TY - JOUR
T1 - Modeling Particle Versus SEI Cracking in Lithium-Ion Battery Degradation
T2 - Why Calendar and Cycle Aging Cannot Simply be Added
AU - Karger, Alexander
AU - O’Kane, Simon E.J.
AU - Rogge, Marcel
AU - Kirst, Cedric
AU - Singer, Jan P.
AU - Marinescu, Monica
AU - Offer, Gregory J.
AU - Jossen, Andreas
N1 - Publisher Copyright:
© 2024 The Author(s). Published on behalf of The Electrochemical Society by IOP Publishing Limited.
PY - 2024
Y1 - 2024
N2 - Degradation models are important tools for understanding and mitigating lithium-ion battery aging, yet a universal model that can predict degradation under all operating conditions remains elusive. One challenge is the coupled influence of calendar and cycle aging phases on degradation mechanisms, such as solid electrolyte interphase (SEI) formation. In this work, we identify and systematically compare three different SEI interaction theories found in the literature, and apply them to experimental degradation data from a commercial lithium-ion cell. In a step-by-step process, and after careful data selection, we show that SEI delamination without any cracking of the active particles, and SEI microcracking, where cycling only affects SEI growth during the cycle itself, are both unlikely candidates. Instead, the results indicate that upon cycling, both the SEI and the active particle crack, and we provide a simple, 4-parameter equation that can predict the particle crack rate. Contrary to the widely-accepted Paris’ law, the particle crack rate decreases with increasing cycles, potentially due to changing intercalation dynamics resulting from the increasing surface-to-volume ratio of the active particles. The proposed model predicts SEI formation accurately at different storage conditions, while simply adding the degradation from pure calendar and cycle aging underestimates the total degradation.
AB - Degradation models are important tools for understanding and mitigating lithium-ion battery aging, yet a universal model that can predict degradation under all operating conditions remains elusive. One challenge is the coupled influence of calendar and cycle aging phases on degradation mechanisms, such as solid electrolyte interphase (SEI) formation. In this work, we identify and systematically compare three different SEI interaction theories found in the literature, and apply them to experimental degradation data from a commercial lithium-ion cell. In a step-by-step process, and after careful data selection, we show that SEI delamination without any cracking of the active particles, and SEI microcracking, where cycling only affects SEI growth during the cycle itself, are both unlikely candidates. Instead, the results indicate that upon cycling, both the SEI and the active particle crack, and we provide a simple, 4-parameter equation that can predict the particle crack rate. Contrary to the widely-accepted Paris’ law, the particle crack rate decreases with increasing cycles, potentially due to changing intercalation dynamics resulting from the increasing surface-to-volume ratio of the active particles. The proposed model predicts SEI formation accurately at different storage conditions, while simply adding the degradation from pure calendar and cycle aging underestimates the total degradation.
KW - calendar aging
KW - cycle aging
KW - particle cracking
KW - path dependence
KW - SEI layer
UR - http://www.scopus.com/inward/record.url?scp=85205081234&partnerID=8YFLogxK
U2 - 10.1149/1945-7111/ad76da
DO - 10.1149/1945-7111/ad76da
M3 - Article
AN - SCOPUS:85205081234
SN - 0013-4651
VL - 171
JO - Journal of the Electrochemical Society
JF - Journal of the Electrochemical Society
IS - 9
M1 - 090512
ER -