Xu Mingliang, Li Dandan, Sun Kang, Jiao Long, Xie Chenfan, Ding Chunmei, Jiang Hai-Long
Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Soft Matter Chemistry, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Institute of Physical Science and Information Technology, Anhui University, Hefei, Anhui, 230601, P. R. China.
Angew Chem Int Ed Engl. 2021 Jul 19;60(30):16372-16376. doi: 10.1002/anie.202104219. Epub 2021 Jun 24.
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 ), Pt with partially removed PVP (Pt ), and clean Pt without PVP (Pt), were encapsulated into a metal-organic framework (MOF), UiO-66-NH , to afford Pt @UiO-66-NH , Pt @UiO-66-NH , and Pt@UiO-66-NH , 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 @UiO-66-NH , the removal of interfacial PVP improves the sluggish kinetics of electron transfer, boosting photocatalytic hydrogen production.
助催化剂与光敏剂之间的界面电子转移是多相光催化的关键，但潜在机制仍微妙且不明。涂覆在金属助催化剂上的表面活性剂极大地调节了催化位点的微环境，却在很大程度上被忽视。在此，一系列具有调节微环境的铂助催化剂，包括聚乙烯吡咯烷酮（PVP）包覆的铂纳米颗粒（记为Pt ）、部分去除PVP的Pt（Pt ）和无PVP的纯净Pt（Pt），被封装到金属有机框架（MOF）UiO-66-NH 中，分别得到Pt @UiO-66-NH 、Pt @UiO-66-NH 和Pt@UiO-66-NH 用于光催化产氢。PVP似乎对Pt与MOF之间的界面电子转移有负面影响。与Pt @UiO-66-NH 相比，界面PVP的去除改善了迟缓的电子转移动力学，促进了光催化产氢。
