Interfacial Microenvironment Modulation Boosting Electron Transfer between Metal Nanoparticles and MOFs for Enhanced Photocatalysis,Angewandte Chemie International Edition

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Interfacial Microenvironment Modulation Boosting Electron Transfer between Metal Nanoparticles and MOFs for Enhanced Photocatalysis
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-05-14 , DOI: 10.1002/anie.202104219
Mingliang Xu ₁ , Dandan Li ₂ , Kang Sun ₁ , Long Jiao ₁ , Chenfan Xie ₁ , Chunmei Ding ₃ , Hai-Long Jiang ₁

Affiliation

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.

中文翻译：

界面微环境调节促进金属纳米颗粒和 MOF 之间的电子转移以增强光催化

助催化剂和光敏剂之间的界面电子转移是多相光催化的关键，但其潜在机制仍然微妙和不清楚。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，但在很大程度上被忽略了。在此，一系列具有调节微环境的 Pt 助催化剂，包括聚乙烯吡咯烷酮（PVP）封端的 Pt 纳米粒子（表示为 Pt _PVP）、部分去除 PVP 的 Pt（Pt _rPVP）和不含 PVP 的清洁 Pt（Pt），被封装到金属有机骨架 (MOF) UiO-66-NH ₂，以提供 Pt _PVP @UiO-66-NH ₂、Pt _rPVP @UiO-66-NH ₂和 Pt@UiO-66-NH ₂分别用于光催化制氢。PVP 似乎对 Pt 和 MOF 之间的界面电子转移有负面影响。与 Pt _PVP @UiO-66-NH _{2 相比}，界面 PVP 的去除改善了电子转移的缓慢动力学，促进了光催化产氢。

更新日期：2021-07-12

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