The development of an efficient artificial H_(2)O_(2)photosynthesis system is a challenging work using H_(2)O and O_(2)as starting materials.Herein,3D In2.77S_(4)nanoflower precursor was in-situ deposited on K^(+)-dop...The development of an efficient artificial H_(2)O_(2)photosynthesis system is a challenging work using H_(2)O and O_(2)as starting materials.Herein,3D In2.77S_(4)nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In2.77S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2)production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In2.77S_(4),respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In2.77S_(4)according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2)production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2)around the active centers,the energy barriers of O_(2)protonation and H_(2)O_(2)desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2)photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.展开更多
以五水硝酸铋、溴化钾和三聚氰胺为原料,采用溶剂热法制备了摩尔比不同的BiOBr/g-C_3N_4复合光催化剂,并进行了XRD、SEM和DRS表征分析。以50 W LED紫光灯为光源,采用罗丹明B为目标降解物考察了制备样品的光催化性能。结果表明:摩尔比为1...以五水硝酸铋、溴化钾和三聚氰胺为原料,采用溶剂热法制备了摩尔比不同的BiOBr/g-C_3N_4复合光催化剂,并进行了XRD、SEM和DRS表征分析。以50 W LED紫光灯为光源,采用罗丹明B为目标降解物考察了制备样品的光催化性能。结果表明:摩尔比为1∶1的BiOBr/g-C_3N_4复合光催化剂的具有最优的光催化性能。机理实验结果表明:超氧自由基(O_2·^-)和空穴(h+)为BiOBr/g-C_3N_4复合光催化剂光催化过程最为主要的活性物种。展开更多
基金supported by the National Natural Science Foundation of China(51602297)Fundamental Research Funds for the Central Universities(201612007)+1 种基金Postdoctoral Innovation Program of Shandong Province(201603043)the Major Research Project of Shandong Province(2016ZDJS11A04)
文摘The development of an efficient artificial H_(2)O_(2)photosynthesis system is a challenging work using H_(2)O and O_(2)as starting materials.Herein,3D In2.77S_(4)nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In2.77S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2)production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In2.77S_(4),respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In2.77S_(4)according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2)production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2)around the active centers,the energy barriers of O_(2)protonation and H_(2)O_(2)desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2)photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.
文摘以五水硝酸铋、溴化钾和三聚氰胺为原料,采用溶剂热法制备了摩尔比不同的BiOBr/g-C_3N_4复合光催化剂,并进行了XRD、SEM和DRS表征分析。以50 W LED紫光灯为光源,采用罗丹明B为目标降解物考察了制备样品的光催化性能。结果表明:摩尔比为1∶1的BiOBr/g-C_3N_4复合光催化剂的具有最优的光催化性能。机理实验结果表明:超氧自由基(O_2·^-)和空穴(h+)为BiOBr/g-C_3N_4复合光催化剂光催化过程最为主要的活性物种。
