Au单晶电极上H2O2的氧化反应研究

doi:10.13208/j.electrochem.160568

电化学（中英文） ›› 2016, Vol. 22 ›› Issue (6): 602-606. doi: 10.13208/j.electrochem.160568

• 界面电化学近期研究专辑（厦门大学毛秉伟教授） • 上一篇下一篇

Au单晶电极上H₂O₂的氧化反应研究

郑勇力，魏杰，陈艳霞*

中国科技大学化学物理系, 合肥微尺度物质科学国家实验室（筹）, 安徽合肥 230026

收稿日期:2016-07-15 修回日期:2016-09-18 出版日期:2016-12-28 发布日期:2016-09-26
通讯作者: 陈艳霞 E-mail:yachen@ustc.edu.cn
基金资助:
国家自然科学基金项目（No. 21473175），973 计划 (No.2015CB932301)资助

A Study on the Oxidation of Hydrogen peroxide at Au(111) and Au(100) Electrodes

ZHENG Yong-li, WEI Jie, CHEN Yan-xia*

Hefei National Laboratory for Physical Sciences at Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China

Received:2016-07-15 Revised:2016-09-18 Published:2016-12-28 Online:2016-09-26
Contact: CHEN Yan-xia E-mail:yachen@ustc.edu.cn

摘要/Abstract

摘要：

本文利用旋转圆盘电极系统研究了酸性介质中H₂O₂在Au(100)和Au(111)电极表面的电化学行为. 实验发现在Au电极上H₂O₂难以发生还原，但是当电位稍微正于H₂O₂氧化为O₂的平衡电势时即可发生氧化. 在Au(111)上H₂O₂氧化的起始电位比在Au(100)正0.1 V左右. Au(100)上的双桥位位点能增强反应中间体*OOH的吸附，可能是导致Au(100)上H₂O₂氧化反应超电势比Au(111)低的主要原因. 在较正电位区(E>1.2 V), 当电极表面被氧物种覆盖时，H₂O₂在两个电极上的氧化都会受到一定程度的抑制，这种影响在Au(111)上比Au(100)上更加明显，这与Au(111)上氧物种的生成与逆向还原可逆性差的趋势一致. 最后还将Au与Pt单晶电极上H₂O₂氧化的行为进行了对比分析.

关键词: 过氧化氢氧化, Au单晶电极, 旋转圆盘电极

Abstract:

The oxidation reactions of hydrogen peroxide (H₂O₂) at Au(111) and Au(100) electrodes in 0.1 mol·L^-1 HClO₄ were investigated by using rotating disk electrode system. It was found that H₂O₂ could be readily oxidized to O₂ at both Au(100) and Au(111) surfaces with the onset potential close to its equilibrium potential. In contrast, the onset overpotential for H₂O₂ reduction was above 0.4 V, while the onset overpotential for H₂O₂ oxidation at Au(100) was ca. 0.1 V more negative than that at Au(111), this is probably due to special double bridge sites which facilitate the adsorption of OOH* intermediates and its further splitting of the O-H bond. When the electrode potential exceeded 1.2 V, the Au surface was gradually covered by oxides, which significantly inhibit the oxidation reaction of H₂O₂. The inhibition effect became more obvious at Au(111) than that at Au(100), which corresponds well to the worse reversibility for the formation and reduction of Au oxides at Au(111). Finally, the comparisons in the H₂O₂ oxidation behaviors at Au(100) and Au(111) with that at Pt(111) indicated that the onset potential for H₂O₂oxidation at Pt(111) should also be quite close to its equilibrium potential, and the observed high onset anodic current was due to the mixed potential effects of both the oxidation and reduction of H₂O₂ which occurred at the interface simultaneously.

Key words: Hydrogen peroxide Oxidation, Au single crystal electrode, rotating disk electrode

中图分类号:

O646

郑勇力，魏杰，陈艳霞. Au单晶电极上H₂O₂的氧化反应研究[J]. 电化学（中英文）, 2016, 22(6): 602-606.

ZHENG Yong-li, WEI Jie, CHEN Yan-xia. A Study on the Oxidation of Hydrogen peroxide at Au(111) and Au(100) Electrodes[J]. Journal of Electrochemistry, 2016, 22(6): 602-606.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.13208/j.electrochem.160568

https://electrochem.xmu.edu.cn/CN/Y2016/V22/I6/602

参考文献

[1] Li M.F., Liao L.W., Yuan D.F., et al. pH effect on oxygen reduction reaction at Pt(111) electrode[J], Electrochimica Acta, 2013,110: 780-789.

[2] Strbac S., Anastasijevic N.A., Adzic R.R., Oxygen Reduction on Au(100) and Vicinal Au(910) and Au(11, 1, 1) Faces in Alkaline-Solution - A Rotating-Disk Ring Study[J], Journal of Electroanalytical Chemistry, 1992, 323: 179-195.

[3] Adzic R.R., Strbac S., Anastasijevic N., Electrocatalysis of Oxygen on Single-Crystal Gold Electrodes[J], Materials Chemistry and Physics, 1989, 22: 349-375.

[4] Norskov J.K., Rossmeisl J., Logadottir A., et al. Origin of the overpotential for oxygen reduction at a fuel-cell cathode[J], The Journal of Physical Chemistry B, 2004, 108: 17886-17892.

[5] Schmidt T.J., Stamenkovic V., Arenz M., et al. Oxygen electrocatalysis in alkaline electrolyte: Pt(hkl), Au(hkl) and the effect of Pd-modification[J], Electrochimica Acta, 2002, 47: 3765-3776.

[6] Sitta E., Gomez-Marin A.M., Aldaz A., et al. Electrocatalysis of H2O2 reduction/oxidation at model platinum surfaces[J], Electrochemistry Communications, 2013, 33: 39-42.

[7] Sitta E., Feliu J.M., The Role of PtOH on H2O2 Interactions with Platinum Surfaces in an Electrochemical Environment[J], Chemelectrochem, 2014, 1: 55-58.

[8] Katsounaros I., Schneider W.B., Meier J.C., et al. Hydrogen peroxide electrochemistry on platinum: towards understanding the oxygen reduction reaction mechanism[J], Physical Chemistry Chemical Physics, 2012, 14: 7384-7391.

[9] Gomez-Marin A.M., Feliu J.M., New Insights into the Oxygen Reduction Reaction Mechanism on Pt(111): A Detailed Electrochemical Study[J], Chemsuschem, 2013, 6: 1091-1100.

[10] Zheng Y.L., Mei D., Chen Y.X., et al. The redox reaction of hydrogen peroxide at an Au(100) electrode: Implications for oxygen reduction kinetics[J], Electrochemistry Communications, 2014, 39: 19-21.

[11] Clavilier J., Faure R., Guinet G., et al. Preparation of Mono-Crystalline Pt Microelectrodes and Electrochemical Study of the Plane Surfaces Cut in the Direction of the (111) and (110) Planes[J], Journal of Electroanalytical Chemistry, 1980, 107: 205-209.

[12] Mei D., He Z.D., Zheng Y.L., et al. Mechanistic and kinetic implications on the ORR on a Au(100) electrode: pH, temperature and H-D kinetic isotope effects[J], Physical Chemistry Chemical Physics, 2014, 16: 13762-13773.

[13] Prieto A., Hernandez J., Herrero E., et al. The role of anions in oxygen reduction in neutral and basic media on gold single-crystal electrodes[J], Journal of Solid State Electrochemistry, 2003, 7: 599-606.

[14] Li H., Li Y., Koper M.T.M., et al. Bond-Making and Breaking between Carbon, Nitrogen, and Oxygen in Electrocatalysis[J], Journal of the American Chemical Society, 2014, 136: 15694-15701.

[15] B.L. Wu, H.W. Lei, C.S. Cha, et al. Investigation of the Intermediates of the O-2 Reduction Reaction on Au Electrodes in Alkaline-solution[J], Journal of Electroanalytical Chemistry, 1994, 377: 227-230.

Au单晶电极上H₂O₂的氧化反应研究

A Study on the Oxidation of Hydrogen peroxide at Au(111) and Au(100) Electrodes

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