub>15</sub>H<sub>13</sub>(DPPH)<sub>5</sub>]<sup>2+</sup> and [Ag<sub>27</sub>H<sub>22</sub>(DPPB)<sub>7</sub>]<sup>3+</sup>: Two New Hydride and Phosphine Co-Protected Clusters and Their Fragmentation Leading to Naked Clusters, Ag<sub>13</sub><sup>+</sup> and 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[{M<sub>2</sub>(OH<sub>2</sub>)<sub>2</sub>}<sub>2</sub>{M(OH<sub>2</sub>)<sub>2</sub>}<sub>4</sub>P<sub>8</sub>W<sub>48</sub>O<sub>176</sub>(OCH<sub>3</sub>)<sub>8</sub>]<sup>16–</sup> (M = Mn, Co, Ni, Cu, Zn)"}]},{"@id":"https://cir.nii.ac.jp/crid/1360861287063726080","@type":"Article","resourceType":"学術雑誌論文(journal article)","relationType":["isReferencedBy"],"jpcoar:relatedTitle":[{"@value":"Variable control of the electronic states of a silver nanocluster <i>via</i> protonation/deprotonation of polyoxometalate ligands"}]},{"@id":"https://cir.nii.ac.jp/crid/1360861704791017728","@type":"Article","resourceType":"学術雑誌論文(journal article)","relationType":["isReferencedBy"],"jpcoar:relatedTitle":[{"@value":"Metal–oxo-cluster-based crystals as solid catalysts"}]},{"@id":"https://cir.nii.ac.jp/crid/1361137044577993728","@type":"Article","relationType":["references"],"jpcoar:relatedTitle":[{"@value":"Atomically Precise Clusters of Noble Metals: Emerging Link between Atoms and 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