Photocatalytic hydrogen peroxide(H_(2)O_(2))production is a promising strategy to replace the traditional production processes;however,the inefficient H_(2)O_(2) productivity limits its application.In this study,oxyge...Photocatalytic hydrogen peroxide(H_(2)O_(2))production is a promising strategy to replace the traditional production processes;however,the inefficient H_(2)O_(2) productivity limits its application.In this study,oxygen-rich g-C_(3)N_(4) with abundant nitrogen vacancies(OCN)was synthesized for photocatalytic H_(2)O_(2) production.X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy indicated that oxygen-containing functional groups(–COOH and C–O–C)were obtained.Electron paramagnetic resonance confirmed the successful introduction of nitrogen vacancies.OCN exhibited efficient photocatalytic H_(2)O_(2) production performance of 1965μmol L^(−1) h^(−1) in air under visible-light irradiation.The high H_(2)O_(2) production was attributed to the enhanced adsorption of oxygen,enlarged specific surface area,and promoted carrier separation.An increased H_(2)O_(2) production rate(5781μmol L^(−1) h^(−1))was achieved in a Na_(3)PO_(4) solution.The improved performance was attributed to the changed reactive oxygen species.Specifically,the adsorbed PO_(4)^(3−) on the surface of the OCN promoted the transfer of holes to the catalyst surface.•O_(2)−obtained by O_(2) reduction reacted with adjacent holes to generate 1O_(2),which could efficiently generate H_(2)O_(2) with isopropanol.Additionally,PO_(4)^(3−),as a stabilizer,inhibited the decomposition of H_(2)O_(2).展开更多
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
文摘Photocatalytic hydrogen peroxide(H_(2)O_(2))production is a promising strategy to replace the traditional production processes;however,the inefficient H_(2)O_(2) productivity limits its application.In this study,oxygen-rich g-C_(3)N_(4) with abundant nitrogen vacancies(OCN)was synthesized for photocatalytic H_(2)O_(2) production.X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy indicated that oxygen-containing functional groups(–COOH and C–O–C)were obtained.Electron paramagnetic resonance confirmed the successful introduction of nitrogen vacancies.OCN exhibited efficient photocatalytic H_(2)O_(2) production performance of 1965μmol L^(−1) h^(−1) in air under visible-light irradiation.The high H_(2)O_(2) production was attributed to the enhanced adsorption of oxygen,enlarged specific surface area,and promoted carrier separation.An increased H_(2)O_(2) production rate(5781μmol L^(−1) h^(−1))was achieved in a Na_(3)PO_(4) solution.The improved performance was attributed to the changed reactive oxygen species.Specifically,the adsorbed PO_(4)^(3−) on the surface of the OCN promoted the transfer of holes to the catalyst surface.•O_(2)−obtained by O_(2) reduction reacted with adjacent holes to generate 1O_(2),which could efficiently generate H_(2)O_(2) with isopropanol.Additionally,PO_(4)^(3−),as a stabilizer,inhibited the decomposition of H_(2)O_(2).
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.
