Entropy production and energy dissipation in symmetric redox supercapacitors

Entropy production and energy dissipation in symmetric redox supercapacitors In this work we propose a theoretical model that accounts for the main features of the loading-unloading process of a symmetric redox MnO2-based supercapacitor dominated by fast electrochemical reactions at the electrodes. The model is formulated on the basis of nonequilibrium thermodynamics from which we are able to deduce generalized expressions for the electrochemical affinity, the load-voltage and the current-voltage equations that constitute generalizations of the current-overpotential and Butler-Volmer equations, and that are used to describe experimental voltagram data with good agreement. These equations allowed us to derive the behavior of the energy dissipated per cycle showing that it has a nonmonotonic behavior and that in the operation regime it follows a power-law behavior as a function of the frequency. The existence of a maximum for the energy dissipated as a function of the frequency suggests the that the corresponding optimal operation frequency should be similar in value to ωmax. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Physical Review E American Physical Society (APS)

Entropy production and energy dissipation in symmetric redox supercapacitors

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Entropy production and energy dissipation in symmetric redox supercapacitors

Abstract

In this work we propose a theoretical model that accounts for the main features of the loading-unloading process of a symmetric redox MnO2-based supercapacitor dominated by fast electrochemical reactions at the electrodes. The model is formulated on the basis of nonequilibrium thermodynamics from which we are able to deduce generalized expressions for the electrochemical affinity, the load-voltage and the current-voltage equations that constitute generalizations of the current-overpotential and Butler-Volmer equations, and that are used to describe experimental voltagram data with good agreement. These equations allowed us to derive the behavior of the energy dissipated per cycle showing that it has a nonmonotonic behavior and that in the operation regime it follows a power-law behavior as a function of the frequency. The existence of a maximum for the energy dissipated as a function of the frequency suggests the that the corresponding optimal operation frequency should be similar in value to ωmax.
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Publisher
American Physical Society (APS)
Copyright
Copyright © ©2017 American Physical Society
ISSN
1539-3755
eISSN
550-2376
D.O.I.
10.1103/PhysRevE.96.022103
Publisher site
See Article on Publisher Site

Abstract

In this work we propose a theoretical model that accounts for the main features of the loading-unloading process of a symmetric redox MnO2-based supercapacitor dominated by fast electrochemical reactions at the electrodes. The model is formulated on the basis of nonequilibrium thermodynamics from which we are able to deduce generalized expressions for the electrochemical affinity, the load-voltage and the current-voltage equations that constitute generalizations of the current-overpotential and Butler-Volmer equations, and that are used to describe experimental voltagram data with good agreement. These equations allowed us to derive the behavior of the energy dissipated per cycle showing that it has a nonmonotonic behavior and that in the operation regime it follows a power-law behavior as a function of the frequency. The existence of a maximum for the energy dissipated as a function of the frequency suggests the that the corresponding optimal operation frequency should be similar in value to ωmax.

Journal

Physical Review EAmerican Physical Society (APS)

Published: Aug 2, 2017

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