The morphology of interfaces is known to play a fundamental role in the efficiency of energy-related applications, such as light harvesting or ion intercalation. Altering the morphology on demand, however, is a very difficult task. Here, we show ways the morphology of interfaces can be tuned by driven electron transfer reactions. By using non-equilibrium thermodynamic stability theory, we uncover the operating conditions that alter the interfacial morphology. We apply the theory to ion intercalation and surface growth where electrochemical reactions are described using Butler–Volmer or coupled ion–electron transfer kinetics. The latter connects microscopic/quantum mechanical concepts with the morphology of electrochemical interfaces. Finally, we construct non-equilibrium phase diagrams in terms of the applied driving force (current/voltage) and discuss the importance of engineering the density of states of the electron donor in applications related to energy harvesting and storage, electrocatalysis, and photocatalysis.
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14 May 2020
Research Article|
May 08 2020
Tuning the stability of electrochemical interfaces by electron transfer reactions
Special Collection:
Interfacial Structure and Dynamics for Electrochemical Energy Storage
Dimitrios Fraggedakis
;
Dimitrios Fraggedakis
a)
1
Department of Chemical Engineering, Massachusetts Institute of Technology
, Cambridge, Massachusetts 02139, USA
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Martin Z. Bazant
Martin Z. Bazant
b)
2
Departments of Chemical Engineering and Mathematics, Massachusetts Institute of Technology
, Cambridge, Massachusetts 02139, USA
b)Author to whom correspondence should be addressed: bazant@mit.edu
Search for other works by this author on:
a)
Email: dimfraged@gmail.com
b)Author to whom correspondence should be addressed: bazant@mit.edu
Note: This paper is part of the JCP Special Topic on Interfacial Structure and Dynamics for Electrochemical Energy Storage.
J. Chem. Phys. 152, 184703 (2020)
Article history
Received:
March 06 2020
Accepted:
April 20 2020
Citation
Dimitrios Fraggedakis, Martin Z. Bazant; Tuning the stability of electrochemical interfaces by electron transfer reactions. J. Chem. Phys. 14 May 2020; 152 (18): 184703. https://doi.org/10.1063/5.0006833
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