Solid polymer electrolytes (SPEs), with the potential to resolve safety issues of traditional liquid electrolytes and be compatible with the high-voltage cathode, have been attracting attention from global researchers. Due to the limited Li+ transference number, crystallinity at room temperature, and instability towards oxidation, polyether-based SPEs have been excluded from the application in state-of-the-art batteries with the high-voltage cathode and Li-metal anode. Low ionic conductivity remains one of the biggest challenges for other types of SPEs and the reliance on trial-and-error approach in experimental study render the search of high-conductivity SPEs inefficient. Furthermore, the understanding of Li+ transport mechanisms and the related correlations with polymer structure is limited. Molecular dynamics (MD) simulations provide a quick access to physical insights of Li+ transport mechanisms and possibility to establish correlations between details of polymer chain architecture and Li+ mobility. In this study, we focus on comb-branched polymers with side chains containing ethylene carbonate (EC) groups mixed with lithium bis(trifluoromethane)sulfonimide (LiTFSI) salt. By systematically varying polymer architecture (degree of functionalization with function side chains and tether length), we establish Li+ transport mechanism and dynamical correlations between segmental relaxation of EC group and jump frequency of the cation. The insights obtained from MD simulations led to proposed an optimal polymer structure as well as generic principles for the design of novel SPE with high conductivity.

Optimizing Li-ion transport through architecture design of ethylene carbonate based comb-branched chains in solid polymer electrolyte

Macromolecular Chemistry: The Second Century

[Author Benefits](https://scimeetings.acs.org/?utm_source=pubs_content_marketing&utm_medium=website&utm_campaign=0320_MCF_NPI_Launch_Spring_Homepage&ref=pubs_content_marketing)

[How to use SciMeetings](https://storage.googleapis.com/dl.morressier.com/acs/SciMeetings-ACSSpring2020-HowToGuide_M3020-Final.pdf)

[Frequently Asked Questions](https://storage.googleapis.com/dl.morressier.com/acs/SciMtng_ACSNMSp2020_FAQ_M3120_Final.pdf)

ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.