Oxygen evolution reaction(OER),a critical half-reaction in photocatalytic overall water splitting for producing hydrogen,is a key step toward sustainable energy conversion.Conventional photocatalysts often suffer from...Oxygen evolution reaction(OER),a critical half-reaction in photocatalytic overall water splitting for producing hydrogen,is a key step toward sustainable energy conversion.Conventional photocatalysts often suffer from limited light absorption and rapid charge recombination,hindering their further applications.To address these challenges,we have designed and synthesized a novel series of self-sensitized metal-organic frameworks(MOFs),Fe_(2)MCDDB(M=Ni,Mn,or Co).By incorporating photosensitive ligands,we have achieved efficient charge separation and promoted the transfer of photogenerated electrons to the active metal sites for water oxidation.Among the series,Fe_(2)NiCDDB exhibits exceptional OER activity,achieving an oxygen evolution rate of 125.3μmol g^(−1)h^(−1)under visible light irradiation.Experimental and theoretical results reveal that the optimized electronic structure and prolonged excited-state lifetime of Fe_(2)NiCDDB contribute to its enhanced catalytic performance.This work provides a promising strategy for designing two-in-one MOF photocatalysts for water oxidation.展开更多
基金funded by the National Natural Science Foundation of China(22271063 and 22371054)the Foundation of Basic and Applied Basic Research of Guangdong Province(2024A1515010423)+1 种基金Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01Z032)Science and Technology Planning Project of Guangdong Province(2021A0505030066).
文摘Oxygen evolution reaction(OER),a critical half-reaction in photocatalytic overall water splitting for producing hydrogen,is a key step toward sustainable energy conversion.Conventional photocatalysts often suffer from limited light absorption and rapid charge recombination,hindering their further applications.To address these challenges,we have designed and synthesized a novel series of self-sensitized metal-organic frameworks(MOFs),Fe_(2)MCDDB(M=Ni,Mn,or Co).By incorporating photosensitive ligands,we have achieved efficient charge separation and promoted the transfer of photogenerated electrons to the active metal sites for water oxidation.Among the series,Fe_(2)NiCDDB exhibits exceptional OER activity,achieving an oxygen evolution rate of 125.3μmol g^(−1)h^(−1)under visible light irradiation.Experimental and theoretical results reveal that the optimized electronic structure and prolonged excited-state lifetime of Fe_(2)NiCDDB contribute to its enhanced catalytic performance.This work provides a promising strategy for designing two-in-one MOF photocatalysts for water oxidation.
