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Here, we develop high\u2010entropy topologically close\u2010packed C15\u2010(IrRh)\n                    <jats:sub>2<\/jats:sub>\n                    PrNdTb nanocrystals with enhanced interatomic hydrogen spillover from oxophilic sites (Pr\/Nd\/Tb) to nucleophilic sites (Ir\/Rh) as efficient HER electrocatalysts for anion exchange membrane water electrolyzers (AEMWEs). Compared to the disordered (A1) counterpart, intermetallic C15\u2010(IrRh)\n                    <jats:sub>2<\/jats:sub>\n                    PrNdTb features a higher coordination number for Pr\/Nd\/Tb and a more electron\u2010rich environment for Ir\/Rh with compressed Ir\u2013Ir(Rh) bonds. In 1.0\u00a0M KOH, C15\u2010(IrRh)\n                    <jats:sub>2<\/jats:sub>\n                    PrNdTb reveals an ultralow HER overpotential of only 8 and 34\u00a0mV to reach 10 and 100\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , respectively. The AEMWE with C15\u2010(IrRh)\n                    <jats:sub>2<\/jats:sub>\n                    PrNdTb cathode delivers an industrial\u2010level current density of 1 A cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at only 1.69\u00a0V, and could be operated stably for over 2000\u00a0h (64 \u00b5V h\n                    <jats:sup>\u22121<\/jats:sup>\n                    loss), representing one of the best alkaline HER catalysts ever reported. The markedly enhanced hydrogen adsorption\/desorption kinetics on C15\u2010(IrRh)\n                    <jats:sub>2<\/jats:sub>\n                    PrNdTb demonstrates an additional active hydrogen migration step via hydrogen spillover during HER. Density functional theory (DFT) calculations indicate that the strong\n                    <jats:italic>d<\/jats:italic>\n                    \u2010\n                    <jats:italic>f<\/jats:italic>\n                    orbital coupling in C15\u2010(IrRh)\n                    <jats:sub>2<\/jats:sub>\n                    PrNdTb establishes efficient interatomic hydrogen spillover pathways through Pr(Nd\/Tb)\u2013Ir(Rh) hollow site to Ir(Rh)\u2013Ir(Rh) bridge site to Ir(Rh)\u2013Ir(Rh) hollow site, thereby accelerating HER kinetics.\n                  <\/jats:p>","DOI":"10.1002\/anie.202517120","type":"journal-article","created":{"date-parts":[[2025,11,3]],"date-time":"2025-11-03T07:20:11Z","timestamp":1762154411000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["High\u2010Entropy Topologically Close\u2010Packed Ir Alloys Enable Interatomic Hydrogen Spillover for Hydrogen Evolution toward High\u2010Performing Anion Exchange Membrane Water Electrolyzers"],"prefix":"10.1002","volume":"65","author":[{"given":"Qiyan","family":"Wu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology  Wuhan 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunan","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology  Wuhan 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuzhe","family":"Cao","sequence":"additional","affiliation":[{"name":"Faculty of Materials Science and Chemistry China University of Geosciences (Wuhan)  Wuhan 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinhui","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Microstructure and Property of Solids Faculty of Materials and Manufacturing Beijing University of Technology  Beijing 100124 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jialun","family":"Mao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology  Wuhan 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuan","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology  Wuhan 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Qu","sequence":"additional","affiliation":[{"name":"PEM Fuel Cell Catalyst Research and Development Center Shenzhen Academy of Aerospace Technology  Shenzhen 518057 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pengfei","family":"Yan","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Microstructure and Property of Solids Faculty of Materials and Manufacturing Beijing University of Technology  Beijing 100124 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhao","family":"Cai","sequence":"additional","affiliation":[{"name":"Faculty of Materials Science and Chemistry China University of Geosciences (Wuhan)  Wuhan 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haifeng","family":"Lv","sequence":"additional","affiliation":[{"name":"PEM Fuel Cell Catalyst Research and Development Center Shenzhen Academy of Aerospace Technology  Shenzhen 518057 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunhui","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; 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