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
The Bi_4Ti_3O_(12)/g-C_3N_4 composites with microsheet and nanosheet structure were prepared through facile ultrasonic-assisted method. The SEM and TEM results suggested that the nanosheets g-C_3N_4 were stacked on th...The Bi_4Ti_3O_(12)/g-C_3N_4 composites with microsheet and nanosheet structure were prepared through facile ultrasonic-assisted method. The SEM and TEM results suggested that the nanosheets g-C_3N_4 were stacked on the surface of regular Bi_4Ti_3O_(12) sheets. Comparing with pure Bi_4Ti_3O_(12) and g-C_3N_4, the Bi_4Ti_3O_(12)/g-C_3N_4 composites showed significant enhancement in photocatalytic efficiency for the degradation of RhB in solution. With the mass ratio of g-C_3N_4 increasing to 10 wt%, the Bi_4Ti_3O_(12)/g-C_3N_4-10% presented the best photocatalytic activity. Its photocatalysis reaction constant was approximately 2 times higher than the single component Bi_4Ti_3O_(12) or g-C_3N_4. Meanwhile, good stability and durability for the Bi_4Ti_3O_(12)/g-C_3N_4-10% were confirmed by the recycling experiment and FT-IR analysis. The possible mechanism for the improvements was the matched band positions and the effective separation of photo-excited electrons(e-) and holes(h+). Furthermore, based on the results of active species trapping, photo-generated holes(h+) and superoxide radical(·O2-) could be the main radicals in reaction.展开更多
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.
基金Supported by the National Natural Science Foundation of China(51509220)the Natural Science Foundation of Zhejiang Province(LQ14E090003)+1 种基金Ningbo Science and Technology Plan Projects(2014C50007,2014C51003)Ningbo major social development projects(2017C510006)
文摘The Bi_4Ti_3O_(12)/g-C_3N_4 composites with microsheet and nanosheet structure were prepared through facile ultrasonic-assisted method. The SEM and TEM results suggested that the nanosheets g-C_3N_4 were stacked on the surface of regular Bi_4Ti_3O_(12) sheets. Comparing with pure Bi_4Ti_3O_(12) and g-C_3N_4, the Bi_4Ti_3O_(12)/g-C_3N_4 composites showed significant enhancement in photocatalytic efficiency for the degradation of RhB in solution. With the mass ratio of g-C_3N_4 increasing to 10 wt%, the Bi_4Ti_3O_(12)/g-C_3N_4-10% presented the best photocatalytic activity. Its photocatalysis reaction constant was approximately 2 times higher than the single component Bi_4Ti_3O_(12) or g-C_3N_4. Meanwhile, good stability and durability for the Bi_4Ti_3O_(12)/g-C_3N_4-10% were confirmed by the recycling experiment and FT-IR analysis. The possible mechanism for the improvements was the matched band positions and the effective separation of photo-excited electrons(e-) and holes(h+). Furthermore, based on the results of active species trapping, photo-generated holes(h+) and superoxide radical(·O2-) could be the main radicals in reaction.