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Bidirectional O2 reduction/H2O oxidation boosted by a pentadentate pyridylalkylamine copper(II) complex

文献类型: 外文期刊

作者: Zhang, Xiao 1 ; Chen, Gui-Shan 1 ; Liu, Hao-Cheng 1 ; Zhu, Ming -Jun 1 ; Xie, Ming-Yi 1 ; Cen, Ming-Sheng 1 ; Li, Qi-Jun 1 ; Wang, Tian -Shun 1 ; Zhang, Hua-Xin 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

关键词: Copper(II) complex; Polypyridine ligand; Oxygen reduction reaction; Water oxidation reaction; Electrocatalyst

期刊名称:ELECTROCHIMICA ACTA ( 影响因子:6.6; 五年影响因子:6.0 )

ISSN: 0013-4686

年卷期: 2023 年 446 卷

页码:

收录情况: SCI

摘要: The development of catalysts for oxygen reduction reaction (ORR) and water oxidation reaction (WOR) is important for promoting the utilization of renewable energy sources. Catalysts based on Earth-abundant metals are low-cost and benefit the widespread use. Herein a mononuclear copper complex [Cu(tpmen)](ClO4)2 (Cu-tpmen) of the pentadentate pyridylalkylamine ligand N,N,N'-tris(2-pyridylmethyl)-N'-methylethylenediamine (tpmen) was synthesized and characterized. The electrochemical properties and the catalysis for the ORR and the WOR by Cu-tpmen in aqueous solutions were studied. Cu-tpmen in pH 7.0 0.1 M phosphate buffer solution (PBS) can boost the ORR with an onset potential at 0.47 V versus the reversible hydrogen electrode (RHE), generating mainly H2O2. The foot-of-the-wave analysis showed that turnover frequency (TOF) of the reduction of O2 to H2O2 mediated by Cu-tpmen was 6.5 x 104 s-1. Meanwhile, Cu-tpmen exhibited catalytic activities for the WOR with the TOF values of 50.9 s-1 (at pH 7.0) and 8.4 s-1 (at pH 10.5). Cu-tpmen was thus a homogeneous bidirectional ORR/WOR catalyst and the reaction mechanisms were proposed. The synergic effect of the flexibility and the electron-donating ability of tpmen benefited the bidirectional catalytic properties of Cu-tpmen.

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