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Molecular phthalocyanine electrocatalysts on carbon nanotubes have achieved production of methanol as the sole liquid\u2010phase product but with the activity and stability far from meeting industrial demands. Herein, phthalocyaninato cobalt is fabricated into covalent organic frameworks PE\u2010COF via polymerization with ellagic acid. Subsequent hydrolyzation of the ester groups in this framework affords COOH\/OH\u2010containing PEH\u2010COF, resulting in the successful modulation over the local microenvironment of Co as electrochemical active center and in turn rendering the production of CH\n                    <jats:sub>3<\/jats:sub>\n                    OH with high yield and durability. Experimental and theoretical investigations reveal that construction of the COOH group and H\n                    <jats:sub>2<\/jats:sub>\n                    O participated catalytic cages in PEH\u2010COF can effectively fix hydrated potassium ions, which efficiently enhances the PCET kinetics and lowers the energy barriers for the conversion of CO\n                    <jats:sub>2<\/jats:sub>\n                    to CH\n                    <jats:sub>3<\/jats:sub>\n                    OH. The partial current density (\n                    <jats:italic>j<\/jats:italic>\n                    ) and Faraday efficiency of methanol for PEH\u2010COF could reach 100.9\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and 38.5%, respectively. Moreover, the  of PEH\u2010COF can be maintained at 100.4\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    after 9\u00a0h of electrocatalysis, superior to the thus far reported catalysts.\n                  <\/jats:p>","DOI":"10.1002\/adma.202502644","type":"journal-article","created":{"date-parts":[[2025,3,30]],"date-time":"2025-03-30T13:41:19Z","timestamp":1743342079000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":40,"title":["Modulating Active Center Microenvironment in Phthalocyanine\u2010Based Covalent Organic Frameworks for Enhanced Electrocatalytic CO\n                    <sub>2<\/sub>\n                    to CH\n                    <sub>3<\/sub>\n                    OH"],"prefix":"10.1002","volume":"37","author":[{"given":"Qin","family":"Wang","sequence":"first","affiliation":[{"name":"Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials School of Chemistry and Biological Engineering University of Science and Technology Beijing  Beijing 100083 P. 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