First-Principles Computational and Experimental Investigation of Molten-Salt Electrolytes: Implications for Li–O2 Battery
Date Published |
02/2021
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Publication Type | Journal Article
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Authors | |
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DOI |
10.1021/acs.jpcc.0c09755
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Abstract |
Nitrate-based molten salts have been the most stable electrolytes in Li–O2 electrochemical systems. While the high temperature of operation is a disadvantage, the molten-salt electrolytes offer a compelling inorganic alternative to both organic electrolytes and inorganic solid electrolytes. In this article, we explore the electrochemical and transport properties of the eutectic binary mixture, Li–K/NO3, using ab initio simulations and compare against experimental studies. Our analysis of the eutectic mixture shows that the Li+ ions are the most mobile species while K+ and NO3– ions have lower, comparable mobilities. The high mobility of the Li+ ion is found to result from its small atomic radius, which allows more transport through “hopping” between solvation shells than larger ions such as K+. Furthermore, ab initio computations of band gaps show much larger stability windows than observed in experiments. Electrochemical stability analysis, performed for the first time using grand-potential analysis on liquid electrolytes, shows that the electrochemical window of the nitrate mixture is restricted by the interface reactions with the electrodes. |
Journal |
The Journal of Physical Chemistry C
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Volume |
125
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Year of Publication |
2021
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Issue |
7
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Pagination |
3698 - 3705
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ISSN Number |
1932-7447
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URL | |
Short Title |
J. Phys. Chem. C
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Refereed Designation |
Refereed
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Organizations | |
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