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异金属镧系-钛氧簇:一类新型水氧化催化剂

Heterometallic Lanthanide-Titanium Oxo Clusters: A New Family of Water Oxidation Catalysts.

作者信息

Lu Dong-Fei, Kong Xiang-Jian, Lu Tong-Bu, Long La-Sheng, Zheng Lan-Sun

机构信息

Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surface, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University , Xiamen 361005, China.

Key Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-Sen University , Guangzhou 510275, China.

出版信息

Inorg Chem. 2017 Feb 6;56(3):1057-1060. doi: 10.1021/acs.inorgchem.6b03072. Epub 2017 Jan 24.

Abstract

We report the synthesis and photoelectrochemical activity of three lanthanide-titanium oxo clusters (LTOCs), formulated as [LnTi(μ-O)(tbba)(Ac)(HO)(THF)]·2Htbba [Ln = Eu (1), Sm (2), and Gd (3); Htbba = 4-tert-butylbenzoic acid; Ac = acetate]. These stable compounds are efficient catalysts of photoelectrochemical water oxidation with high turnover numbers (7581.0 for 1, 5172.4 for 2, and 5413.0 for 3) and high turnover frequencies (2527.0 for 1, 1724.1 for 2, and 1804.0 for 3). The differences in the photoelectrochemical activity among these three compounds may be related to the differences in their band gaps. This work shows that the heterometallic LTOCs provide a tunable platform for the design of highly effective water oxidation catalysts.

摘要

我们报道了三种镧系-钛氧簇(LTOCs)的合成及其光电化学活性,其化学式为[LnTi(μ-O)(tbba)(Ac)(HO)(THF)]·2Htbba [Ln = Eu (1)、Sm (2) 和 Gd (3);Htbba = 4-叔丁基苯甲酸;Ac = 乙酸盐]。这些稳定的化合物是光电化学水氧化的高效催化剂,具有高周转数(1为7581.0,2为5172.4,3为5413.0)和高周转频率(1为2527.0,2为1724.1,3为1804.0)。这三种化合物之间光电化学活性的差异可能与其带隙差异有关。这项工作表明,异金属LTOCs为设计高效水氧化催化剂提供了一个可调节的平台。

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