One of the most general methods to enhance the separation of photogenerated carriers for g‐C3N4is to construct a suitable heterojunctional composite,according to the principle of matching energy levels.The interface ...One of the most general methods to enhance the separation of photogenerated carriers for g‐C3N4is to construct a suitable heterojunctional composite,according to the principle of matching energy levels.The interface contact in the fabricated nanocomposite greatly influences the charge transfer and separation so as to determine the final photocatalytic activities.However,the role of interface contact is often neglected,and is rarely reported to date.Hence,it is possible to further enhance the photocatalytic activity of g‐C3N4‐based nanocomposite by improving the interfacial connection.Herein,phosphate-oxygen(P-O)bridged TiO2/g‐C3N4nanocomposites were successfully synthesized using a simple wet chemical method,and the effects of the P-O functional bridges on the photogenerated charge separation and photocatalytic activity for pollutant degradation and CO2reduction were investigated.The photocatalytic activity of g‐C3N4was greatly improved upon coupling with an appropriate amount of nanocrystalline TiO2,especially with P-O bridged TiO2.Atmosphere‐controlled steady‐state surface photovoltage spectroscopy and photoluminescence spectroscopy analyses revealed clearly the enhancement of photogenerated charge separation of g‐C3N4upon coupling with the P-O bridged TiO2,resulting from the built P-O bridges between TiO2and g‐C3N4so as to promote effective transfer of excited electrons from g‐C3N4to TiO2.This enhancement was responsible for the improved photoactivity of the P-O bridged TiO2/g‐C3N4nanocomposite,which exhibited three‐time photocatalytic activity enhancement for2,4‐dichlorophenol degradation and CO2reduction compared with bare g‐C3N4.Furthermore,radical‐trapping experiments revealed that the·OH species formed as hole‐modulated direct intermediates dominated the photocatalytic degradation of2,4‐dichlorophenol.This work provides a feasible strategy for the design and synthesis of high‐performance g‐C3N4‐based nanocomposite photocatalysts for pollutant degradation and CO2reduction.展开更多
基金supported by the National Natural Science Foundation of China(U1401245,91622119)the Program for Innovative Research Team in Chinese Universities(IRT1237)+1 种基金the Research Project of Chinese Ministry of Education(213011A)the Science Foundation for Excellent Youth of Harbin City of China(2014RFYXJ002)~~
文摘One of the most general methods to enhance the separation of photogenerated carriers for g‐C3N4is to construct a suitable heterojunctional composite,according to the principle of matching energy levels.The interface contact in the fabricated nanocomposite greatly influences the charge transfer and separation so as to determine the final photocatalytic activities.However,the role of interface contact is often neglected,and is rarely reported to date.Hence,it is possible to further enhance the photocatalytic activity of g‐C3N4‐based nanocomposite by improving the interfacial connection.Herein,phosphate-oxygen(P-O)bridged TiO2/g‐C3N4nanocomposites were successfully synthesized using a simple wet chemical method,and the effects of the P-O functional bridges on the photogenerated charge separation and photocatalytic activity for pollutant degradation and CO2reduction were investigated.The photocatalytic activity of g‐C3N4was greatly improved upon coupling with an appropriate amount of nanocrystalline TiO2,especially with P-O bridged TiO2.Atmosphere‐controlled steady‐state surface photovoltage spectroscopy and photoluminescence spectroscopy analyses revealed clearly the enhancement of photogenerated charge separation of g‐C3N4upon coupling with the P-O bridged TiO2,resulting from the built P-O bridges between TiO2and g‐C3N4so as to promote effective transfer of excited electrons from g‐C3N4to TiO2.This enhancement was responsible for the improved photoactivity of the P-O bridged TiO2/g‐C3N4nanocomposite,which exhibited three‐time photocatalytic activity enhancement for2,4‐dichlorophenol degradation and CO2reduction compared with bare g‐C3N4.Furthermore,radical‐trapping experiments revealed that the·OH species formed as hole‐modulated direct intermediates dominated the photocatalytic degradation of2,4‐dichlorophenol.This work provides a feasible strategy for the design and synthesis of high‐performance g‐C3N4‐based nanocomposite photocatalysts for pollutant degradation and CO2reduction.