The selective oxidation of toluene and its derivatives is extremely important in the chemical industry.The use of photocatalysis in organic synthesis has attracted considerable attention among synthetic chemists becau...The selective oxidation of toluene and its derivatives is extremely important in the chemical industry.The use of photocatalysis in organic synthesis has attracted considerable attention among synthetic chemists because of its ＂green＂ environmental characteristics.In this study,nanoscale Bi_2WO_6with a flower-like morphology was found to be a highly efficient photocatalyst in the catalytic oxidation of toluene and its derivatives using O_2 as the oxidant.The loading of Pd nanoparticles as a cocatalyst onto the flower-like Bi_2WO_6 was found to produce a significant enhancement in the catalytic activity.Mechanistic investigation showed that the superior performance of Pd/Bi_2WO_6 could be attributed to the improvement of both the reductive and oxidative abilities of Bi_2WO_6 by the loading of the cocatalyst.展开更多
Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are st...Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are still low due to the sluggish dynamics of transfer processes involved in proton-assisted multi-electron reactions.Lowering the formation energy barriers of intermediate products is an effective method to enhance the selectivity and productivity of final products.In this study,we aim to regulate the surface electronic structure of Bi_(2)WO_(6)by doping surface chlorine atoms to achieve effective photocatalytic CO_(2)reduction.Surface Cl atoms can enhance the absorption ability of light,affect its energy band structure and promote charge separation.Combined with DFT calculations,it is revealed that surface Cl atoms can not only change the surface charge distribution which affects the competitive adsorption of H_(2)O and CO_(2),but also lower the formation energy barrier of intermediate products to generate more intermediate*COOH,thus facilitating CO production.Overall,this study demonstrates a promising surface halogenation strategy to enhance the photocatalytic CO_(2)reduction activity of a layered structure Bi-based catalyst.展开更多
基金supported by the National Natural Science Foundation of China(21322202,21472187)the National Basic Research Program of China(2010CB833300)~~
文摘The selective oxidation of toluene and its derivatives is extremely important in the chemical industry.The use of photocatalysis in organic synthesis has attracted considerable attention among synthetic chemists because of its ＂green＂ environmental characteristics.In this study,nanoscale Bi_2WO_6with a flower-like morphology was found to be a highly efficient photocatalyst in the catalytic oxidation of toluene and its derivatives using O_2 as the oxidant.The loading of Pd nanoparticles as a cocatalyst onto the flower-like Bi_2WO_6 was found to produce a significant enhancement in the catalytic activity.Mechanistic investigation showed that the superior performance of Pd/Bi_2WO_6 could be attributed to the improvement of both the reductive and oxidative abilities of Bi_2WO_6 by the loading of the cocatalyst.
基金supported by the National Natural Science Foundation of China(Grant No.51708078)Natural Science Foundation of Chongqing(Grant No.CSTB2022NSCQ-MSX0815)+2 种基金Science and Technology Research Program of Chongqing Municipal Education Commission(Grant No.KJQN202200542)the Chongqing Innovative Research Group Project(Grant No.CXQT21015)Foundation of Chongqing Normal University(22XLB022).
文摘Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are still low due to the sluggish dynamics of transfer processes involved in proton-assisted multi-electron reactions.Lowering the formation energy barriers of intermediate products is an effective method to enhance the selectivity and productivity of final products.In this study,we aim to regulate the surface electronic structure of Bi_(2)WO_(6)by doping surface chlorine atoms to achieve effective photocatalytic CO_(2)reduction.Surface Cl atoms can enhance the absorption ability of light,affect its energy band structure and promote charge separation.Combined with DFT calculations,it is revealed that surface Cl atoms can not only change the surface charge distribution which affects the competitive adsorption of H_(2)O and CO_(2),but also lower the formation energy barrier of intermediate products to generate more intermediate*COOH,thus facilitating CO production.Overall,this study demonstrates a promising surface halogenation strategy to enhance the photocatalytic CO_(2)reduction activity of a layered structure Bi-based catalyst.
