The development of photocatalysts that combine high efficiency,durability,and visible-light responsiveness remains a central challenge for solar-to-hydrogen conversion.In a recent study,Cabrero-Antonino et al.report a...The development of photocatalysts that combine high efficiency,durability,and visible-light responsiveness remains a central challenge for solar-to-hydrogen conversion.In a recent study,Cabrero-Antonino et al.report a 2D/2D Schottky heterojunction constructed from ultrasmall Cu_(2)[CuTCPP]MOF nanosheets and conductive Ti_(3)C_(2)MXene.This hybrid interface generates a built-in interfacial electric field that promotes directional charge transfer,suppresses recombination,and significantly prolongs carrier lifetimes,as evidenced by femtosecond transient absorption spectroscopy.The MXene component not only functions as a hole acceptor to improve charge separation but also mitigates photooxidative degradation of the MOF,thereby enhancing long-term stability.The optimized heterojunction achieves a hydrogen evolution rate exceeding 5000μmol g^(-1)under visible light,nearly 20 times higher than that of pristine MOF,with notable operational durability.These findings demonstrate the critical role of interfacial engineering in achieving synergistic charge dynamics across hybrid architectures.The work provides a scalable,sustainable strategy for noble-metalfree photocatalysis,offering valuable insights for the rational design of next-generation systems for water splitting,CO_(2)reduction,and solar-driven chemical transformations.展开更多
As one of the highly effective methods to prepare catalysts for photocatalytic reduction of CO2 into valueadded chemicals,using metalloporphyrin as light-harvesting mixed ligand to modify metal-organic framework(MOF)i...As one of the highly effective methods to prepare catalysts for photocatalytic reduction of CO2 into valueadded chemicals,using metalloporphyrin as light-harvesting mixed ligand to modify metal-organic framework(MOF)is very valuable since it can greatly improve the prophyrin dispersibility and consequently inhibit its potential agglomeration.Herein,we employed a one-pot synthetic strategy to chemically immobilize Cu(II)tetra(4-carboxylphenyl)porphyrin(CuTCPP)into UiO-66 MOF structure through coordination mode.Meanwhile,in-situ growth of TiO2 nanoparticles onto the MOF is actualized with the generation of CuTCPP c UiO-66/TiO2(CTU/TiO2)composites.Under Xe lamp irradiation(λ>300 nm),the catalytic result presents that an optimal value of 31.32 μmol g^-1 h^-1 CO evolution amount,about 7 times higher than that of pure TiO2 was obtained through the photocatalysis.It is supposed owning to a consistent augment of light absorption derived from chemically implanted porphyrin derivative,which is simultaneously functioning with an efficacious separation of photo-induced carries given by the newly engendered composites between MOF and TiO2,an effective catalytic activity and approving recyclability of CTU/TiO2 can be achieved in the photocatalytic reduction of CO2 into CO.展开更多
基金financially supported by the National Natural Science Foundation of China(No.22202187)the Hubei Provincial Natural Science Foundation of China(No.2025AFB492)
文摘The development of photocatalysts that combine high efficiency,durability,and visible-light responsiveness remains a central challenge for solar-to-hydrogen conversion.In a recent study,Cabrero-Antonino et al.report a 2D/2D Schottky heterojunction constructed from ultrasmall Cu_(2)[CuTCPP]MOF nanosheets and conductive Ti_(3)C_(2)MXene.This hybrid interface generates a built-in interfacial electric field that promotes directional charge transfer,suppresses recombination,and significantly prolongs carrier lifetimes,as evidenced by femtosecond transient absorption spectroscopy.The MXene component not only functions as a hole acceptor to improve charge separation but also mitigates photooxidative degradation of the MOF,thereby enhancing long-term stability.The optimized heterojunction achieves a hydrogen evolution rate exceeding 5000μmol g^(-1)under visible light,nearly 20 times higher than that of pristine MOF,with notable operational durability.These findings demonstrate the critical role of interfacial engineering in achieving synergistic charge dynamics across hybrid architectures.The work provides a scalable,sustainable strategy for noble-metalfree photocatalysis,offering valuable insights for the rational design of next-generation systems for water splitting,CO_(2)reduction,and solar-driven chemical transformations.
基金financially supported by the National Natural Science Foundation of China (21663027, 21808189)the Science and Technology Support Project of Gansu Province (1504GKCA027)
文摘As one of the highly effective methods to prepare catalysts for photocatalytic reduction of CO2 into valueadded chemicals,using metalloporphyrin as light-harvesting mixed ligand to modify metal-organic framework(MOF)is very valuable since it can greatly improve the prophyrin dispersibility and consequently inhibit its potential agglomeration.Herein,we employed a one-pot synthetic strategy to chemically immobilize Cu(II)tetra(4-carboxylphenyl)porphyrin(CuTCPP)into UiO-66 MOF structure through coordination mode.Meanwhile,in-situ growth of TiO2 nanoparticles onto the MOF is actualized with the generation of CuTCPP c UiO-66/TiO2(CTU/TiO2)composites.Under Xe lamp irradiation(λ>300 nm),the catalytic result presents that an optimal value of 31.32 μmol g^-1 h^-1 CO evolution amount,about 7 times higher than that of pure TiO2 was obtained through the photocatalysis.It is supposed owning to a consistent augment of light absorption derived from chemically implanted porphyrin derivative,which is simultaneously functioning with an efficacious separation of photo-induced carries given by the newly engendered composites between MOF and TiO2,an effective catalytic activity and approving recyclability of CTU/TiO2 can be achieved in the photocatalytic reduction of CO2 into CO.
