中国科学技术大学江海龙报道了界面微环境调制促进金属纳米粒子与MOFs之间的电子转移增强光催化。 相关研究成果于2021年5月14日发表于国际一流学术期刊《德国应用化学》。

共催化剂与光敏剂之间的界面电子转移在多相光催化中起着关键作用，但其机理尚不清楚。尤其是金属助催化剂表面包裹的表面活性剂极大地调节了催化中心的微环境，但很大程度上被忽略了。

该文中，一系列具有调节微环境的铂共催化剂，包括聚乙烯吡咯烷酮（PVP）包覆的铂纳米颗粒（表示为Pt-PVP）、部分去除PVP的铂（Pt-rPVP）和不含PVP的清洁铂（Pt），已被封装到具有代表性的金属-有机骨架（MOF）UiO-66-NH 2中，提供铂PVP@UiO‐66‐NH 2，铂rPVP@UiO‐66‐NH 2，以及Pt@UiO66-NH 2，分别用于光催化制氢。

系统研究表明，PVP对Pt与MOF之间的界面电子转移有负面影响。与Pt-PVP@UiO‐66‐nh2相比，界面PVP的去除有效地改善了电子转移的迟滞动力学，从而促进了光催化制氢。

附：英文原文

Title: Interfacial Microenvironment Modulation Boosting Electron Transfer between Metal Nanoparticles and MOFs for Enhanced Photocatalysis

Author: Mingliang Xu, Dandan Li, Kang Sun, Long Jiao, Chenfan Xie, Chunmei Ding, Hai-Long Jiang

Issue&Volume: 2021-05-14

Abstract: Interfacial electron transfer between cocatalyst and photosensitizer plays a key role in heterogeneous photocatalysis, yet the underlying mechanism remains subtle and unclear. Particularly, the 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), have been encapsulated into a representative metal‐organic framework (MOF), UiO‐66‐NH  2  , to afford Pt  PVP  @UiO‐66‐NH  2  , Pt  rPVP  @UiO‐66‐NH  2  , and Pt@UiO‐66‐NH  2  , respectively, for photocatalytic hydrogen production. Systemic investigations suggest that the PVP presents a negative influence on the interfacial electron transfer between Pt and the MOF. Compared with Pt  PVP  @UiO‐66‐NH  2  , the removal of interfacial PVP effectively improves the sluggish kinetics of electron transfer, accordingly boosting the photocatalytic hydrogen production.

DOI: 10.1002/anie.202104219

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202104219