Lithium-ion battery performance model including solvent segregation effects

TL;DR

This paper develops a two-solvent lithium-ion battery model that captures solvent segregation effects, improving accuracy over traditional single-solvent models and providing insights into electrolyte transport and degradation.

Contribution

It introduces a novel two-solvent electrolyte model within PyBaMM that accounts for solvent segregation and transport effects, enhancing battery performance prediction accuracy.

Findings

Predicts 6% more power loss at 4.5C discharge

Shows ~0.32% more capacity loss after 1000 cycles

Demonstrates importance of solvent segregation in modeling

Abstract

A model of a lithium-ion battery containing a cosolvent electrolyte is developed and implemented within the open-source PyBaMM platform. Lithium-ion electrolytes are essential to battery operation and normally contain at least two solvents to satisfy performance requirements. The widely used Doyle-Fuller-Newman battery model assumes that the electrolyte comprises a salt dissolved in a single effective solvent, however. This single-solvent approximation has been disproved experimentally and may hinder accurate battery modelling. Here, we present a two-solvent model that resolves the transport of ethylene carbonate (EC) and lithium salt in a background linear carbonate. EC concentration polarization opposes that of Li+ during cycling, affecting local electrolyte properties and cell-level overpotentials. Concentration gradients of Li+ can be affected by cross-diffusion, whereby EC gradients enhance or impede salt flux. A rationally parametrized model that includes EC transport predicts 6% more power loss at 4.5C discharge and ~0.32% more capacity loss after a thousand 1C cycles than its single-solvent equivalent. This work provides a tool to model more transport behaviour in the electrolyte that may affect degradation and enables the transfer of microscopic knowledge about solvation structure-dependent performance to the macroscale.