物理化学学报2023，Vol.39Issue(11)：120-130,11.DOI:10.3866/PKU.WHXB202302017
S-型异质结CeO2/ZnxCd1-xIn2S4空心结构的构建及其可见光分解水制氢性能
Constructing a CeO2/ZnxCd1-xIn2S4 S-Scheme Hollow Heterostructure for Efficient Photocatalytic H2 Evolution
摘要
Abstract
With the exhaustion of fossil energy,the energy crisis is becoming increasingly serious,which greatly hinders the sustainable development of society.Therefore,the development of new energy technologies as a substitute for non-renewable and highly polluting fossil energy is extremely urgent.The environmental benefits and high energy density of hydrogen(H2)make it an ideal clean energy source.Photocatalytic water splitting,which was first demonstrated in the pioneering work on TiO2 photoelectrodes under UV-light irradiation,has been extensively researched and has been shown to be an effective method for addressing the global energy crisis.However,most of the photocatalysts used for H2 production still suffer from low solar energy utilization and fast photogenerated charge recombination,which seriously limit their practical applications in the field of solar-to-hydrogen energy conversion.Therefore,it is necessary yet greatly challenging to develop a visible-light-responsive photocatalyst with efficient photogenerated charge separation through reasonable modification strategy.Layered structured ZnIn2S4(ZIS)is a promising photocatalyst to split water for H2 evolution owing to its suitable electronic structure,strong light absorption,chemical stability,and low toxicity.However,its low charge separation efficiency renders its photocatalytic performance unsatisfactory.Herein,to overcome this issue,a band structure regulation strategy that integrates solid solution formation with heterostructure construction was proposed.By growing ZnxCd1-xIn2S4(ZCIS)nanosheets on the surface of CeO2 hollow spheres in situ,a novel hollow heterostructure CeO2/ZCIS with efficient charge separation was constructed as photocatalyst for H2 generation.The introduction of the Cd cation in ZIS upshifts the conduction band(CB)and valence band(VB)of ZCIS,enhancing the built-in electrical field on the interface.Those electronic band changes induce the S-scheme structure in CeO2/ZCIS,promoting charge separation for photocatalysis.Moreover,the upshift of the CB generates photoelectrons with high H2 generation ability.As a result,the optimal 1:6-CeO2/Zn0.9Cd0.1In2S4 heterostructure exhibits 4.09 mmol·g-1·h-1 H2 generation during photocatalysis,which is 6.8-,3.0-,and 2.2-fold as those of ZIS,ZCIS,and CeO2/ZIS,respectively.This work provides one efficient strategy to develop highly active S-scheme photocatalysts for hydrogen generation.关键词
光催化/制氢/S-型异质结/内建电场/电荷分离Key words
Photocatalysis/Hydrogen generation/S-scheme heterostructure/Build-in electrical field/Charge separation分类
化学化工引用本文复制引用
蔡晓燕,杜家豪,钟光明,张一鸣,毛梁,娄在祝..S-型异质结CeO2/ZnxCd1-xIn2S4空心结构的构建及其可见光分解水制氢性能[J].物理化学学报,2023,39(11):120-130,11.基金项目
国家自然科学基金(22209203,22175076),中国博士后科学基金(2021M693419),江苏省煤基温室气体减排与资源化利用重点实验室"鹏程尚学教育金"(PCSX202202),中国矿业大学材料科学与工程学科引导基金(CUMTMS202202,CUMTMS202207),中国矿业大学大学生创新创业训练计划(202210290200Y)资助项目 The project was supported by the National Natural Science Foundation of China(22209203,22175076),the China Postdoctoral Science Foundation(2021M693419),the Pengcheng Shangxue Education Fund of Jiangsu Key Laboratory of Coal-Based Greenhouse Gas Control and Utilization(PCSX202202),the Material Science and Engineering Discipline Guidance Fund of China University of Mining and Technology(CUMTMS202202,CUMTMS202207),and the Undergraduate Training Program for Innovation and Entrepreneurship of China University of Mining and Technology(202210290200Y). （22209203,22175076）
