Superoxide Disproportionation Driven by Zinc Complexes with Various Steric and Electrostatic Properties

Wada, Akira; Jitsukawa, Koichiro; Masuda, Hideki

doi:10.1002/anie.201305459

Cited by 15 publications

(10 citation statements)

References 33 publications

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“…À0.4 V), onset potentials of oxygen reduction were observed to shift positively in the ZnCl 2 solution (À0.16 V) and the precursor solution (À0.30 V). Similar results have been reported previously [21][22][23] and Zn II was demonstrated as aLewis acid to facilitate the reduction of O 2 to O 2 À at more positive potentials and form superoxo-Zn II complex [Eq. (2)].…”

mentioning

confidence: 99%

Oxygen‐Assisted Cathodic Deposition of Zeolitic Imidazolate Frameworks with Controlled Thickness

Zhang

Yuan

et al. 2018

Angew Chem Int Ed

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Processing metal-organic frameworks (MOFs) as films with controllable thickness on asubstrate is increasingly crucial for many applications to realizef unction integration and performance optimization. Herein, we report af acile cathodic deposition process that enables the large-area preparation of uniform films of zeolitic imidazolate frameworks (ZIF-8, ZIF-71, and ZIF-67) with highly tunable thickness ranging from approximately 24 nm to hundreds of nanometers. Importantly,t his oxygen-reduction-triggered cathodic deposition does not lead to the plating of reduced metals (Zn and Co). It is also operable cost-effectively in the absence of supporting electrolyte and facilitates the construction of well-defined submicrometer-sized heterogeneous structures within ZIF films.Metal-organic frameworks (MOFs), ac lass of porous crystalline materials with large surface areas,r egular pore sizes,a nd tailorable surface chemistry, [1] have received considerable attention in av ariety of fields. [2][3][4][5][6][7][8] Form any applications,s uch as separations, [3] energy storage [5] and conversion, [6] chemical sensing, [7] and electronics, [8] it is often necessary to process MOF materials as films on as pecific substrate.A mong methods established for preparing MOF films, [9,10] strategies based on electrochemical synthesis are attractive for many advantages including technological flexibility,scalable preparation, and industrial production potential. [11] Nevertheless,t heir potential for preparing MOF films with precisely tunable morphology and thickness has not been fully explored. These variables,h owever,a re critically important for structure integration and performance optimization in (especially device) applications. [8,9] MOFs could be deposited on the electrode surface anodically [12] or cathodically. [13] In cathodic deposition, reduction of some special molecules or ions (e.g.n itrate ions) on electrode surface results in an increase in pH, which promotes the deprotonation of organic ligands and induces the formation of MOFs.Atfirst glance,cathodic deposition appears to be attractive for the direct synthesis of MOFs on conductive substrates.H owever,r eports on the cathodic deposition of MOFs are comparably few.The challenge arises from the more negative reduction potential of nitrate ions relative to those of some important metal ions,f or example, Zn II ,C o II ,a nd Cu II ,w hich constitute the most extensively studied MOFs. [13b,g] As ar esult, cathodic deposition of these MOF materials is commonly accompanied with plating of the corresponding metals, [13a,e] which is in most cases undesirable.Herein, we report the first cathodic deposition of zeolitic imidazolate framework materials (ZIFs), an important subgroup of MOFs that have been extensively studied owing to their outstanding thermal stability and chemical robustness. [14,15] Our strategy is based on an oxygen reduction triggered-electrochemical-chemical-reaction Scheme responsible for the formation of ZIF materials (Scheme 1). Electrochemical oxyge...

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confidence: 99%

Oxygen‐Assisted Cathodic Deposition of Zeolitic Imidazolate Frameworks with Controlled Thickness

Zhang

Yuan

et al. 2018

Angew Chem Int Ed

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“…−0.4 V), onset potentials of oxygen reduction were observed to shift positively in the ZnCl 2 solution (−0.16 V) and the precursor solution (−0.30 V). Similar results have been reported previously and Zn II was demonstrated as a Lewis acid to facilitate the reduction of O 2 to O 2 − at more positive potentials and form superoxo‐Zn II complex [Eq. ].…”

Section: Methodsmentioning

confidence: 99%

Oxygen‐Assisted Cathodic Deposition of Zeolitic Imidazolate Frameworks with Controlled Thickness

Zhang

Yuan

et al. 2018

Angewandte Chemie

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Processing metal–organic frameworks (MOFs) as films with controllable thickness on a substrate is increasingly crucial for many applications to realize function integration and performance optimization. Herein, we report a facile cathodic deposition process that enables the large‐area preparation of uniform films of zeolitic imidazolate frameworks (ZIF‐8, ZIF‐71, and ZIF‐67) with highly tunable thickness ranging from approximately 24 nm to hundreds of nanometers. Importantly, this oxygen‐reduction‐triggered cathodic deposition does not lead to the plating of reduced metals (Zn and Co). It is also operable cost‐effectively in the absence of supporting electrolyte and facilitates the construction of well‐defined sub‐micrometer‐sized heterogeneous structures within ZIF films.

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“…Therefore, complexes 1 and 2 can be applied as models for superoxide dismutase, because the redox potentials of the two complexes are located in the allowed ranges of SOD mimics. To confirm the formation of superoxo-/peroxo-copper(II) intermediates in the catalytic reaction, we performed a cyclic voltammogram experiment after O 2 2À binding to the complex with the methods of Hideki Masuda and co-workers [5]. As shown in Fig.…”

Section: Cyclic Voltammetrymentioning

confidence: 99%

“…Copper-zinc superoxide dismutase (Cu,Zn-SOD) is an essential enzyme in the natural antioxidant system, which catalyzes the dismutation of superoxide to hydrogen peroxide and the oxygen molecule under physiological conditions [3,4]. A copper-zinc heterobimetallic complex is located at the active site of Cu,Zn-SOD, in which the copper(II) ion is pentacoordinated by four histidine residues and one water molecule with a distorted tetragonal pyramidal coordination environment [5]. Due to the limitations of solution instability, immunogenicity, bell-shaped dose response curves, short half-lives, costs of production and proteolytic digestion, the direct utilization of Cu,Zn-SOD as a pharmaceutical agent still has many problems [6].…”

Section: Introductionmentioning

confidence: 99%

Synthesis, structure and superoxide dismutase-like activity of copper(II) complexes based on N,N′-bis(2-quinolinylmethyl)amantadine

et al. 2015

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Superoxide Disproportionation Driven by Zinc Complexes with Various Steric and Electrostatic Properties

Cited by 15 publications

References 33 publications

Oxygen‐Assisted Cathodic Deposition of Zeolitic Imidazolate Frameworks with Controlled Thickness

Oxygen‐Assisted Cathodic Deposition of Zeolitic Imidazolate Frameworks with Controlled Thickness

Oxygen‐Assisted Cathodic Deposition of Zeolitic Imidazolate Frameworks with Controlled Thickness

Synthesis, structure and superoxide dismutase-like activity of copper(II) complexes based on N,N′-bis(2-quinolinylmethyl)amantadine

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