Further Investigation of a Nickel-Based Homogeneous Water Oxidation Catalyst with Two cis Labile Sites

ChemSusChem
Gang-Yi LuoTong-Bu Lu

Abstract

The reaction of N,N'-dimethyl-N,N'-bis(pyridin-2-ylmethyl)-1,2-diaminoethane ligand (L) with Ni(ClO4)2 ⋅6 H2O generated a complex of [NiL(H2O)2](ClO4)2 (1) with two cis labile sites occupied by two coordinated H2O molecules, which can homogeneously electrocatalyze water oxidation in pH 6.5 acetate (OAc(-)) buffer at room temperature. The catalytic mechanism was studied by electrochemical experiments and density functional theory calculations to elucidate the following steps: (a) one of two water molecules in 1 is exchanged by OAc(-) to generate [NiL(H2O)(OAc)](+) when dissolved in OAc(-) buffer, (b) Ni(II) is directly oxidized to Ni(IV) and OAc(-) is replaced with OH(-) to form [Ni(IV) L(OH)2 ](2+), and (c) a peroxide intermediate is formed through the intramolecular O-O coupling in the presence of OAc(-), which undergoes further oxidation to release O2.

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Citations

Aug 7, 2017·Chemical Communications : Chem Comm·Hai-Hua HuangTong-Bu Lu
Mar 22, 2019·Chemical Society Reviews·Biaobiao Zhang, Licheng Sun
May 10, 2019·Chemical Communications : Chem Comm·Lu-Hua ZhangHenan Li
Jan 11, 2020·Acta Crystallographica. Section C, Structural Chemistry·Diego da S PadilhaMarciela Scarpellini
Dec 13, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Hadi FeiziMohammad Mahdi Najafpour
Jul 12, 2017·Chemistry, an Asian Journal·Wei SuFrancis Verpoort
Aug 2, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Burg ArielaMeyerstein Dan
May 12, 2019·ChemSusChem·Qiaoqiao Zhang, Jingqi Guan
Feb 6, 2021·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Jinmiao WangMei Wang
May 13, 2021·Chemical Society Reviews·Mio KondoShigeyuki Masaoka
May 22, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Sethuraman MuthuramalingamRamasamy Mayilmurugan
Nov 4, 2017·Inorganic Chemistry·Dong Wang, Charlie O Bruner
Sep 20, 2019·Inorganic Chemistry·Sethuraman MuthuramalingamRamasamy Mayilmurugan
Dec 10, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Amirreza ValizadehMohammad Mahdi Najafpour

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