The effect of temperature on the coupled slow and fast dynamics of an electrochemical oscillator

Zülke, Alana A. and Varela, Hamilton (2016) The effect of temperature on the coupled slow and fast dynamics of an electrochemical oscillator. Scientific Reports, 6. ISSN 2045-2322

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Abstract

The coupling among disparate time-scales is ubiquitous in many chemical and biological systems. We have recently investigated the effect of fast and, long-term, slow dynamics in surface processes underlying some electrocatalytic reactions. Herein we report on the effect of temperature on the coupled slow and fast dynamics of a model system, namely the electro-oxidation of formic acid on platinum studied at five temperatures between 5 and 45 °C. The main result was a turning point found at 25 °C, which clearly defines two regions for the temperature dependency on the overall kinetics. In addition, the long-term evolution allowed us to compare reaction steps related to fast and slow evolutions. Results were discussed in terms of the key role of PtO species, which chemically couple slow and fast dynamics. In summary we were able to: (a) identify the competition between two reaction steps as responsible for the occurrence of two temperature domains; (b) compare the relative activation energies of these two steps; and (c) suggest the role of a given reaction step on the period-increasing set of reactions involved in the oscillatory dynamics. The introduced methodology could be applied to other systems to uncover the temperature dependence of complex chemical networks.

Item Type:
Journal Article
Journal or Publication Title:
Scientific Reports
Uncontrolled Keywords:
/dk/atira/pure/subjectarea/asjc/1000
Subjects:
ID Code:
136940
Deposited By:
Deposited On:
24 Sep 2019 14:15
Refereed?:
Yes
Published?:
Published
Last Modified:
10 Sep 2020 05:19