摘要
光生载流子无定向的迁移及高的反应能垒,严重地抑制了光催化产氢及协同苄胺氧化的效率.本文利用简单的水热与碱刻蚀法制备了富含锌、硫双空位的硫铟化锌.在无共催化剂的条件下,该催化剂展现出优异的光催化产氢性能与苄胺转化速率.实验数据及理论计算表明,双空位重置了硫铟化锌的电子结构,并增强了其极化电场.这些调控将有助于激子的分离及载流子的定向迁移.另外,Zn与S空位充当了氢离子与苄胺吸附的活性位点,极大地提高了其催化活性.因此,本文不仅提供了一种调控极化电场的方法,也为苄胺氧化与协同产氢提供了更深入的见解.
Nondirectional migration of photogenerated electron-hole pairs and the coordinated activation of multiple molecules are large barriers to simultaneous photocatalytic reactions.Here,ZnIn_(2)S_(4)nanosheets with dual vacancies(DZIS)were synthesized using a facile hydrothermal and alkali-etching strategy.In the absence of cocatalysts,an outstanding photocatalytic hydrogen evolution rate(4650.1μmol h^(-1))coupled with a selective benzylamine oxidation rate(7386.7μmol h^(-1))was obtained over DZIS.Theoretical and experimental results uncovered that the dual vacancies induced a reorganization of electronic structure and enlarged the polarization electric field to promote the directional migration of charge carriers and exciton dissociation.Additionally,the Zn and S vacancies acted as active sites for the adsorption of H~+ions and benzylamine to reduce the surface reaction barrier.This work establishes a new method for the polarization electric field and provides a deep understanding of the hydrogen evolution mechanism.
作者
邓晓婿
陈鹏
王旭
崔瑞瑞
邓朝勇
Xiaoxu Deng;Peng Chen;Xu Wang;Ruirui Cui;Chaoyong Deng(School of Electronics and Information Engineering,Guiyang University,Guiyang 550005,China;Key Laboratory of Electronic Composites Materials of Guizhou Province,College of Big Data and Information Engineering,Guizhou University,Guiyang 550025,China;Key Laboratory of Green Chemical and Clean Energy Technology of Guizhou Provincial,School of Chemistry and Chemical Engineering,Guizhou University,Guiyang 550025,China)
基金
supported by the Science and Technology Foundation of Guizhou Province(ZK[2021]yiban 328)
the Postgraduate Education Innovation Program in Guizhou Province(YJSCXJH(2021)202)。
