Science China Materials ( IF 6.8 ) Pub Date : 2023-03-27 , DOI: 10.1007/s40843-022-2380-x Xiaoxu Deng , Peng Chen , Xu Wang , Ruirui Cui , Chaoyong Deng
Nondirectional migration of photogenerated electron-hole pairs and the coordinated activation of multiple molecules are large barriers to simultaneous photocatalytic reactions. Here, ZnIn2S4 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 (4650.1 µmol h−1) coupled with a selective benzylamine oxidation rate (7386.7 µmol 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.
中文翻译:
ZnIn2S4 中双空位介导的极化电场增强光催化析氢与选择性苄胺氧化
光生电子-空穴对的非定向迁移和多个分子的协同激活是同时进行光催化反应的巨大障碍。在这里,使用简便的水热和碱蚀刻策略合成了具有双空位的ZnIn 2 S 4纳米片 (DZIS)。在没有助催化剂的情况下,出色的光催化析氢速率 (4650.1 µmol h -1 ) 和选择性的苄胺氧化速率 (7386.7 µmol h -1) 是通过 DZIS 获得的。理论和实验结果表明,双空位引起电子结构重组并扩大极化电场,促进电荷载流子的定向迁移和激子解离。此外,Zn 和 S 空位充当吸附 H +离子和苯甲胺的活性位点,以降低表面反应势垒。这项工作为极化电场建立了一种新方法,并提供了对析氢机制的深刻理解。