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Issue 27, 2018
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First-principles calculations of oxidation potentials of electrolytes in lithium–sulfur batteries and their variations with changes in environment

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Abstract

Oxidation potentials of electrolyte molecules in Li–sulfur (Li/S) batteries and their variations in various solvent environments are investigated using first-principles calculations in order to understand oxidative decomposition reactions of electrolytes for cathode passivation. Electrolyte solvents, Li salts, and various additives in Li/S batteries along with some Li-ion battery additives are studied. Oxidation potentials of isolated electrolyte molecules are found to be out of the operating range of typical Li/S batteries. The complexation of electrolyte molecules with Li+, salt anion, salt, S8, and pyrene alters oxidation potentials compared to those of the isolated systems. The salt anion lowers oxidation potentials of electrolyte molecules by at least 4.7% while the complexes with Li+ have higher oxidation potentials than the isolated molecules by at least 10.4%. S8 and pyrene, used as model compounds for sulfur and sulfur/carbon composite cathode materials, also affect oxidation potentials of electrolyte molecules, but their influence is negligible and the oxidation trends differ from those of the Li+ and salt anion. Although complexations change the oxidation potentials of electrolyte molecules, they are still higher than the operating voltage range of Li/S batteries, which indicates that oxidation of the studied electrolytes in Li/S batteries is not expected under ambient conditions.

Graphical abstract: First-principles calculations of oxidation potentials of electrolytes in lithium–sulfur batteries and their variations with changes in environment

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Publication details

The article was received on 08 May 2018, accepted on 25 Jun 2018 and first published on 27 Jun 2018


Article type: Paper
DOI: 10.1039/C8CP02912A
Citation: Phys. Chem. Chem. Phys., 2018,20, 18811-18827
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    First-principles calculations of oxidation potentials of electrolytes in lithium–sulfur batteries and their variations with changes in environment

    J. Han and P. B. Balbuena, Phys. Chem. Chem. Phys., 2018, 20, 18811
    DOI: 10.1039/C8CP02912A

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