Boosting Hydrogenation of Graphene Quantum Dot-Modified Photocatalysts: Specific Functionalized Modulation at Active Sites

作者：Linjia Li, Rui Zhang, Pan Hou, Yanhong Lin, Dejun Wang, Tengfeng Xie · 发表于：ACS Catalysis · 年份：2023 · DOI：10.1021/acscatal.3c01181 · 被引用次数：38 · 研究领域：Advanced Photocatalysis Techniques、Carbon and Quantum Dots Applications、Quantum Dots Synthesis And Properties

Engineering the electronic structure of active sites on photocatalyst surfaces can help realize high activity through strong interactions with reactants. However, unimpeded photo-charge transport is highly limited by a mismatch between pristine catalysts and reactants because of the lack of group-specific modulated synthesis of semiconductor-based catalysts. In this study, hollow TiO 2 /poly(diallyl-dimethylammonium chloride)/graphene quantum dot (GQD) hybrid catalysts were established through a noncovalent self-assembly surface modification strategy. The multilayered nanostructure of the composite catalysts ensures a synchronous charge transfer chain for directional photo-charge migration. Furthermore, GQDs with different hydroxyl contents were deposited onto the hybrids for tuning the catalyst-reactant interfacial coupling. Transient-state surface photovoltage analysis revealed that group-specific absorption and activation dominated the interfacial photo-charge transport dynamics between the catalysts and reactants. The proposed strategy may facilitate the maneuvering of the active sites of semiconductor-based catalysts for improving specific hydrogenation reactions.