Heterogeneous and Homogeneous Routes in Water Oxidation Catalysis Starting from Cu(II) Complexes with Tetraaza Macrocyclic Ligands

Chemistry, an Asian Journal
Andrea SartorelMarc Robert

Abstract

Since the first report in 2012, molecular copper complexes have been proposed as efficient electrocatalysts for water oxidation reactions, carried out in alkaline/neutral aqueous media. However, in some cases the copper species have been recognized as precursors of an active copper oxide layer, electrodeposited onto the working electrode. Therefore, the question whether copper catalysis is molecular or not is particularly relevant in the field of water oxidation. In this study, we investigate the electrochemical activity of copper(II) complexes with two tetraaza macrocyclic ligands, distinguishing heterogeneous or homogeneous processes depending on the reaction media. In an alkaline aqueous solution, and upon application of an anodic bias to working electrodes, an active copper oxide layer is observed to electrodeposit at the electrode surface. Conversely, water oxidation in neutral aqueous buffers is not associated to formation of the copper oxide layer, and could be exploited to evaluate and optimize a molecular, homogeneous catalysis.

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Citations

Jul 23, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Ting-Ting Li, Yue-Qing Zheng
Aug 3, 2016·Chemical Communications : Chem Comm·Fengshou YuLicheng Sun
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Oct 24, 2019·Chemistry : a European Journal·Shanti G PatraDan Meyerstein
Aug 2, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Burg ArielaMeyerstein Dan
Jul 21, 2021·The Journal of Physical Chemistry. a·Koteswara Rao Gorantla, Bhabani S Mallik
Jul 27, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Ziyi XuQijian Zhang

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