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Anchoring PGM\u2010based materials on supports can not only improve the atomic utilization of active sites but also enhance the intrinsic activity. However, in practical PEM electrolysis, it is still challenging to mediate hydrogen adsorption\/desorption pathways with high coverage of hydrogen intermediates over catalyst surface. Here, operando generated stable palladium (Pd) hydride nanoclusters anchored on tungsten carbide (WC\n                    <jats:sub>x<\/jats:sub>\n                    ) supports were constructed for hydrogen evolution in PEM electrolysis. Under PEM operando conditions, hydrogen intercalation induces formation of Pd hydrides (PdH\n                    <jats:sub>x<\/jats:sub>\n                    ) featuring weakened hydrogen binding energy (HBE), thus triggering reverse hydrogen spillover from WC\n                    <jats:sub>x<\/jats:sub>\n                    (strong HBE) supports to PdH\n                    <jats:sub>x<\/jats:sub>\n                    sites, which have been evidenced by operando characterizations, electrochemical results and theoretical studies. This PdH\n                    <jats:sub>x<\/jats:sub>\n                    \u2010WC\n                    <jats:sub>x<\/jats:sub>\n                    material can be directly utilized as cathode electrocatalysts in PEM electrolysis with ultralow Pd loading of 0.022\u2005mg\u2009cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , delivering the current density of 1\u2005A\u2009cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at the cell voltage of ~1.66\u2005V and continuously running for 200\u2005hours without obvious degradation. This innovative strategy via tuning the operando characteristics to mediate reverse hydrogen spillover provide new insights for designing high\u2010performance supported PGM\u2010based electrocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.202412080","type":"journal-article","created":{"date-parts":[[2024,9,5]],"date-time":"2024-09-05T04:27:05Z","timestamp":1725510425000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":48,"title":["Operando Stable Palladium Hydride Nanoclusters Anchored on Tungsten Carbides Mediate Reverse Hydrogen Spillover for Hydrogen Evolution"],"prefix":"10.1002","volume":"63","author":[{"given":"Hao","family":"Fan","sequence":"first","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and Engineering East China University of Science and Technology  130 Meilong 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Ning","family":"Xu","sequence":"additional","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and Engineering East China University of Science and Technology  130 Meilong Road 200237 Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yao","family":"Lv","sequence":"additional","affiliation":[{"name":"Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine Chemicals School of Chemistry and Molecular Engineering East China University of Science and Technology  130 Meilong Road 200237 Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao Yang","family":"Lin","sequence":"additional","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials School of 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Xiao","family":"Wu","sequence":"additional","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and Engineering East China University of Science and Technology  130 Meilong Road 200237 Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hai Yang","family":"Yuan","sequence":"additional","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and Engineering East China University of Science and Technology  130 Meilong Road 200237 Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sheng","family":"Dai","sequence":"additional","affiliation":[{"name":"Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine Chemicals School of 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