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On the stochastic thermodynamics of mesoscopic electrochemical reactions
Tiejun Xiao
作者单位E-mail
Tiejun Xiao Guizhou Provincial Key Laboratory of Computational Nano-Material Science, Guizhou Synergetic Innovation Center of Scienti c Big Data for Advanced Manufacturing Technology, Guizhou Education University, Guiyang, Guizhou 550018 P. R. China tjxiao3@mail.ustc.edu.cn 
摘要:
In this paper, we discussed the stochastic thermodynamics of mesoscopic electron transfer reactions between ions and electrodes. With a relationship between the reaction rate constant and the electrode potential, we find that the heat dissipation q equals to the dynamic irreversibility of the reaction system minus an internal entropy change term. The total entropy change Δst is defined as the summation of the system entropy change Δs and the heat dissipation q such that Δst = Δs q. Even though the heat dissipation depends linearly on the electrode potential, the total entropy change is found to satisfy the fluctuation theorem ?e??Δst ? = 1, and hence a second law-like inequality reads ?Δst? ≥ 0. Our study provides a practical methodology for the stochastic thermodynamics of electrochemical reactions, which may find applications in biochemical and electrochemical reaction systems.
关键词:  Mesoscopic chemical reaction, Electron transfer, Electrode potential, Entropy production , Fluctuation theorem
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On the stochastic thermodynamics of mesoscopic electrochemical reactions
Tiejun Xiao
Abstract:
In this paper, we discussed the stochastic thermodynamics of mesoscopic electron transfer reactions between ions and electrodes. With a relationship between the reaction rate constant and the electrode potential, we find that the heat dissipation q equals to the dynamic irreversibility of the reaction system minus an internal entropy change term. The total entropy change Δst is defined as the summation of the system entropy change Δs and the heat dissipation q such that Δst = Δs q. Even though the heat dissipation depends linearly on the electrode potential, the total entropy change is found to satisfy the fluctuation theorem ?e??Δst ? = 1, and hence a second law-like inequality reads ?Δst? ≥ 0. Our study provides a practical methodology for the stochastic thermodynamics of electrochemical reactions, which may find applications in biochemical and electrochemical reaction systems.
Key words:  Mesoscopic chemical reaction, Electron transfer, Electrode potential, Entropy production , Fluctuation theorem