期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 30, 页码 16372-16376出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202104219
关键词
hydrogen production; interfacial electron transfer; metal-organic frameworks; microenvironment modulation; photocatalysis
资金
- NSFC [21725101, 22161142001, 21521001]
- Dalian National Laboratory Cooperation Fund, CAS [DNL201911]
- Collaborative Innovation Program of Hefei Science Center, CAS [2020HSCCIP005]
The presence of surfactants on the surface of metal cocatalysts can significantly affect the electron transfer rate between the metal and MOF, and removing these surfactants can improve the efficiency of photocatalytic hydrogen production.
Interfacial electron transfer between cocatalyst and photosensitizer is key in heterogeneous photocatalysis, yet the underlying mechanism remains subtle and unclear. Surfactant coated on the metal cocatalysts, greatly modulating the microenvironment of catalytic sites, is largely ignored. Herein, a series of Pt co-catalysts with modulated microenvironments, including polyvinylpyrrolidone (PVP) capped Pt nanoparticles (denoted as Pt-PVP), Pt with partially removed PVP (Pt-rPVP), and clean Pt without PVP (Pt), were encapsulated into a metal-organic framework (MOF), UiO-66-NH2, to afford Pt-PVP@UiO-66-NH2, Pt-rPVP@UiO-66-NH2, and Pt@UiO-66-NH2, respectively, for photocatalytic hydrogen production. The PVP appears to have a negative influence on the interfacial electron transfer between Pt and the MOF. Compared with Pt-PVP@UiO-66-NH2, the removal of interfacial PVP improves the sluggish kinetics of electron transfer, boosting photocatalytic hydrogen production.
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