NaOH溶液中Ni基石墨修饰电极上甲醇电氧化过程中钴与铜的协同效应

doi:10.1016/S1872-2067(15)60959-7

催化学报 ›› 2015, Vol. 36 ›› Issue (11): 1867-1874.DOI: 10.1016/S1872-2067(15)60959-7

NaOH溶液中Ni基石墨修饰电极上甲醇电氧化过程中钴与铜的协同效应

Tayebe Rostami^a, Majid Jafarian^a, Somaieh Miandari^a, Mohammad G. Mahjani^a, Fereydoon Gobal^b

a K.N.图什理工大学化学系，德黑兰, 伊朗;
b 谢里夫理工大学化学系, 德黑兰, 伊朗

收稿日期:2015-05-25 修回日期:2015-07-30 出版日期:2015-11-02 发布日期:2015-11-02
通讯作者: Majid Jafarian. 电话: +98-21-22853551; 传真: +98-21-2285 3650; 电子信箱: mjafarian@kntu.ac.ir

Synergistic effect of cobalt and copper on a nickel-based modified graphite electrode during methanol electro-oxidation in NaOH solution

Tayebe Rostami^a, Majid Jafarian^a, Somaieh Miandari^a, Mohammad G. Mahjani^a, Fereydoon Gobal^b

a Department of Chemistry, K. N. Toosi University of Technology, Tehran, Iran;
b Department of Chemistry, Sharif University of Technology, Tehran, Iran

Received:2015-05-25 Revised:2015-07-30 Online:2015-11-02 Published:2015-11-02

摘要/Abstract

摘要：

在NaOH溶液(0.1 mol/L)中考察了Ni, Co和Cu二元和三元合金修饰的石墨电极上甲醇电氧化反应性能. 采用循环伏安法、计时电流法和电化学阻抗谱(EIS)等技术研究了修饰电极的催化活性和协同效应. 这些催化剂在含有Ni, Cu 和Co离子溶液的阴极电位上反复浸渍石墨电极制得. 结果表明, 在甲醇存在下, Ni基三元合金修饰电极(G/NiCuCo)对甲醇氧化反应的响应值明显高于其它样品. 阳极峰值电流与扫描速率的平方根呈线性关系, 表明该过程受扩散控制. 在CA区域, 该反应遵循Cottrellin特性, 甲醇扩散系数为6.25×10^-6 cm²/s. 甲醇氧化反应速率常数为40×10⁷ cm³/(mol·s). 另外, 采用EIS研究了修饰电极表面上甲醇催化氧化反应.

关键词: 甲醇电氧化, 电催化, 协同效应, 镍, 修饰电极

Abstract:

The electrocatalytic oxidation of methanol was studied over Ni, Co and Cu binary or ternary alloys on graphite electrodes in a NaOH solution (0.1 mol/L). The catalysts were prepared by cycling the graphite electrode in solutions containing Ni, Cu and Co ions at cathodic potentials. The synergistic effects and catalytic activity of the modified electrodes were investigated by cyclic voltammetry (CV), chronoamperometry (CA) and electrochemical impedance spectroscopy (EIS). It was found that, in the presence of methanol, the modified Ni-based ternary alloy electrode (G/NiCuCo) exhibited a significantly higher response for methanol oxidation compared to the other samples. The anodic peak currents showed a linear dependency on the square root of the scan rate, which is a characteristic of a diffusion controlled process. During CA studies, the reaction exhibited Cottrellin behavior and the diffusion coefficient of methanol was determined to be 6.25×10^-6 cm²/s and the catalytic rate constant, K, for methanol oxidation was found to be 40×10⁷ cm³/(mol·s). EIS was used to investigate the catalytic oxidation of methanol on the surface of the modified electrode.

Key words: Methanol electro-oxidation, Electrocatalysis, Synergistic effect, Nickel, Modified electrode

Tayebe Rostami, Majid Jafarian, Somaieh Miandari, Mohammad G. Mahjani, Fereydoon Gobal. NaOH溶液中Ni基石墨修饰电极上甲醇电氧化过程中钴与铜的协同效应[J]. 催化学报, 2015, 36(11): 1867-1874.

Tayebe Rostami, Majid Jafarian, Somaieh Miandari, Mohammad G. Mahjani, Fereydoon Gobal. Synergistic effect of cobalt and copper on a nickel-based modified graphite electrode during methanol electro-oxidation in NaOH solution[J]. Chinese Journal of Catalysis, 2015, 36(11): 1867-1874.

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NaOH溶液中Ni基石墨修饰电极上甲醇电氧化过程中钴与铜的协同效应

Synergistic effect of cobalt and copper on a nickel-based modified graphite electrode during methanol electro-oxidation in NaOH solution

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