Ab initio calculations of the atomic and electronic structures of crystalline PEO3:LiCF3SO3 electrolytes

TL;DR

This paper uses ab initio density functional theory to investigate the atomic and electronic structures of crystalline PEO3:LiCF3SO3 electrolytes, providing insights into their bonding, electronic properties, and conductivity.

Contribution

It presents the first ab initio calculations of crystalline PEO3:LiCF3SO3, complementing previous studies on amorphous phases and aligning well with experimental data.

Findings

Bonding configurations match experimental observations

Electronic structures are consistent with conductivity measurements

Crystalline phase properties differ from amorphous phase insights

Abstract

The PEO3:LiCF3SO3 polymer electrolyte has attracted significant research due to its enhanced stability at the lithium/polymer interface of high conductivity polymer batteries. Experimental studies have shown that, depending on the preparation conditions, both the PEO3:LiCF3SO3 crystalline complex and the PEO3:LiCF3SO3 amorphous phase can be formed. However, previous theoretical investigations focused on the short chain amorphous PEO3:LiCF3SO3 system. We report ab initio density-functional-theory calculations of crystalline PEO3:LiCF3SO3. The calculated results about the bonding configuration, electronic structures, and conductivity properties are in good agreement with the experimental measurements.