Driven by endless solar energy,photocatalytic H2 evolution from water splitting and CO_(2) conversion to hydrocarbon fuels over semiconductor photocatalysts are of great potential to simultaneously settle the greenhou...Driven by endless solar energy,photocatalytic H2 evolution from water splitting and CO_(2) conversion to hydrocarbon fuels over semiconductor photocatalysts are of great potential to simultaneously settle the greenhouse effect and energy shortage.Herein,Cr-doped zinc sulfide(ZnS)with accompanying sulphur vacancies(Vs)photocatalytic materials is developed by a facile hydrothermal method.The Cr dopants centralize photoinduced holes and Vs trap electrons,forming a synergistic effect for accelerating charge separation and transfer.The reaction energy barrier for both H2 evolution and CO_(2) reduction has been optimized.Therefore,in the absence of a cocatalyst,the optimal catalyst(Zn_(0.94) Cr_(0.06) S)achieves an out-standing H_(2) evolution activity of 20.3 mmol g^(-1) h^(-1),which is approximately 2.9 times higher than 6.9 mmol g^(-1) h^(-1) for pristine ZnS.In addition,in the gas-solid reaction system without co-catalysts or sacrificial agents,the Zn_(0.94) Cr_(0.06) S exhibits a considerable CO evolution rate of 19.56μmol g^(-1) h^(-1),about 10.1 times higher than ZnS(1.94μmol g^(-1) h^(-1)).Both the performances for H_(2) evolution and CO_(2) reduction of Zn_(0.94) Cr_(0.06) S outperform most of the previously reported photocatalysts.Particularly,the Zn_(0.94) Cr_(0.06) S possesses superior stability,the photoactivity of which exhibits no noticeable deactiva-tion after six cycles’reactions.This work may shed light on the rational design and fabrication of highly efficient materials via combining individual element doping and defect engineering.展开更多
基金supported by the National Natural Sci-ence Foundation of China(No.52002158)the Natural Science Foundation of Jiangxi Province(Nos.20204BCJL23039,20192ACBL21027)The authors would like to thank Prince Sultan University for computational support and Wenjuan Li from Shiyan-jia Lab(www.shiyanjia.com)for the XPS analysis.
文摘Driven by endless solar energy,photocatalytic H2 evolution from water splitting and CO_(2) conversion to hydrocarbon fuels over semiconductor photocatalysts are of great potential to simultaneously settle the greenhouse effect and energy shortage.Herein,Cr-doped zinc sulfide(ZnS)with accompanying sulphur vacancies(Vs)photocatalytic materials is developed by a facile hydrothermal method.The Cr dopants centralize photoinduced holes and Vs trap electrons,forming a synergistic effect for accelerating charge separation and transfer.The reaction energy barrier for both H2 evolution and CO_(2) reduction has been optimized.Therefore,in the absence of a cocatalyst,the optimal catalyst(Zn_(0.94) Cr_(0.06) S)achieves an out-standing H_(2) evolution activity of 20.3 mmol g^(-1) h^(-1),which is approximately 2.9 times higher than 6.9 mmol g^(-1) h^(-1) for pristine ZnS.In addition,in the gas-solid reaction system without co-catalysts or sacrificial agents,the Zn_(0.94) Cr_(0.06) S exhibits a considerable CO evolution rate of 19.56μmol g^(-1) h^(-1),about 10.1 times higher than ZnS(1.94μmol g^(-1) h^(-1)).Both the performances for H_(2) evolution and CO_(2) reduction of Zn_(0.94) Cr_(0.06) S outperform most of the previously reported photocatalysts.Particularly,the Zn_(0.94) Cr_(0.06) S possesses superior stability,the photoactivity of which exhibits no noticeable deactiva-tion after six cycles’reactions.This work may shed light on the rational design and fabrication of highly efficient materials via combining individual element doping and defect engineering.
