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Proton-coupled redox properties and water oxidation catalysis of an aqua-coordinated (mu-oxo)diruthenium(III) complex

文献类型： 外文期刊

作者： Luo, Bo-Hong 1 ; Ren, Ya-Jie 1 ; Cui, Hai-Bin 1 ; Fu, Qiang 1 ; Jiang, Hao-Dong 1 ; Du, Huan-Fa 1 ; Xie, Qin 1 ; Li, Peng 1 ;

作者机构： 1.Guangxi Univ, Coll Chem & Chem Engn, 100 Daxue East Rd, Nanning 530004, Guangxi, Peoples R China

2.Guangxi Acad Agr Sci, Res Inst Agroprod Qual Safety & Testing Technol, Nanning 530007, Guangxi, Peoples R China

3.Guangxi Coll & Univ Key Lab Appl Chem Technol & R, Nanning 530004, Guangxi, Peoples R China

关键词： Ruthenium complex; Proton-coupled electron transfer; Catalysis; Water oxidation reaction

期刊名称：INORGANICA CHIMICA ACTA （ 影响因子：2.545； 五年影响因子：2.235 ）

ISSN： 0020-1693

年卷期： 2021 年 514 卷

页码：

收录情况： SCI

摘要： The electronic absorption and redox properties as well as the catalysis for water oxidation reaction (WOR) of an aqua-coordinated oxo-bridged diruthenium(III) complex trans(mu-O,OH2)-[Ru-2(mu-O)(mu-CH3COO)(2)(bpy)(2)(H2O)(2)] (PF6)(2)center dot 3H(2)O ([1](PF6)(2)center dot 3H(2)O; bpy = 2,2'-bipyridine) in aqueous media are reported. [1](2+) displays a visible absorption band at 566 nm ascribed to metal-to-metal charge transition (MMCT) within the Ru2O core. This visible band redshifts due to the deprotonation of the terminal aqua ligands of [1](2+) in alkaline solutions. [1](2+) shows proton-coupled electron transfer behaviors in aqueous solutions at pH 0-14. The oxidation of (RuRuII)-Ru-III in [1](2+) has successfully reached the higher oxidation states including (RuRuIV)-Ru-IV and (RuRuV)-Ru-V which are stabilized by the deprotonation of the terminal aqua ligands and are important for catalytic water oxidation. WOR catalyzed by [1](2+) in acidic solutions was studied using electrochemical and chemical oxidation. In the solution of [1](2+) at pH 1.0, the overpotential for WOR was similar to 0.38 V. A turnover number of 23 was obtained by using (NH4)(2)Ce(NO3)(6 )as the oxidant. A nucleophilic-attack catalytic mechanism was proposed.

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