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Stability of Calcium Ion Battery Electrolytes: Predictions from Ab Initio Molecular Dynamics Simulations

submitted on 01.02.2021, 09:40 and posted on 02.02.2021, 10:11 by Sharma Yamijala, Hyuna Kwon, Juchen Guo, Bryan Wong

Multivalent batteries, such as magnesium-ion, calcium-ion, and zinc-ion batteries, have attracted significant attention as next-generation electrochemical energy storage devices to complement conventional lithium-ion batteries (LIBs). Among them, calcium-ion batteries (CIBs) are the least explored due to the difficult reversible Ca deposition-dissolution. In this work, we examined the stability of four different Ca salts with weakly coordinating anions and three different solvents commonly employed in existing battery technologies to identify suitable candidates for CIBs. By employing Born-Oppenheimer molecular dynamics (BOMD) simulations on salt-Ca and solvent-Ca interfaces, we find that the tetraglyme solvent and carborane salt are promising candidates for CIBs. Due to the strong reducing nature of the calcium surface, the other salts and solvents readily decompose. We explain the microscopic mechanisms of salt/solvent decomposition on the Ca surface using time-dependent projected density of states, time-dependent charge-transfer plots, and climbing-image nudged elastic band calculations. Collectively, this work presents the first mechanistic assessment of the dynamical stability of candidate salts and solvents on a Ca surface using BOMD simulations, and provides a predictive path toward designing stable electrolytes for CIBs.


Department of Energy, Office of Science, Award No. DE-SC0016269

National Science Foundation grant No. DMR-2004497


Email Address of Submitting Author


University of California, Riverside


United States

ORCID For Submitting Author


Declaration of Conflict of Interest

no conflict of interest