Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Materials Chemistry and Service Failure, Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 10691, Stockholm, Sweden.
ChemSusChem. 2017 Nov 23;10(22):4236-4263. doi: 10.1002/cssc.201701374. Epub 2017 Oct 19.
The design of efficient and robust water oxidation catalysts has proven challenging in the development of artificial photosynthetic systems for solar energy harnessing and storage. Tremendous progress has been made in the development of homogeneous transition-metal complexes capable of mediating water oxidation. To improve the efficiency of the catalyst and to design new catalysts, a detailed mechanistic understanding is necessary. Quantum chemical modeling calculations have been successfully used to complement the experimental techniques to suggest a catalytic mechanism and identify all stationary points, including transition states for both O-O bond formation and O release. In this review, recent progress in the applications of quantum chemical methods for the modeling of homogeneous water oxidation catalysis, covering various transition metals, including manganese, iron, cobalt, nickel, copper, ruthenium, and iridium, is discussed.
在开发用于太阳能利用和存储的人工光合作用系统中，高效且稳健的水氧化催化剂的设计一直具有挑战性。在开发能够介导水氧化的均相过渡金属配合物方面已经取得了巨大进展。为了提高催化剂的效率并设计新的催化剂，需要深入了解其作用机制。量子化学建模计算已成功用于补充实验技术，以提出催化机制并确定所有的稳定点，包括 O-O 键形成和 O 释放的过渡态。在这篇综述中，讨论了量子化学方法在均相水氧化催化模拟中的应用的最新进展，涵盖了各种过渡金属，包括锰、铁、钴、镍、铜、钌和铱。
