Trinuclear Nickel Catalyst for Water Oxidation: Intramolecular Proton- Coupled Electron Transfer Triggered Trimetallic Cooperative O-O Bond Formation

被引：24

作者：

Chen, Qi-Fa ^{[1
]}

Xiao, Yao ^{[1
]}

Liao, Rong-Zhen ^{[2
]}

Zhang, Ming-Tian ^{[1
]}

机构：

[1] Tsinghua Univ, Dept Chem, Ctr Basic Mol Sci CBMS, Beijing 100084, Peoples R China

[2] Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Key Lab Mat Chem Energy Convers & Storage, Minist Educ, Wuhan 430074, Peoples R China

来源：

CCS CHEMISTRY | 2023年 / 5卷 / 01期

基金：

美国国家科学基金会;

关键词：

water oxidation; proton-coupled electron transfer; nickel catalyst; artificial photosynthesis; O-O bond formation; NEUTRAL PH; OXYGEN-EVOLUTION; ARTIFICIAL PHOTOSYNTHESIS; ONE-SITE; COMPLEXES; ELECTROCATALYST; CLUSTER; EFFICIENT; HYDROXYLATION; INTERMEDIATE;

D O I：

10.31635/ccschem.022.202101668

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We report a molecular trinuclear nickel (TNC-Ni) catalyst for water oxidation that exhibited high catalytic performance and stability under neutral conditions (pH 7). Electrochemical studies disclosed that cooperation among the three nickel sites plays a vital role in both charge accumulation and O-O bond formation. This TNC-Ni catalyst could accomplish 4e(-) oxidation of water by involving all three nickel sites and the O-O bond formation was triggered by a charge distribution process from 5 to 5dp via proton-coupled electron transfer.

引用

页码：245 / 256

页数：12

共 40 条

[1] Pivotal Role of Geometry Regulation on O-O Bond Formation Mechanism of Bimetallic Water Oxidation Catalysts
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[2] Bimetallic cooperative effect on O-O bond formation: copper polypyridyl complexes as water oxidation catalyst
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[9] O-O bond formation via radical coupling in a dinuclear iron water oxidation catalyst with high catalytic activity
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[10] Impact of the Ligand Flexibility and Solvent on the O-O Bond Formation Step in a Highly Active Ruthenium Water Oxidation Catalyst
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