The efficiency of organic semiconductor photocatalysts is typically limited by their capability of photogenerated electron transport.Herein,a photocatalyst is proposed initially through the specific axial coordination...The efficiency of organic semiconductor photocatalysts is typically limited by their capability of photogenerated electron transport.Herein,a photocatalyst is proposed initially through the specific axial coordination interaction between imidazole-C_(60)(ImC_(60))and zinc tetraphenyl porphyrin(ZnTPP)named ImC_(60)-ZnTPP.Subsequently,detailed structural characterizations along with theoretical calculation reveal that the unique ImC_(60)-ZnTPP possesses head-to-tail stacking supra-structures,leading to the formation of a continuous array of C_(60)–C_(60) with ultrashort spacing and ensuring strongπ–πinteractions and homogeneous electronic coupling,which could tremendously promote electron transport along the(−111)crystal facet of ImC_(60)-ZnTPP.Consequently,compared to other fullerene-based photocatalysts,ImC_(60)-ZnTPP shows exceptional photocatalytic hydrogen production activity,with an efficiency of up to 80.95 mmol g^(-1) h^(-1).This study provides a novel strategy to design highly efficient fullerene-based photocatalytic systems for solar-driven energy conversion and extend their artificial photosynthetic use.展开更多
基金supported by the National Natural Science Foundation of China(52322204,52072374,52272052)the National Key R&D Program of China(Grant No.2022YFA1205900)the Youth Innovation Promotion Association of CAS(Y2022015).
文摘The efficiency of organic semiconductor photocatalysts is typically limited by their capability of photogenerated electron transport.Herein,a photocatalyst is proposed initially through the specific axial coordination interaction between imidazole-C_(60)(ImC_(60))and zinc tetraphenyl porphyrin(ZnTPP)named ImC_(60)-ZnTPP.Subsequently,detailed structural characterizations along with theoretical calculation reveal that the unique ImC_(60)-ZnTPP possesses head-to-tail stacking supra-structures,leading to the formation of a continuous array of C_(60)–C_(60) with ultrashort spacing and ensuring strongπ–πinteractions and homogeneous electronic coupling,which could tremendously promote electron transport along the(−111)crystal facet of ImC_(60)-ZnTPP.Consequently,compared to other fullerene-based photocatalysts,ImC_(60)-ZnTPP shows exceptional photocatalytic hydrogen production activity,with an efficiency of up to 80.95 mmol g^(-1) h^(-1).This study provides a novel strategy to design highly efficient fullerene-based photocatalytic systems for solar-driven energy conversion and extend their artificial photosynthetic use.
