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Kinetic differentiation of bulk/interfacial oxygen reduction mechanisms at/near liquid/liquid interfaces using scanning electrochemical microscopy
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Deng, Haiqiang, Peljo, Pekka, Momotenko, Dmitry, Cortés-Salazar, Fernando, Jane Stockmann, T., Kontturi, Kyösti, Opallo, Marcin and Girault, Hubert H. (2014) Kinetic differentiation of bulk/interfacial oxygen reduction mechanisms at/near liquid/liquid interfaces using scanning electrochemical microscopy. Journal of Electroanalytical Chemistry, Volume 732 . pp. 101-109. doi:10.1016/j.jelechem.2014.08.031 ISSN 1572-6657.
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Official URL: http://dx.doi.org/10.1016/j.jelechem.2014.08.031
Abstract
The present work describes the application of scanning electrochemical microscopy (SECM) in the feedback
mode to determine the kinetics of oxygen reduction at or near the liquid/liquid interface – between
water and 1,2-dichloroethane (w/DCE). The system contained decamethylferrocene (DMFc) in DCE as the
electron donor and acids in water as a proton source. In this approach, decamethylferrocenium (DMFc+
) is
reduced at the tip of a microelectrode in DCE and the electrogenerated DMFc reacts with protons and
oxygen to be re-oxidized in a following chemical reaction (catalytic EC’ mechanism). When a high Galvani
potential difference was applied across the liquid/liquid interface, protons would transfer rapidly to the
organic phase. Under this condition, SECM approach curves toward the liquid/liquid interface showed
dramatic current increases at distances far from the interface. This indicates that oxygen reduction takes
place mainly in the bulk DCE; however, at lower Galvani potential differences, where the proton transfer
is slow, oxygen reduction was also observed at the interface. Finally, SECM feedback mode measurements
with the tip approaching a conductive substrate were used to determine the kinetics of the homogeneous
reaction, with an obtained apparent rate constant of 0.2–0.5 m3 mol1 s1
.
Item Type: | Journal Article | ||||||||||
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||||||
Journal or Publication Title: | Journal of Electroanalytical Chemistry | ||||||||||
Publisher: | Elsevier Science SA | ||||||||||
ISSN: | 1572-6657 | ||||||||||
Official Date: | 15 October 2014 | ||||||||||
Dates: |
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Volume: | Volume 732 | ||||||||||
Page Range: | pp. 101-109 | ||||||||||
DOI: | 10.1016/j.jelechem.2014.08.031 | ||||||||||
Status: | Peer Reviewed | ||||||||||
Publication Status: | Published | ||||||||||
Access rights to Published version: | Restricted or Subscription Access | ||||||||||
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