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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Self-assembled monolayer formation of a (N-5)Fe(II) complex on gold electrodes: electrochemical properties and coordination chemistry on a surface
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Self-assembled monolayer formation of a (N-5)Fe(II) complex on gold electrodes: electrochemical properties and coordination chemistry on a surface

机译:金电极上(N-5)Fe(II)配合物的自组装单层形成:表面的电化学性质和配位化学

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摘要

A coordinatively unsaturated Fell complex bearing a pentadentate ligand (N,N',N'-tris(2-pyridyl-methyl)1,2-diaminoethane) functionalized with a cyclic disulfide group has been prepared in order to graft reactive metal entities as self-assembled monolayers (SAMs) on gold electrodes. Prior to grafting, exogenous ligand exchange has been investigated by cyclic voltammetry (CV) in solution, showing that the nature of the first coordination sphere (N-5)Fe-II-X (X = Cl-, OTf-, MeCN, acetone) can be tuned, thanks to the control of the chemical conditions. The Fe-II complex has been immobilized on gold electrodes by spontaneous (passive) adsorption as well as by an electro-assisted method. The resulting SAMs were characterised by XPS and AFM analyses. CV experiments implementing these SAMs as working electrodes showed that the first coordination sphere of the grafted Fe-II complex can be controlled by adjusting the chemical conditions, similarly to the studies in a homogeneous solution. Finally, the supported Fell complex proved to be reactive with superoxide generated at the electrode surface by reduction of dissolved dioxygen. Under the employed conditions, leaking of the metal complex was not observed.
机译:制备了带有五环配体的五齿配体(N,N',N'-三(2-吡啶基甲基)1,2-二氨基乙烷)的配位不饱和Fell络合物,以便将活性金属实体作为自身接枝电极上组装的单层膜(SAMs)。接枝之前,已通过溶液中的循环伏安法(CV)研究了外源性配体交换,结果表明第一配位球(N-5)Fe-II-X(X = Cl-,OTf-,MeCN,丙酮)的性质得益于化学条件的控制,可以对其进行调整。 Fe-II络合物已经通过自发(被动)吸附以及通过电辅助方法固定在金电极上。通过XPS和AFM分析对所得的SAM进行表征。使用这些SAM作为工作电极的CV实验表明,与均相溶液中的研究相似,可以通过调节化学条件来控制接枝的Fe-II配合物的第一个配位球。最后,事实证明,负载的Fell络合物可通过还原溶解的双氧与电极表面产生的超氧化物发生反应。在使用条件下,未观察到金属络合物的泄漏。

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