Engineering the electronic properties of semiconductor-based photocatalysts using elemental doping is an effective approach to improve their catalytic activity.Nevertheless,there still remain contradictions regarding ...Engineering the electronic properties of semiconductor-based photocatalysts using elemental doping is an effective approach to improve their catalytic activity.Nevertheless,there still remain contradictions regarding the role of the dopants played in photocatalysis.Herein,ultrathin ZnIn_(2)S_(4)(ZIS) nanosheets with oxygen doping were synthesized by a one-pot solvothermal method.XRD,XPS and Raman spectral measurements support the presence of lattice oxygen in the oxygen-doped ZIS(O-ZIS) sample.With optimum doping of oxygen,the ultrathin O-ZIS nanosheets show enhanced CO_(2)-to-CO conversion activity with a CO_(2)-evolving rate of 1680 μmol h^(-1) g^(-1) under visible light irradiation,which is about 7 times higher than that of the pristine ZIS.First-principle calculations support that doping of oxygen in the lattice of ZnIn_(2)S_(4) nanosheets plays a key role in tuning its electronic properties.The remarkable photocatalytic performance of O-ZIS can be assigned to a synergistic consequence of a unique ultrathin-layered structure and an upward shift of the conduction band minimum(CBM) caused by the oxygen doping into ZIS and the quantum confinement effect(QCE) induced by the decreased particle size after doping as well as to the improved charge separation efficiency.The present work offers a simple elemental doping method to promote charge separation at atomic level and illustrates the roles played by oxygen doping in photocatalysis,giving new insights into highly efficient artificial photosynthesis.展开更多
基金financially supported by the National Natural Science Foundation of China(Grants Nos.21976116 and 21902095)Shaanxi Science and Technology Program(2020KWZ005)+3 种基金SAFEA of China(High-end foreign expert project # G20190241013)Natural Foundation of Shaanxi Province(No.2020JQ-711)Group Linkage Program of Alexander-vonHumboldt Foundation of Germanythe scientific research startup fund of Shannxi University of Science and Technology。
文摘Engineering the electronic properties of semiconductor-based photocatalysts using elemental doping is an effective approach to improve their catalytic activity.Nevertheless,there still remain contradictions regarding the role of the dopants played in photocatalysis.Herein,ultrathin ZnIn_(2)S_(4)(ZIS) nanosheets with oxygen doping were synthesized by a one-pot solvothermal method.XRD,XPS and Raman spectral measurements support the presence of lattice oxygen in the oxygen-doped ZIS(O-ZIS) sample.With optimum doping of oxygen,the ultrathin O-ZIS nanosheets show enhanced CO_(2)-to-CO conversion activity with a CO_(2)-evolving rate of 1680 μmol h^(-1) g^(-1) under visible light irradiation,which is about 7 times higher than that of the pristine ZIS.First-principle calculations support that doping of oxygen in the lattice of ZnIn_(2)S_(4) nanosheets plays a key role in tuning its electronic properties.The remarkable photocatalytic performance of O-ZIS can be assigned to a synergistic consequence of a unique ultrathin-layered structure and an upward shift of the conduction band minimum(CBM) caused by the oxygen doping into ZIS and the quantum confinement effect(QCE) induced by the decreased particle size after doping as well as to the improved charge separation efficiency.The present work offers a simple elemental doping method to promote charge separation at atomic level and illustrates the roles played by oxygen doping in photocatalysis,giving new insights into highly efficient artificial photosynthesis.
