Nonambient Thermodynamics in Solid-State Batteries

Most solid-state electrochemical reactions, such as those in lithium-ion batteries, are described well using thermodynamics under ambient conditions. In this work, we show that the microscopic stress in the composite cathode of solid-state batteries is highly heterogeneous and can exceed several hundreds of MPa via quasi in situ confocal Raman spectroscopy, making expansion work (pΔV) no longer negligible. We observed a strong correlation between the state of charge of cathode particles with their state of stress. By building a nonambient thermodynamics framework to describe cathode reactions in solid-state batteries, we identified the substantial mechanical potential (up to tens of mV) as a primary cause of capacity loss upon electrochemical cycling. Pairing a cathode and solid electrolyte of similar partial molar volumes is suggested to mitigate this issue. This work highlights the importance of considering expansion work in solid-state batteries and suggests new materials’ design rules for improved electrochemical performance.

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Publication Details

Journal
ACS Energy Letters
Published
2025-08-11
DOI
https://doi.org/10.1021/acsenergylett.5c01704
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
0.00

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article

Nonambient Thermodynamics in Solid-State Batteries

Yunlong Guo, Jincheng Zhong, Jingying Zhou, Zhe-Tao Sun et al.
ACS Energy Letters
Advancements in Battery Materials
article

Nonambient Thermodynamics in Solid-State Batteries

Yunlong Guo, Jincheng Zhong, Jingying Zhou, Zhe-Tao Sun, Hong Zhu, Wenge Yang, Shou‐Hang Bo, Shiwei Chen, Xinyu Yu, Yuping Huang, Nana Li
article en

Abstract

Most solid-state electrochemical reactions, such as those in lithium-ion batteries, are described well using thermodynamics under ambient conditions. In this work, we show that the microscopic stress in the composite cathode of solid-state batteries is highly heterogeneous and can exceed several hundreds of MPa via quasi in situ confocal Raman spectroscopy, making expansion work (pΔV) no longer negligible. We observed a strong correlation between the state of charge of cathode particles with their state of stress. By building a nonambient thermodynamics framework to describe cathode reactions in solid-state batteries, we identified the substantial mechanical potential (up to tens of mV) as a primary cause of capacity loss upon electrochemical cycling. Pairing a cathode and solid electrolyte of similar partial molar volumes is suggested to mitigate this issue. This work highlights the importance of considering expansion work in solid-state batteries and suggests new materials’ design rules for improved electrochemical performance.

ACS Energy LettersVol. 10(9)
Shanghai Jiao Tong University (CN), Joint Institute for Nuclear Astrophysics (US), University of Michigan (US), Bio-Synthesis (United States) (US), Center for High Pressure Science and Technology Advanced Research (CN), Chemical Synthesis Lab (SG)
National Natural Science Foundation of China, National Key Research and Development Program of China
Affordable and clean energy
Openalex Percentile: Top 81%
Advancements in Battery Materials
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