Understanding reaction mechanisms using dynamic electrochemical impedance spectroscopy: Methanol oxidation on Pt

被引:13
作者
Holm, Thomas [1 ,3 ]
Sunde, Svein [2 ]
Seland, Frode [2 ]
Harrington, David A. [1 ]
机构
[1] Univ Victoria, Dept Chem, Victoria, BC V8W 2Y2, Canada
[2] Norwegian Univ Sci & Technol NTNU, Dept Mat Sci & Engn, NO-7491 Trondheim, Norway
[3] Univ British Columbia, CERC, Vancouver, BC V6T 1Z4, Canada
基金
加拿大自然科学与工程研究理事会;
关键词
Dynamic electrochemical impedance spectroscopy; Methanol oxidation; Temperature; Reaction mechanism; IN-SITU; TAFEL KINETICS; FORMIC-ACID; ELECTROOXIDATION; ELECTRODE; CO; VOLTAMMETRY; SYSTEMS;
D O I
10.1016/j.electacta.2019.134764
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
Data from a combined cyclic voltammetry and dynamic electrochemical impedance spectroscopy (dEIS) study of the methanol oxidation reaction (MOR) at high temperatures was revisited using a new method for mechanistic modeling. Through iterative optimization of kinetic parameters, a total of five reaction mechanisms of the indirect pathway of the MOR were modeled. The calculated dEIS spectra from the kinetic parameters were used to verify the reaction mechanisms and best fits were found where i) water adsorption is reversible and hinders the MOR at lower potentials (< 0.50 V vs RHE), and ii) the surface reaction between adsorbed CO and OH is chemical. (C) 2019 Elsevier Ltd. All rights reserved.
引用
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页数:8
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