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首页> 外文期刊>Journal of Applied Electrochemistry >Nickel-dimethylglyoxime complex modified graphite and carbon paste electrodes: preparation and catalytic activity towards methanol/ethanol oxidation
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Nickel-dimethylglyoxime complex modified graphite and carbon paste electrodes: preparation and catalytic activity towards methanol/ethanol oxidation

机译:镍-二甲基乙二肟复合物修饰的石墨和碳糊电极:制备及其对甲醇/乙醇氧化的催化活性

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Nickel-dimethylglyoxime complex (abbreviated as Ni(II)(DMG)2) modified carbon paste and graphite electrodes were prepared by mixing Ni(II)(DMG)2 with graphite paste, and coating Ni(II)(DMG)2 to the graphite surface. It is necessary to cycle the electrode potential to a high value (e.g. 0.8 V versus SCE) for the preparation of the modified electrodes. The electrochemical reaction was originally assumed to be a one-electron process converting Ni(II)(DMG)2 to [(DMG)2(H2O)Ni(III)ONi(III)(OH)(DMG)2]−. [(DMG)2(H2O)Ni(III)ONi(III)(OH)(DMG)2]− showed a strong catalytic activity toward electro-oxidation of methanol and ethanol. The electrocatalytic oxidation currents consistently increase with the increase in Ni(II)(DMG)2 loading, OH−, and alcohol concentrations. Rotating disk electrode results obtained with a Ni(II)(DMG)2 coated graphite disk electrode showed that the electrocatalytic oxidation of alcohol is a 4-electron process producing formate anion (methanol oxidation) or acetate anion (ethanol oxidation). A mechanism for the electrocatalytic oxidation of methanol/ethanol was proposed, and a rate-determining step was also discussed.
机译:通过将Ni(II)(DMG) 2 与石墨混合制备镍-二甲基乙二肟配合物(缩写为Ni(II)(DMG) 2 )和石墨电极糊剂,然后将Ni(II)(DMG) 2 涂覆到石墨表面。为了制备改性电极,必须将电极电势循环到高值(例如0.8V相对于SCE)。最初,电化学反应是将Ni(II)(DMG) 2 转换为[(DMG) 2 (H 2 O)Ni(III)ONi(III)(OH)(DMG) 2 ] -。 [(DMG) 2 (H 2 O)Ni(III)ONi(III)(OH)(DMG) 2 ] -对甲醇和乙醇的电氧化具有很强的催化活性。随着Ni(II)(DMG) 2 负载,OH -和酒精浓度的增加,电催化氧化电流持续增加。用涂有Ni(II)(DMG) 2 的石墨圆盘电极获得的转盘电极结果表明,醇的电催化氧化是产生甲酸根阴离子(甲醇氧化)或乙酸根阴离子的4电子过程(乙醇氧化)。提出了甲醇/乙醇电催化氧化的机理,并讨论了速率确定步骤。

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