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Herein, gradient spin\u2010state Ni\n                    <jats:sub>2<\/jats:sub>\n                    P as cocatalyst simultaneously including spin\u2010electronic configurations of tetra\u2010 (Ni\n                    <jats:sup>2+<\/jats:sup>\n                    \u2500(P)\n                    <jats:sub>4<\/jats:sub>\n                    ) and penta\u2010coordination (Ni\n                    <jats:sup>\u03b4+<\/jats:sup>\n                    \u2013(P)\n                    <jats:sub>5<\/jats:sub>\n                    ) is designed for amplifying In\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>3<\/jats:sub>\n                    polarization by spin\u2010orbit coupling. So photo\u2010generated\n                    <jats:italic>\n                      e\n                      <jats:sup>\u2212<\/jats:sup>\n                    <\/jats:italic>\n                    and\n                    <jats:italic>h<\/jats:italic>\n                    <jats:sup>+<\/jats:sup>\n                    from the In\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>3<\/jats:sub>\n                    photocatalyst vectorially transfer to Ni 2\n                    <jats:italic>p<\/jats:italic>\n                    and In 3\n                    <jats:italic>d<\/jats:italic>\n                    as redox active sites with charge density enhanced to \u22489.48 and 8.52 folds and long lifetime up to 289% (180.39 ns). Observably, energetic chemical adsorption and activation for *H and *OH at Ni 2\n                    <jats:italic>p<\/jats:italic>\n                    and In 3\n                    <jats:italic>d<\/jats:italic>\n                    are completed through electron nimble transfer into the corresponding orbits, performing an activation energy for H\n                    <jats:sub>2<\/jats:sub>\n                    O splitting down to \u224859%. Also, the gradient spin\u2010polarized photocatalytic system with the two regulated electronic structures of Ni\n                    <jats:sub>2<\/jats:sub>\n                    P as cocatalyst presents a remarkable productivity for solar energy conversion into H\n                    <jats:sub>2<\/jats:sub>\n                    of 7.32% at 75\u00a0\u00b0C under AM 1.5 G irradiation through *OH dehydrogenation and *H coupling paths, ranking in one of the best H\n                    <jats:sub>2<\/jats:sub>\n                    \u2010generation catalysts for photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O overall splitting. This research first paves a novel path to completely unlock photocatalytic efficiency through regulating spin\u2010electronic structures of cocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/smll.202508219","type":"journal-article","created":{"date-parts":[[2025,8,23]],"date-time":"2025-08-23T09:52:12Z","timestamp":1755942732000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Regulating Cocatalyst Spin\u2010Electronic Structures for Achieving Solar\u2010To\u2010H\n                    <sub>2<\/sub>\n                    of 7.32% in Photothermal\u2010Catalytic H\n                    <sub>2<\/sub>\n                    O Overall Splitting"],"prefix":"10.1002","volume":"21","author":[{"given":"Yiyuan","family":"Liu","sequence":"first","affiliation":[{"name":"School of Materials Science &amp; Chemical Engineering Ningbo University  Ningbo 315211 P. R. 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