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首页> 外文期刊>Transition Metal Chemistry >Synthesis, characterization, crystal structure, electrochemical properties and electrocatalytic activity of an unexpected nickel(II) Schiff base complex derived from bis(acetylacetonato)nickel(II), acetone and ethylenediamineDDepartment of Chemistry, Faculty of Science, University of Peradeniya, Peradeniya, Sri LankaMmyug@pdn.ac.lk; mdechem@yahoo.com
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Synthesis, characterization, crystal structure, electrochemical properties and electrocatalytic activity of an unexpected nickel(II) Schiff base complex derived from bis(acetylacetonato)nickel(II), acetone and ethylenediamineDDepartment of Chemistry, Faculty of Science, University of Peradeniya, Peradeniya, Sri LankaMmyug@pdn.ac.lk; mdechem@yahoo.com

机译：双（乙酰丙酮基）镍（II），丙酮和乙二胺衍生的意料之外的镍（II）Schiff碱配合物的合成，表征，晶体结构，电化学性质和电催化活性D Peradeniya大学理学院化学系，Peradeniya ，斯里兰卡M myug@pdn.ac.lk; mdechem@yahoo.com

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摘要

The synthesis, crystal structure and electrochemical properties of a Ni(II) Schiff base complex, [Ni(L)]PF6 (where L is 2,4,9,11,1 1-pentamethyl-2,3,4 tri-aza-1-one-4-amine) are reported herein. The complex has been characterized by its electrochemical behavior, X-ray crystallographic structural analysis, physio-chemical methods and spectroscopic techniques. Electrospray mass spectroscopic analysis gives a dominant ion peak with ml z = 296 which corresponds to the {[Ni(L)]PF6-HPF6}~+ fragment. Cyclic voltammograms for [Ni(L)]PF6, obtained in DMF (0.1 M Bu4NPF6) at a glassy carbon electrode with a scan rate of 100 mV s~(-1), exhibit reversible ([Ni~(II)(L)]~+/ [Ni~I(L)]) reduction and chemically irreversible ([Ni~(II)(L)]~+/ [Ni~(III)(L)]~(2+) → electroactive product) oxidation processes at -2.05 and 0.62 V, respectively. The diffusion coefficient, calculated using the Randles-Sevcik relationship, is 9.7 x 10~(-6) cm~2 s~(-1). Electrochemical studies reveal that the Ni~I reduced form of the complex is capable of catalyzing CO2 reduction at a potential that is thermodynami-cally more favorable than for the reduced [Ni(N,N'-ethylenebis(acetylacetoneiminato)]complex. Spectroelect-rochemical analyses following bulk electrolysis of [Ni(L)]PF6 under CO2 revealed the formation of oxalate and bicarbonate.
机译：Ni（II）Schiff碱配合物[Ni（L）] PF6（其中L为2,4,9,11,1 1-五甲基-2,3,4三氮杂）的合成，晶体结构和电化学性质-1-一-4-胺）在本文报道。该配合物的特征在于其电化学行为，X射线晶体学结构分析，物理化学方法和光谱技术。电喷雾质谱分析给出了一个主离子峰，m 1 z = 296，与{[Ni（L）] PF6-HPF6}〜+片段相对应。在DMF（0.1 M Bu4NPF6）中在玻璃碳电极上以100 mV s〜（-1）的扫描速率获得的[Ni（L）] PF6的循环伏安图显示可逆的[[Ni〜（II）（L） ]〜+ / [Ni〜I（L）]）还原且化学不可逆（[Ni〜（II）（L）]〜+ / [Ni〜（III）（L）]〜（2+）→电活性产物）氧化过程分别在-2.05和0.62 V下进行。利用Randles-Sevcik关系计算出的扩散系数为9.7×10〜（-6）cm〜2 s〜（-1）。电化学研究表明，该复合物的Ni〜I还原形式能够催化CO2的还原，其电势比还原的[Ni（N，N'-亚乙基双（乙酰丙酮亚氨基））络合物]热动力学更有利。 [Ni（L）] PF6在二氧化碳下大量电解后的化学分析表明，草酸盐和碳酸氢盐形成了。

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