Aqueous colloidal dispersions containing Znx Cd1‐x S quantum dots (QDs) of different x compositions were prepared by precipitating zinc and cadmium acetates with sodium sulphide,in the presence of a cetyltrimethylamm...Aqueous colloidal dispersions containing Znx Cd1‐x S quantum dots (QDs) of different x compositions were prepared by precipitating zinc and cadmium acetates with sodium sulphide,in the presence of a cetyltrimethylammonium bromide stabilizer.Ultraviolet‐visible absorption spectroscopy was used to determine the transition energies of the QDs,which in turn were used to calculate their sizes,which depended on their composition.The QD size decreased with increasing Zn content.The photocatalytic activity of the Znx Cd1‐x S QDs was studied by the decomposition of methylene blue under ultraviolet irradiation,at a maximum intensity at 365 nm (3.4 e V).Three different photo‐catalytic activity regions were observed,which depended on the Zn content.The quantum levels of the QDs could be excited by incident irradiation,and influenced the resulting photocatalytic activity.Maximum photocatalytic activity was achieved at x = 0.6,where the QD transition energy was equal to the irradiation photon energy.The photocatalytic efficiency of the QDs depended on their surface area and arrangement of quantum levels,because of the quantum size effect.展开更多
Photocatalytic water splitting for hydrogen(H_(2))production is a green sustainable technology,in which highly-efficient steady photocatalysts are fundamentally required.In this work,unique CdS/Cd_(0.5)Zn_(0.5)S-M0_(1...Photocatalytic water splitting for hydrogen(H_(2))production is a green sustainable technology,in which highly-efficient steady photocatalysts are fundamentally required.In this work,unique CdS/Cd_(0.5)Zn_(0.5)S-M0_(1-x)W_(x)S_(2) photocatalyst constructed by CdS hollow nano-spheres with successively surface-modified Cd_(0.5)Zn_(0.5)S shell and defect-rich MO_(1-x)W_(x)S_(2) ultrathin nanosheets was reported for the first time.Interestingly,the Cd_(0.5)Zn_(0.5)S shell could greatly enhance the photo-stability and reduce the carrier recombination of CdS.Meanwhile,enriching active sites and accelerating charge transfer could be achieved via anchoring defect-rich Mo_(1-x)W_(x)S_(2) onto CdS/Cd_(0.5)Zn_(0.5)S hollow heterostructures.Specifically,the optimized CdS/Cd_(0.5)Zn_(0.5)S-Mo_(1-x)W_(x)Sa(6 h Cd_(0.5)Zn_(0.5)S-coating,7 wt.%Mo_(1-x)W_(x)S_(2),x=0.5)hybrid delivered an exceptional H_(2) generation rate of 215.99 mmol·g^(-1)·h^(-1),which is approximately 502,134,and 23 times that of pure CdS,CdS/Cd_(0.5)Zn_(0.5)S,and 3 wt.%Pt-loaded CdS/Cd_(0.5)Zn_(0.5)S,respectively.Remarkably,a high H_(2) evolution reaction(HER)apparent quantum yield(AQY)of 64.81%was obtained under 420-nm irradiation.In addition,the CdS/Cd_(0.5)Zn_(0.5)S-Mo_(1-x)W_(x)S_(2) was also durable for H2 production under long-term irradiation.This work provides valuable inspirations to rational design and synthesis of efficient and stable hybrid photocatalysts for solar energy conversion.展开更多
基金supported by the Czech Science Foundation(P107/11/1918)by the Ministry of Education,Youth and Sports of the Czech Republic in the“National Feasibility Program I”,project LO1208“TEWEP”by VSB‐Technical University of Ostrava(SP 2014/55)
文摘Aqueous colloidal dispersions containing Znx Cd1‐x S quantum dots (QDs) of different x compositions were prepared by precipitating zinc and cadmium acetates with sodium sulphide,in the presence of a cetyltrimethylammonium bromide stabilizer.Ultraviolet‐visible absorption spectroscopy was used to determine the transition energies of the QDs,which in turn were used to calculate their sizes,which depended on their composition.The QD size decreased with increasing Zn content.The photocatalytic activity of the Znx Cd1‐x S QDs was studied by the decomposition of methylene blue under ultraviolet irradiation,at a maximum intensity at 365 nm (3.4 e V).Three different photo‐catalytic activity regions were observed,which depended on the Zn content.The quantum levels of the QDs could be excited by incident irradiation,and influenced the resulting photocatalytic activity.Maximum photocatalytic activity was achieved at x = 0.6,where the QD transition energy was equal to the irradiation photon energy.The photocatalytic efficiency of the QDs depended on their surface area and arrangement of quantum levels,because of the quantum size effect.
基金support from the National Natural Science Foundation of China(Nos.51802170,51772162,and 21801150)the Natural Science Foundation of Shandong Province(Nos.ZR2019MB001,ZR2018BEM014,and ZR2019JQ14)+3 种基金the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2019KJC004)the Taishan Scholar Project of Shandong Province(No.ts201712047)the Special Fund Project to Guide Development of Local Science and Technology by Central Government,the Open Research Fund of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry of Jilin University(No.2019-22)the Taishan Scholar Program of Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology.
文摘Photocatalytic water splitting for hydrogen(H_(2))production is a green sustainable technology,in which highly-efficient steady photocatalysts are fundamentally required.In this work,unique CdS/Cd_(0.5)Zn_(0.5)S-M0_(1-x)W_(x)S_(2) photocatalyst constructed by CdS hollow nano-spheres with successively surface-modified Cd_(0.5)Zn_(0.5)S shell and defect-rich MO_(1-x)W_(x)S_(2) ultrathin nanosheets was reported for the first time.Interestingly,the Cd_(0.5)Zn_(0.5)S shell could greatly enhance the photo-stability and reduce the carrier recombination of CdS.Meanwhile,enriching active sites and accelerating charge transfer could be achieved via anchoring defect-rich Mo_(1-x)W_(x)S_(2) onto CdS/Cd_(0.5)Zn_(0.5)S hollow heterostructures.Specifically,the optimized CdS/Cd_(0.5)Zn_(0.5)S-Mo_(1-x)W_(x)Sa(6 h Cd_(0.5)Zn_(0.5)S-coating,7 wt.%Mo_(1-x)W_(x)S_(2),x=0.5)hybrid delivered an exceptional H_(2) generation rate of 215.99 mmol·g^(-1)·h^(-1),which is approximately 502,134,and 23 times that of pure CdS,CdS/Cd_(0.5)Zn_(0.5)S,and 3 wt.%Pt-loaded CdS/Cd_(0.5)Zn_(0.5)S,respectively.Remarkably,a high H_(2) evolution reaction(HER)apparent quantum yield(AQY)of 64.81%was obtained under 420-nm irradiation.In addition,the CdS/Cd_(0.5)Zn_(0.5)S-Mo_(1-x)W_(x)S_(2) was also durable for H2 production under long-term irradiation.This work provides valuable inspirations to rational design and synthesis of efficient and stable hybrid photocatalysts for solar energy conversion.
