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钌（乙二胺四乙酸）配合物作为分子氧化还原催化剂用于氧气和过氧化氢的化学及电化学还原：内界 外界机理

Ru(edta) complexes as molecular redox catalysts in chemical and electrochemical reduction of dioxygen and hydrogen peroxide: inner-sphere outer-sphere mechanism.

作者信息

Chatterjee Debabrata, Chrzanowska Marta, Katafias Anna, Oszajca Maria, van Eldik Rudi

机构信息

Vice-Chancellor's Research Group at Zoology Department, University of Burdwan Burdwan-713104 India

Faculty of Chemistry, Nicolaus Copernicus University in Toruń Gagarina 7 87-100 Toruń Poland

出版信息

RSC Adv. 2021 Jun 16;11(35):21359-21366. doi: 10.1039/d1ra03293c. eCollection 2021 Jun 15.

DOI:10.1039/d1ra03293c
PMID:35478799
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9034107/
Abstract

The reduction of molecular oxygen (O) and hydrogen peroxide (HO) by [Ru(edta)(pz)] (edta = ethylenediaminetetraacetate; pz = pyrazine) has been studied spectrophotometrically and kinetically in aqueous solution. Exposure of the aqua-analogue [Ru(edta)(HO)] to O and HO resulted in the formation of [Ru(edta)(HO)] species, with subsequent formation of the corresponding Ru[double bond, length as m-dash]O complex. A working mechanism for the O and HO reduction reactions mediated by the Ru(edta) complexes is proposed. The role of the coordinated water molecule (by its absence or presence in the primary coordination sphere) in controlling the mechanistic pathways, outer-sphere or inner-sphere, is discussed.

摘要

已通过分光光度法和动力学方法在水溶液中研究了[Ru(乙二胺四乙酸)(吡嗪)]（乙二胺四乙酸 = 乙二胺四乙酸；吡嗪 = 吡嗪）对分子氧（O）和过氧化氢（HO）的还原作用。水合类似物[Ru(乙二胺四乙酸)(HO)]暴露于O和HO会导致形成[Ru(乙二胺四乙酸)(HO)]物种，随后形成相应的Ru=O络合物。提出了由Ru(乙二胺四乙酸)络合物介导的O和HO还原反应的作用机制。讨论了配位水分子（通过其在一级配位球中的存在或不存在）在控制外层球或内层球的作用机制途径中的作用。

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