Assessing the Long-Term Reactivity to Achieve Compatible Electrolyte–Electrode Interfaces for Solid-State Rechargeable Lithium Batteries Using First-Principles Calculations

Lieven Bekaert, Ashish Raj, Jean-François Gohy, Annick Hubin, Frank De Proft, Mesfin H. Mamme

Research output: Contribution to journalArticlepeer-review

Abstract

Designing compatible electrode–electrolyte interfaces is critical to achieve high and consistent performance and life span in next-generation rechargeable lithium batteries. In the study of nanoscopic interfaces, ab initio molecular dynamics (AIMD) simulations allow for a highly accurate description of interface dynamics and reactions. However, due to the high computational cost, simulations are limited in the size and time domains and therefore merit the need for a new interpretational approach that can deduce the long-term reactivity from such short yet highly accurate simulations. In this study, this is established by means of bond length distribution analysis through which the reactivity of key solid polymer electrolyte (SPE) polymer functional groups in contact with key electrode materials (graphite, silicon, lithium) and the influence of the electric field and temperature was successfully determined. Bond length distributions were found to respond to environmental changes and relate to the long-term reactivity in which the strength of electrode surface interactions and the accessibility of functional groups were found to be critical factors. Furthermore, the balancing of the SPE polymer mobility and functional group–electrode surface attraction, respectively, kinetic and thermodynamic properties, further suggests a selective spatial orientation of functional groups when exposed to an electric field, which could have great implications for low-temperature and high-current-density environments. The obtained knowledge on how reactive key SPE polymer functional groups are and also how their reactivity changes in terms of the electric field orientation effect could provide new insights for designing new stable SPE polymers.
Original languageEnglish
Article number19
Pages (from-to)8227–8237
Number of pages11
JournalJournal of Physical Chemistry C
Volume126
Issue number19
DOIs
Publication statusPublished - 13 Apr 2022

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