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Nevertheless, there is short of systematic studies on the influences of photocatalytic PCET process by regarding the above two factors at the molecular level. Herein, a series of covalent organic framework (COFs)\u00a0(Py\u2010Bd COF, Py\u2010Sa COF and Py\u2010OH\u2010Sa COF) were synthesized by co\u2010controlling charge\u2010distribution of skeletons and microenvironment of pores, and were used as photocatalysts for O\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    and H\n                    <jats:sub>2<\/jats:sub>\n                    O\u2010to\u2010H\n                    <jats:sub>2<\/jats:sub>\n                    reaction. Particularly, the strong electron\u2010withdrawing sulfone groups and strong electron\u2010rich hydroxy groups in Py\u2010OH\u2010Sa COF boosted photo\u2010generated charge separation, also triggered more hydrophilic pores, thus enabling efficient transfer of the photo\u2010induced electrons and protons to catalytic sites. By the above dual regulation, Py\u2010OH\u2010Sa COF showed high photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    yield (4.78\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and H\n                    <jats:sub>2<\/jats:sub>\n                    production (64.21\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ). Moreover, the Py\u2010OH\u2010Sa COF exhibits an extraordinary apparent quantum yield (AQY) of 6.52% and 8.25% at 380 nm for H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    and H\n                    <jats:sub>2<\/jats:sub>\n                    production. This work develops an important strategy for precise regulating PECT by co\u2010regulation of charge\u2010distribution and microenvironment of photocatalyst to enhance catalytic activity, which also offers novel insights for the design anddevelopment of efficient photocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/adma.202507849","type":"journal-article","created":{"date-parts":[[2025,9,30]],"date-time":"2025-09-30T12:53:45Z","timestamp":1759236825000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":62,"title":["Charge\u2010Distribution and Microenvironment Dual Regulation of Covalent Organic Frameworks for Enhancing Photocatalytic H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    and H\n                    <sub>2<\/sub>\n                    Production"],"prefix":"10.1002","volume":"38","author":[{"given":"Pei","family":"Huang","sequence":"first","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yan\u2010Yu","family":"Peng","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiao\u2010Han","family":"Wang","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou 510006 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