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Annu Rev Biochem. 2020 Jun 20;89:795-820. doi: 10.1146/annurev-biochem-011520-104801. Epub 2020 Mar 24.
2
An oxyl/oxo mechanism for oxygen-oxygen coupling in PSII revealed by an x-ray free-electron laser.X 射线自由电子激光揭示 PSII 中氧-氧耦合的氧化/过氧机制。
Science. 2019 Oct 18;366(6463):334-338. doi: 10.1126/science.aax6998. Epub 2019 Oct 17.
3
Critical Hammett Electron-Donating Ability of Substituent Groups for Efficient Water Oxidation Catalysis by Mononuclear Ruthenium Aquo Complexes.单核钌水合配合物高效水氧化催化中取代基的关键哈米特电子给体能力。
Inorg Chem. 2019 Oct 7;58(19):12716-12723. doi: 10.1021/acs.inorgchem.9b01623. Epub 2019 Sep 24.
4
Artificial photosynthesis: opportunities and challenges of molecular catalysts.人工光合作用：分子催化剂的机遇与挑战。
Chem Soc Rev. 2019 Apr 1;48(7):2216-2264. doi: 10.1039/c8cs00897c.
5
Recent Advances in the Development of Molecular Catalyst-Based Anodes for Water Oxidation toward Artificial Photosynthesis.用于人工光合作用水氧化的基于分子催化剂的阳极开发的最新进展
ChemSusChem. 2019 May 8;12(9):1775-1793. doi: 10.1002/cssc.201802795. Epub 2019 Apr 18.
6
Structures of the intermediates of Kok's photosynthetic water oxidation clock.科克光合作用水氧化钟中间产物的结构。
Nature. 2018 Nov;563(7731):421-425. doi: 10.1038/s41586-018-0681-2. Epub 2018 Nov 7.
7
Mechanisms of molecular water oxidation in solution and on oxide surfaces.水溶液和氧化物表面上的分子水氧化机制。
Chem Soc Rev. 2017 Oct 16;46(20):6148-6169. doi: 10.1039/c7cs00465f.
8
O-O bond formation in ruthenium-catalyzed water oxidation: single-site nucleophilic attack vs. O-O radical coupling.钌催化水氧化中的 O-O 键形成：单活性位亲核进攻与 O-O 自由基偶联。
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9
Mechanistic Insight into Reversible Core Structural Changes of Dinuclear μ-Hydroxoruthenium(II) Complexes with a 2,8-Di-2-pyridyl-1,9,10-anthyridine Backbone Prior to Water Oxidation Catalysis.水氧化催化之前具有2,8 - 二 - 2 - 吡啶基 - 1,9,10 - 蒽啶骨架的双核μ - 羟基钌（II）配合物可逆核心结构变化的机理洞察
Inorg Chem. 2017 Sep 5;56(17):10235-10246. doi: 10.1021/acs.inorgchem.7b00978. Epub 2017 Aug 24.
10
A supramolecular ruthenium macrocycle with high catalytic activity for water oxidation that mechanistically mimics photosystem II.一种具有高催化活性的超分子钌大环，可在机制上模拟光合作用 II 系统用于水氧化。
Nat Chem. 2016 Jun;8(6):576-83. doi: 10.1038/nchem.2503. Epub 2016 May 2.

通过低价态 Ru(III)中心顺式羟基金属配体的分子内偶联，促进 H 解离诱导的 O-O 键形成的机理。

Mechanism of H dissociation-induced O-O bond formation via intramolecular coupling of vicinal hydroxo ligands on low-valent Ru(III) centers.

机构信息

Department of Materials Science and Technology, Faculty of Engineering, Niigata University, Niigata 950-2181, Japan.

Photon Factory, High Energy Accelerator Research Organization, Institute of Materials Structure Science, Tsukuba 305-0801, Japan.

出版信息

Proc Natl Acad Sci U S A. 2021 Dec 28;118(52). doi: 10.1073/pnas.2113910118.

DOI:10.1073/pnas.2113910118
PMID:34934002
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8719882/
Abstract

The understanding of O-O bond formation is of great importance for revealing the mechanism of water oxidation in photosynthesis and for developing efficient catalysts for water oxidation in artificial photosynthesis. The chemical oxidation of the Ru(OH)(OH) core with the vicinal OH and OH ligands was spectroscopically and theoretically investigated to provide a mechanistic insight into the O-O bond formation in the core. We demonstrate O-O bond formation at the low-valent Ru(OH) core with the vicinal OH ligands to form the Ru(μ-OOH) core with a μ-OOH bridge. The O-O bond formation is induced by deprotonation of one of the OH ligands of Ru(OH) via intramolecular coupling of the OH and deprotonated O ligands, conjugated with two-electron transfer from two Ru centers to their ligands. The intersystem crossing between singlet and triple states of Ru(μ-OOH) is easily switched by exchange of H between the μ-OOH bridge and the auxiliary backbone ligand.

摘要

O-O 键形成的理解对于揭示光合作用中水氧化的机制以及开发人工光合作用中水氧化的高效催化剂具有重要意义。本研究通过光谱和理论研究考察了偕位 OH 和 OH 配体对 Ru(OH)(OH)核的化学氧化，以深入了解核心中 O-O 键的形成机制。我们证明了偕位 OH 配体的低氧化态 Ru(OH)核中 O-O 键的形成，形成了具有 μ-OOH 桥的 Ru(μ-OOH)核。O-O 键的形成是通过 Ru(OH)的一个 OH 配体的去质子化诱导的，其中 OH 和去质子化的 O 配体通过分子内偶联，伴随着两个 Ru 中心到其配体的两个电子转移。Ru(μ-OOH)的单重态和三重态之间的系间交叉可以通过 μ-OOH 桥和辅助骨架配体之间的 H 交换轻松切换。