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Herein, a novel proton\u2010conducting supramolecular clusters, ([Bi\n                    <jats:sub>6<\/jats:sub>\n                    O\n                    <jats:sub>5<\/jats:sub>\n                    (OH)\n                    <jats:sub>3<\/jats:sub>\n                    ]\n                    <jats:sub>2.24<\/jats:sub>\n                    [PW\n                    <jats:sub>12<\/jats:sub>\n                    O\n                    <jats:sub>40<\/jats:sub>\n                    ]\n                    <jats:sub>1<\/jats:sub>\n                    [NO\n                    <jats:sub>3<\/jats:sub>\n                    ]\n                    <jats:sub>2.4<\/jats:sub>\n                    [H\n                    <jats:sub>3<\/jats:sub>\n                    O]\n                    <jats:sub>5.8<\/jats:sub>\n                    , BPN) has been synthesized and characterized. Molecular dynamics (MD) simulations reveal that charge\u2010assisted dynamic O\u2500H\u22efO hydrogen bonds mediate the supramolecular assembly, while water molecules facilitate proton transport pathways. The material exhibits a maximum proton conductivity of 0.12\u00a0S cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 90\u00a0\u00b0C and 97% (RH) relative humidity, which is comparable to that of Nafion. The spin\u2010lattice relaxation time (\n                    <jats:italic>T<\/jats:italic>\n                    <jats:sub>1<\/jats:sub>\n                    ) of the Bi\u2013O adsorbed protons is significantly shorter than that of the W\u2010O adsorbed protons, indicating that the protons at the Bi\u2013O sites have a higher migration rate.\n                    <jats:sup>1<\/jats:sup>\n                    H magic\u2010angle spinning NMR (\n                    <jats:sup>1<\/jats:sup>\n                    H MAS NMR) and density functional theory (DFT) calculations reveal [Bi\n                    <jats:sub>6<\/jats:sub>\n                    O\n                    <jats:sub>8<\/jats:sub>\n                    ] enhances proton mobility, while [PW\n                    <jats:sub>12<\/jats:sub>\n                    O\n                    <jats:sub>40<\/jats:sub>\n                    ] stabilizes transition states, lowering the activation barrier to 0.14\u00a0eV. The BPN\u2010Nafion hybrid membrane enhances direct methanol fuel cell performance with an open\u2010circuit voltage of 0.82\u00a0V and power density of 86\u00a0mW cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . This integrative design strategy\u2014synergizing inorganic cluster units with dynamic hydrogen\u2010bonding networks\u2014establishes a scalable platform for developing PEMFC materials with programmable proton transport pathways and improved operational stability.\n                  <\/jats:p>","DOI":"10.1002\/anie.202517958","type":"journal-article","created":{"date-parts":[[2025,11,4]],"date-time":"2025-11-04T07:14:36Z","timestamp":1762240476000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":20,"title":["Structural Effects in Polyoxometalate\u2010Based Supramolecular Assemblies for Enhanced Proton Conduction"],"prefix":"10.1002","volume":"65","author":[{"given":"Bo","family":"Hu","sequence":"first","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Faculty of Chemistry Northeast Normal University  Changchun 130024 P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yangguang","family":"Li","sequence":"additional","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Faculty of Chemistry Northeast Normal University  Changchun 130024 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8148-0303","authenticated-orcid":false,"given":"Hong\u2010Ying","family":"Zang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Faculty of Chemistry Northeast Normal University  Changchun 130024 P.R. 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