Sunlight-driven photocatalytic water-splitting for hydrogen(H2)evolution is a desirable strategy to utilize solar energy.However,this strategy is restricted by insufficient light harvesting and high photogenerated ele...Sunlight-driven photocatalytic water-splitting for hydrogen(H2)evolution is a desirable strategy to utilize solar energy.However,this strategy is restricted by insufficient light harvesting and high photogenerated electron-hole recombination rates of TiO2-based photocatalysts.Here,a graphene-modified WO3/TiO2 step-scheme heterojunction(S-scheme heterojunction)composite photocatalyst was fabricated by a facile one-step hydrothermal method.In the ternary composite,TiO2 and WO3 nanoparticles adhered closely to reduced graphene oxide(rGO)and formed a novel S-scheme heterojunction.Moreover,rGO in the composite not only supplied abundant adsorption and catalytically active sites as an ideal support but also promoted electron separation and transfer from the conduction band of TiO2 by forming a Schottky junction between TiO2 and rGO.The positive cooperative effect of the S-scheme heterojunction formed between WO3 and TiO2 and the Schottky heterojunction formed between TiO2 and graphene sheets suppressed the recombination of relatively useful electrons and holes.This effect also enhanced the light harvesting and promoted the reduction reaction at the active sites.Thus,the novel ternary WO3/TiO2/rGO composite demonstrated a remarkably enhanced photocatalytic H2 evolution rate of 245.8μmol g^-1 h^-1,which was approximately 3.5-fold that of pure TiO2.This work not only presents a low-cost graphene-based S-scheme heterojunction photocatalyst that was obtained via a feasible one-step hydrothermal approach to realize highly efficient H2 generation without using noble metals,but also provides new insights into the design of novel heterojunction photocatalysts.展开更多
Although the traditional Fenton reaction is considered an effective strategy for solving problems caused by environmental pollution,construction of an efficient photocatalytic system by coordinating the Fenton reactio...Although the traditional Fenton reaction is considered an effective strategy for solving problems caused by environmental pollution,construction of an efficient photocatalytic system by coordinating the Fenton reaction is challenging.In this study,2D/2D step-schemeα-Fe2O3/Bi2WO6(FO/BWO)heterostructure photo-Fenton catalysts were successfully fabricated by a facile hydrothermal method.The as-prepared materials were characterized by XRD,FT-IR,TEM,XPS,UV-vis DRS,PL,I-t,EIS,and BET analyses.Under visible light irradiation,FO/BWO exhibited remarkably high and stable photo-Fenton catalytic activity for the degradation of methyl blue(MB)at low concentrations of H2O2.It was noted that FO/BWO(0.5)displayed a significantly enhanced photo-Fenton catalytic activity,which was 11.06 and 3.29 times those of FO nanosheets and BWO nanosheets,respectively.The notably improved photo-Fenton catalytic activity of FO/BWO was mainly due to the combination of H2O2 and FO under light illumination and the presence of the 2D/2D S-scheme heterostructure,with the large contact surface,abundant active sites,and efficient separation rate of photogenerated carriers playing contributory roles.Additionally,a possible catalytic mechanism for the FO/BWO composite was preliminarily proposed via active species trapping experiments.In summary,this study provided new insights into the synthesis of an effectively heterogeneous 2D/2D S-scheme photo-Fenton catalyst for degradation of organic pollutants in wastewater.展开更多
基金supported by the National Natural Science Foundation of China(U1705251,21871217,21573170,21433007)the National Key Research and Development Program of China(2018YFB1502001)~~
文摘Sunlight-driven photocatalytic water-splitting for hydrogen(H2)evolution is a desirable strategy to utilize solar energy.However,this strategy is restricted by insufficient light harvesting and high photogenerated electron-hole recombination rates of TiO2-based photocatalysts.Here,a graphene-modified WO3/TiO2 step-scheme heterojunction(S-scheme heterojunction)composite photocatalyst was fabricated by a facile one-step hydrothermal method.In the ternary composite,TiO2 and WO3 nanoparticles adhered closely to reduced graphene oxide(rGO)and formed a novel S-scheme heterojunction.Moreover,rGO in the composite not only supplied abundant adsorption and catalytically active sites as an ideal support but also promoted electron separation and transfer from the conduction band of TiO2 by forming a Schottky junction between TiO2 and rGO.The positive cooperative effect of the S-scheme heterojunction formed between WO3 and TiO2 and the Schottky heterojunction formed between TiO2 and graphene sheets suppressed the recombination of relatively useful electrons and holes.This effect also enhanced the light harvesting and promoted the reduction reaction at the active sites.Thus,the novel ternary WO3/TiO2/rGO composite demonstrated a remarkably enhanced photocatalytic H2 evolution rate of 245.8μmol g^-1 h^-1,which was approximately 3.5-fold that of pure TiO2.This work not only presents a low-cost graphene-based S-scheme heterojunction photocatalyst that was obtained via a feasible one-step hydrothermal approach to realize highly efficient H2 generation without using noble metals,but also provides new insights into the design of novel heterojunction photocatalysts.
文摘Although the traditional Fenton reaction is considered an effective strategy for solving problems caused by environmental pollution,construction of an efficient photocatalytic system by coordinating the Fenton reaction is challenging.In this study,2D/2D step-schemeα-Fe2O3/Bi2WO6(FO/BWO)heterostructure photo-Fenton catalysts were successfully fabricated by a facile hydrothermal method.The as-prepared materials were characterized by XRD,FT-IR,TEM,XPS,UV-vis DRS,PL,I-t,EIS,and BET analyses.Under visible light irradiation,FO/BWO exhibited remarkably high and stable photo-Fenton catalytic activity for the degradation of methyl blue(MB)at low concentrations of H2O2.It was noted that FO/BWO(0.5)displayed a significantly enhanced photo-Fenton catalytic activity,which was 11.06 and 3.29 times those of FO nanosheets and BWO nanosheets,respectively.The notably improved photo-Fenton catalytic activity of FO/BWO was mainly due to the combination of H2O2 and FO under light illumination and the presence of the 2D/2D S-scheme heterostructure,with the large contact surface,abundant active sites,and efficient separation rate of photogenerated carriers playing contributory roles.Additionally,a possible catalytic mechanism for the FO/BWO composite was preliminarily proposed via active species trapping experiments.In summary,this study provided new insights into the synthesis of an effectively heterogeneous 2D/2D S-scheme photo-Fenton catalyst for degradation of organic pollutants in wastewater.