Real-Time Stress Measurements in Lithium-ion Battery Negative-electrodes

TL;DR

This study measures real-time stress changes in lithium-ion battery electrodes during electrolyte wetting and cycling, revealing how stress develops and correlates with electrochemical processes, aiding damage prediction and electrode design.

Contribution

It introduces a wafer-curvature method to monitor stress evolution in practical electrodes, providing new insights into stress behavior during operation.

Findings

Electrode develops rapid compressive stress upon electrolyte addition.

Maximum stress during intercalation reaches 10-12 MPa.

Stress evolution correlates with staging behavior and cycling rate.

Abstract

Real-time stress evolution in a graphite-based lithium-ion battery negative-electrode during electrolyte wetting and electrochemical cycling is measured through wafer-curvature method. Upon electrolyte addition, the composite electrode rapidly develops compressive stress of the order of 1-2 MPa due to binder swelling; upon continued exposure, the stress continues to evolve towards an apparent plateau. During electrochemical intercalation at a slow rate, the compressive stress increases with the electrode's state-of-charge, reaching a maximum value of 10 - 12 MPa. There appears to be an approximate correlation between the rate of stress rise and the staging behavior of the lithiated graphite. De-intercalation at a slow rate results in a similar linear decrease in electrode stress. Tensile stress of a few MPa develops at the end of deintercalation in the first few cycles, after which the electrode remains under compressive stress only. Although higher peak stresses are seen at high C-rates, the dependence appears to be relatively weak (up to 5C). These measurements reveal, for the first time, the nature of stress evolution in practical lithium-ion-battery electrodes and provide useful data to quantify the driving force for mechanical damage that accrues in composite electrodes upon repeated cycling. While the reported results can serve as reference for calibrating theoretical and computational models to predict electrode stress and damage evolution, the methodology demonstrated can be used to measure stresses and characterize fatigue damage in any composite lithium-ion-battery electrode as well as optimize its microstructure to mitigate stress-related damage mechanisms.