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

文献类型： 外文期刊

第一作者： Zhang, Xiao

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

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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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