Plasmon-induced hot electron can transfer from noble metal to its cohesive semiconductor in their heterostructure to initiate the photocatalytic reaction upon resonance excitation.However,the co-excitation of semicond...Plasmon-induced hot electron can transfer from noble metal to its cohesive semiconductor in their heterostructure to initiate the photocatalytic reaction upon resonance excitation.However,the co-excitation of semiconductor in the heterostructure would also lead to the inversus transfer of photo-electron from semiconductor to noble metal,which inevitably limits the use of active electrons.After co-excitation of both localized surface plasmon resonance(LSPR)of noble metal and interband transition of semiconductor,the interfacial electron transfer process strongly depends on the energy band configuration of their heterostructure.When the Au content in the AuAg alloy nanoparticles(NPs)changes from 0 to 100 at.%,the interfacial energy band configuration at AuAg NPs/TiO_(2) NPs in the electrospun nanofibers(NFs)shifts from Ohmic to Schottky contacts.Further investigation finds that the optimal Schottky barrier configuration in Au_(0.25)Ag_(0.75)/TiO_(2) NFs can not only boost the plasmon-induced hot electron transfer from Au_(0.25)Ag_(0.75) to TiO_(2) NPs,but also suppresses the backflow of photo-electrons from TiO_(2) to Au_(0.25)Ag_(0.75) NPs in NFs.Thus,upon UV-visible light irradiation,the CO_(2) photo-reduction activity of Au_(0.25)Ag_(0.75)/TiO_(2) NFs is~3 and~2 times higher than that of either Ag/TiO_(2) or Au/TiO_(2) NFs.展开更多
基金supported by the National Natural Science Foundation of China(Nos.:22472021,U23A20102,12074055,22402021 and 62005036)Liaoning Revitalization Talents Program(XLYC2202036,XLYC1807176)+4 种基金Natural Science Foundation of Liaoning Province for Excellent Young Scholars(2022-YQ-13)Fundamental Research Funds for the Central Universities(044420250072)Dalian Science Foundation for Distinguished Young Scholars(2018RJ05)Natural Science Foundation of Liaoning Province(2023-MS-132)Joint Funds of the Science and Technology Program of Liaoning Province(No.2024JH2/102600101).
文摘Plasmon-induced hot electron can transfer from noble metal to its cohesive semiconductor in their heterostructure to initiate the photocatalytic reaction upon resonance excitation.However,the co-excitation of semiconductor in the heterostructure would also lead to the inversus transfer of photo-electron from semiconductor to noble metal,which inevitably limits the use of active electrons.After co-excitation of both localized surface plasmon resonance(LSPR)of noble metal and interband transition of semiconductor,the interfacial electron transfer process strongly depends on the energy band configuration of their heterostructure.When the Au content in the AuAg alloy nanoparticles(NPs)changes from 0 to 100 at.%,the interfacial energy band configuration at AuAg NPs/TiO_(2) NPs in the electrospun nanofibers(NFs)shifts from Ohmic to Schottky contacts.Further investigation finds that the optimal Schottky barrier configuration in Au_(0.25)Ag_(0.75)/TiO_(2) NFs can not only boost the plasmon-induced hot electron transfer from Au_(0.25)Ag_(0.75) to TiO_(2) NPs,but also suppresses the backflow of photo-electrons from TiO_(2) to Au_(0.25)Ag_(0.75) NPs in NFs.Thus,upon UV-visible light irradiation,the CO_(2) photo-reduction activity of Au_(0.25)Ag_(0.75)/TiO_(2) NFs is~3 and~2 times higher than that of either Ag/TiO_(2) or Au/TiO_(2) NFs.