Exploring the Impact of State of Charge and Aging on the Entropy Coefficient of Silicon–Carbon Anodes

Abstract

Due to its improved capacity compared to graphite, silicon is a promising candidate to handle the demands of high-energy batteries. With the introduction of new materials, further aspects of the battery system must be reconsidered. One of those aspects is the heat generation during the charging and discharging of a cell, which delivers important information for the development of cooling systems, the battery management system and the overall performance of the cell. Since the reversible heat presents an important contribution to the overall heat generation during cycling, the entropy coefficient is the main value that needs to be determined. This study evaluates the entropy coefficient of custom-produced 2032 coin half-cells with lithium counter electrodes, containing 45 wt% nanosilicon and 45 wt% carbon black. The potentiometric method, utilizing VR and self-discharge curves, produced reliable results, yielding entropy coefficient values between 95% SoC and 10% SoC during delithiation. These values of the entropy coefficient are consistently negative. Furthermore, ICA measurements identified two phase transitions during delithiation, with these transitions shifting to lower SoC as SoH decreases, impacting the slope of the entropy coefficient.