Solar-driven H_(2)O_(2)production and emerging organic pollutants(EOPs)elimination are of great significance from the perspective of environmental sustainability.The efficiency of the photocatalytic reaction system is...Solar-driven H_(2)O_(2)production and emerging organic pollutants(EOPs)elimination are of great significance from the perspective of environmental sustainability.The efficiency of the photocatalytic reaction system is the key challenge to be addressed.In this work,the strategy of constructing surface ionic local polarization centers to enhance the exciton dissociation of the polymeric photocatalytic is demonstrated.Selected bipyridinium cation(TMAP)is complexed on a K^(+)-incorporated carbon nitride(CNK)framework,and the combination of local polarization centers both on the surface(bipyridinium cation)and bulk(K+cation)contributes to a superior photocatalytic H_(2)O_(2)production performance,affording a remarkable H_(2)O_(2)generation rate of 46.8μmol h^(-1)mg^(-1)and a high apparent quantum yield(AQY)value of 77.5%under irradiation of 405 nm photons.As substantiated experimentally by steady state/transient spectroscopy techniques,the surface local polarization centers increase the population of the long-lived trapped electrons,and thereby promote the interfacial charge transfer process for chemical conversion reaction.The strategy is potentially applicable to the design of a wide range of efficient solar-to-chemical conversion systems.展开更多
基金Financial supports by the National Natural Science Foundation of China(No.21976041)Guangzhou Municipal Science and Technology Project(No.202201020168)+1 种基金Tertiary Education Scientific Research Project of Guangzhou Municipal Education Bureau(No.202235238)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515010788)are acknowledged。
文摘Solar-driven H_(2)O_(2)production and emerging organic pollutants(EOPs)elimination are of great significance from the perspective of environmental sustainability.The efficiency of the photocatalytic reaction system is the key challenge to be addressed.In this work,the strategy of constructing surface ionic local polarization centers to enhance the exciton dissociation of the polymeric photocatalytic is demonstrated.Selected bipyridinium cation(TMAP)is complexed on a K^(+)-incorporated carbon nitride(CNK)framework,and the combination of local polarization centers both on the surface(bipyridinium cation)and bulk(K+cation)contributes to a superior photocatalytic H_(2)O_(2)production performance,affording a remarkable H_(2)O_(2)generation rate of 46.8μmol h^(-1)mg^(-1)and a high apparent quantum yield(AQY)value of 77.5%under irradiation of 405 nm photons.As substantiated experimentally by steady state/transient spectroscopy techniques,the surface local polarization centers increase the population of the long-lived trapped electrons,and thereby promote the interfacial charge transfer process for chemical conversion reaction.The strategy is potentially applicable to the design of a wide range of efficient solar-to-chemical conversion systems.