High-efficiency photocatalysts are of great significance for the application of photocatalytic technology in water treatment.In this study,N/Cu co-doped ZnS nanosphere photocatalys(N/Cu-ZnS) is synthesized by a hydrot...High-efficiency photocatalysts are of great significance for the application of photocatalytic technology in water treatment.In this study,N/Cu co-doped ZnS nanosphere photocatalys(N/Cu-ZnS) is synthesized by a hydrothermal method for the first time.After doping,the tex ture of nanosphere becomes loose,the nanometer diameter is reduced,making the specific surface area of catalyst increased from 34.73 to 101.59 m^(2)/g.The characterization results show that more ZnS (111) crystal planes are exposed by N/Cu co-doping;the calculations of density functional theory show that N/Cu co-doping can increase the catalytic activity of the ZnS (111) crystal plane,enhance the adsorption capacity of (111) crystal plane to O_(2)and promote the generation of·O_(2)-.The energy levels of the introduced impurities can be hybridized with the energy levels of S and Zn at the top of valence band and the bottom o conduction band,which makes the band gap narrower,thus enhancing the absorption o visible light.Compared with pure ZnS,the degradation rates of 2,4-dichlorophenol (2,4-DCP and tetracycline (TC) by N/Cu-ZnS under visible light (>420 nm) are increased by 83.7 and51 times,respectively.In this research,a promising photocatalyst for photocatalytic degra dation of organic pollutants in wastewater is provided.展开更多
Modulating the electronic structure of a photocatalyst and constructing spatially separated redox sites are key strategies for achieving the photocatalytic dual-channel generation of H_(2)O_(2).In this study,a graphen...Modulating the electronic structure of a photocatalyst and constructing spatially separated redox sites are key strategies for achieving the photocatalytic dual-channel generation of H_(2)O_(2).In this study,a graphene-modified non-compensated Cu/N-co-doped titanium dioxide(Cu-N-TiO_(2)/rGO)photocatalyst was designed for the efficient synthesis of H_(2)O_(2) via a dual-channel pathway.Precise modulation of the TiO_(2) conduction band position was achieved through the synergistic coupling of Cu 3d orbitals hybridized with Ti 3d orbitals and hybridization of N 2p orbitals with O 2p orbitals.This approach significantly improved the utilization of sunlight while satisfying the redox potential requirements.Cu doping not only promoted the formation of oxygen vacancies but also reduced the formation of Ti^(3+)ions,the photogenerated charge recombination centers.The non-compensated doping of N effectively increased the solubility of Cu^(2+)ions in the titanium dioxide lattice,enhanced the adsorption of hydroxyl radical intermediates,and created conditions for the subsequent hydroxyl radical combinations promoting the generation of H_(2)O_(2).In addition,the introduction of highly conductive graphene improved the interfacial carrier separation efficiency while realizing the spatial separation of redox sites,creating conditions for dual-channel reactions.The experimental results showed that the H_(2)O_(2) yield of Cu-N-TiO_(2)/rGO under simulated sunlight reached 1266.7μmol/L,which was 25.2 times higher than that of pristine TiO_(2).This study elucidated the synergistic mechanism of the energy band structure modulation and interfacial optimization,which provided a new idea for the design of dual-channel H_(2)O_(2) production photocatalysts.展开更多
基金supported by CNPC safety and environmental protection key technology research and promotion project (No. 2017D-4613)Sub project of national science and technology major project (No. 2016ZX05040-003)China University of Petroleum (East China) Graduate Innovative Engineering Project (No. YCX2020039)。
文摘High-efficiency photocatalysts are of great significance for the application of photocatalytic technology in water treatment.In this study,N/Cu co-doped ZnS nanosphere photocatalys(N/Cu-ZnS) is synthesized by a hydrothermal method for the first time.After doping,the tex ture of nanosphere becomes loose,the nanometer diameter is reduced,making the specific surface area of catalyst increased from 34.73 to 101.59 m^(2)/g.The characterization results show that more ZnS (111) crystal planes are exposed by N/Cu co-doping;the calculations of density functional theory show that N/Cu co-doping can increase the catalytic activity of the ZnS (111) crystal plane,enhance the adsorption capacity of (111) crystal plane to O_(2)and promote the generation of·O_(2)-.The energy levels of the introduced impurities can be hybridized with the energy levels of S and Zn at the top of valence band and the bottom o conduction band,which makes the band gap narrower,thus enhancing the absorption o visible light.Compared with pure ZnS,the degradation rates of 2,4-dichlorophenol (2,4-DCP and tetracycline (TC) by N/Cu-ZnS under visible light (>420 nm) are increased by 83.7 and51 times,respectively.In this research,a promising photocatalyst for photocatalytic degra dation of organic pollutants in wastewater is provided.
文摘Modulating the electronic structure of a photocatalyst and constructing spatially separated redox sites are key strategies for achieving the photocatalytic dual-channel generation of H_(2)O_(2).In this study,a graphene-modified non-compensated Cu/N-co-doped titanium dioxide(Cu-N-TiO_(2)/rGO)photocatalyst was designed for the efficient synthesis of H_(2)O_(2) via a dual-channel pathway.Precise modulation of the TiO_(2) conduction band position was achieved through the synergistic coupling of Cu 3d orbitals hybridized with Ti 3d orbitals and hybridization of N 2p orbitals with O 2p orbitals.This approach significantly improved the utilization of sunlight while satisfying the redox potential requirements.Cu doping not only promoted the formation of oxygen vacancies but also reduced the formation of Ti^(3+)ions,the photogenerated charge recombination centers.The non-compensated doping of N effectively increased the solubility of Cu^(2+)ions in the titanium dioxide lattice,enhanced the adsorption of hydroxyl radical intermediates,and created conditions for the subsequent hydroxyl radical combinations promoting the generation of H_(2)O_(2).In addition,the introduction of highly conductive graphene improved the interfacial carrier separation efficiency while realizing the spatial separation of redox sites,creating conditions for dual-channel reactions.The experimental results showed that the H_(2)O_(2) yield of Cu-N-TiO_(2)/rGO under simulated sunlight reached 1266.7μmol/L,which was 25.2 times higher than that of pristine TiO_(2).This study elucidated the synergistic mechanism of the energy band structure modulation and interfacial optimization,which provided a new idea for the design of dual-channel H_(2)O_(2) production photocatalysts.
