Department of Chemistry, University of Zurich, Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.
Chem Soc Rev. 2021 Mar 1;50(4):2444-2485. doi: 10.1039/d0cs00978d.
The development of reliable water oxidation catalysts (WOCs) is essential for implementing artificial photosynthesis on a large technological scale. WOC research has evolved into two major branches, namely molecular and heterogeneous catalysts. Manifold design principles and plenty of mechanistic insights have been developed in these individual fields after decades of investigations. Over the past years, a growing need for knowledge transfer between both sides has emerged in order to expedite the development and optimization of next-generation WOCs. In this review, we first provide selected recent highlights in the area of molecular WOCs with different nuclearities, together with current mechanistic insight. WOCs offering molecular integrity under operational conditions are ideal platforms for elucidating reaction mechanisms and well-defined structure-function correlations at the atomic level. Next, recent mechanistic advances and design strategies for heterogeneous WOCs are illustrated for representative examples, together with a discussion of their inherent limitations in mechanistic studies. Finally, illustrative cases of knowledge transfer between molecular and heterogeneous WOCs are discussed to highlight the advantages of combining the best of both catalyst types. For the sake of conciseness, this review focuses primarily on WOCs based on the first-row transition metals, which are attracting increasing attention for both fundamental studies and economic applications.
开发可靠的水氧化催化剂（WOC）对于大规模实施人工光合作用至关重要。WOC 研究已经发展成两个主要分支，即分子和多相催化剂。经过几十年的研究，这两个领域都发展出了多种设计原则和大量的机理见解。近年来，为了加速下一代 WOC 的开发和优化，双方之间越来越需要知识的转移。在这篇综述中，我们首先提供了不同核的分子 WOC 领域的一些最新亮点，以及当前的机理见解。在操作条件下提供分子完整性的 WOC 是阐明反应机理和在原子水平上明确结构-功能关系的理想平台。其次，我们以代表性的例子说明了多相 WOC 的最新机理进展和设计策略，并讨论了它们在机理研究中的固有局限性。最后，我们讨论了分子和多相 WOC 之间知识转移的实例，以突出结合两种催化剂类型的优势。为了简洁起见，本综述主要关注基于第一过渡金属的 WOC，这些催化剂在基础研究和经济应用方面都引起了越来越多的关注。
