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Mechanistic Study of Electrocatalytic Oxidation of Formic Acid at Platinum in Acidic Solution by Time-Resolved Surface-Enhanced Infrared Absorption Spectroscopy
Abstract
Surface-enhanced infrared absorption spectroscopy (SEIRAS) combined with cyclic voltammetry or chronoamperometry has been utilized to examine kinetic and mechanistic aspects of the electrocatalytic oxidation of formic acid on a polycrystalline Pt surface at the molecular scale. Formate is adsorbed on the electrode in a bridge configuration in parallel to the adsorption of linear and bridge CO produced by dehydration of formic acid. A solution-exchange experiment using isotope-labeled formic acids (H(12)COOH and H(13)COOH) reveals that formic acid is oxidized to CO(2) via adsorbed formate and the decomposition (oxidation) of formate to CO(2) is the rate-determining step of the reaction. The adsorption/oxidation of CO and the oxidation/reduction of the electrode surface strongly affect the formic acid oxidation by blocking active sites for formate adsorption and also by retarding the decomposition of adsorbed formate. The interplay of the involved processes also affects the kinetics and complicates the cyclic voltammograms of formic acid oxidation. The complex voltammetric behavior is comprehensively explained at the molecular scale by taking all these effects into account.
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Citations
Cited by
Thermodynamic theory of multi-electron transfer reactions: Implications for electrocatalysis
Koper, M. T. M. (2011) · Journal of Electroanalytical Chemistry · doi:10.1016/j.jelechem.2010.10.004 · Cited by 1,204
Neurock, M., Janik, M., & Wieckowski, A. (2009) · Faraday Discuss. · doi:10.1039/b804591g · Cited by 444
Osawa, M., Tsushima, M., Mogami, H., Samjeské, G., & Yamakata, A. (2008) · The Journal of Physical Chemistry C · doi:10.1021/jp710386g · Cited by 324
Self-citationChen, L., Guo, H., Fujita, T., Hirata, A., Zhang, W., Inoue, A., & Chen, M. (2011) · Advanced Functional Materials · doi:10.1002/adfm.201101227 · Cited by 270
Importance of Acid–Base Equilibrium in Electrocatalytic Oxidation of Formic Acid on Platinum
Joo, J., Uchida, T., Cuesta, A., Koper, M. T. M., & Osawa, M. (2013) · Journal of the American Chemical Society · doi:10.1021/ja403578s · Cited by 269
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Metadata
- Authors
- Samjeské, G., Miki, A., Ye, S., & Osawa, M.
- Venue
- The Journal of Physical Chemistry B
- Publisher
- American Chemical Society (ACS)
- Published
- 2006-07-28
- Volume
- 110
- Issue
- 33
- Pages
- 16559-16566
- ISSN
- 1520-5207 (ISSN-L)
- 1520-6106
- OpenAlex
- W2089020487
- Cited by
- 269
- References
- 0
- FWCI
- 9.21
- Type
- journal article
- Language
- en
- Open access
- closed
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- Samjeské, G., Miki, A., Ye, S., & Osawa, M. (2006). Mechanistic Study of Electrocatalytic Oxidation of Formic Acid at Platinum in Acidic Solution by Time-Resolved Surface-Enhanced Infrared Absorption Spectroscopy. The Journal of Physical Chemistry B. https://doi.org/10.1021/jp061891l
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