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双原子和寡核光催化剂驱动的光解水制氢中催化中心的稳定性。

Stability of Catalytic Centres in Light-Driven Hydrogen Evolution by Di- and Oligonuclear Photocatalysts.

机构信息

Institute of Inorganic Chemistry I, Ulm University, Albert-Einstein-Allee 11, 89081, Ulm, Germany.

Institute of Physical Chemistry, Friedrich Schiller University Jena, Helmholtzweg 4, 07743, Jena, Germany.

出版信息

Chemistry. 2023 Jun 27;29(36):e202202722. doi: 10.1002/chem.202202722. Epub 2023 May 12.

DOI:10.1002/chem.202202722
PMID:36807573
Abstract

A review. In recent decades, mimicking natural photosynthesis by artificial photocatalysis represented a major research direction with the ultimate goal of reducing fossil fuel consumption through efficient solar energy harvesting. To transfer molecular photocatalysis from the lab scale to an industrially relevant process, it is important to overcome instability problems of the catalysts during light-driven operation. As it is well-known that many of the typically utilized noble metal-based catalytic centres (e. g. Pt and Pd) undergo particle formation during (photo)catalysis and thus switch the whole process from a homogeneous into a heterogeneous one, an understanding of the factors governing particle formation is crucially needed. The review therefore focuses on di- and oligonuclear photocatalysts bearing a range of different bridging ligand architectures for drawing structure-catalyst-stability relationships in light-driven intramolecular reductive catalysis. In addition, ligand effects at the catalytic centre and their implications for catalytic activity in intermolecular systems will be discussed, as will important insights into the future design of operationally stable catalysts.

摘要

综述。近几十年来,通过人工光催化模拟自然光合作用是一个主要的研究方向,其最终目标是通过高效的太阳能收集来减少化石燃料的消耗。为了将分子光催化从实验室规模转移到工业相关的过程中,克服催化剂在光驱动操作过程中的不稳定性问题是很重要的。众所周知,许多常用的基于贵金属的催化中心(例如 Pt 和 Pd)在(光)催化过程中会形成颗粒,从而将整个过程从均相转变为多相,因此需要了解控制颗粒形成的因素。因此,本综述重点介绍了一系列具有不同桥联配体结构的双核和寡核光催化剂,以在光驱动的分子内还原催化中得出结构-催化剂-稳定性关系。此外,还将讨论催化中心的配体效应及其对分子间体系催化活性的影响,并深入了解未来操作稳定催化剂的设计。

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