Fracture Dynamics in Silicon Anode Solid-State Batteries

Nelson, Douglas Lars; Sandoval, Stephanie E.; Pyo, Jaechan; Bistri, Donald; Thomas, Talia A.; Cavallaro, Kelsey Anne; Lewis, John A.; Iyer, Abhinav S.; Shevchenko, Pavel; Di Leo, Claudio V.; McDowell, Matthew T.

doi:10.1021/acsenergylett.4c02800

Fracture Dynamics in Silicon Anode Solid-State Batteries

Journal Article · Tue Nov 26 00:00:00 EST 2024 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.4c02800· OSTI ID:2481398

Nelson, Douglas Lars ^[1]; ^[1]; Pyo, Jaechan ^[1]; ^[1]; Thomas, Talia A. ^[1]; Cavallaro, Kelsey Anne ^[1]; Lewis, John A. ^[1]; Iyer, Abhinav S. ^[1]; Shevchenko, Pavel ^[2]; Di Leo, Claudio V. ^[1]; ^[1]

Georgia Institute of Technology, Atlanta, GA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

Solid-state batteries (SSBs) with silicon anodes could enable improved safety and energy density compared to lithium-ion batteries. However, degradation arising from the massive volumetric changes of silicon anodes during cycling is not well understood in solid-state systems. Here, we use operando X-ray computed microtomography to reveal micro- to macro-scale chemo-mechanical degradation processes of silicon anodes in SSBs. Mud-type channel cracks driven by biaxial tensile stress form across the electrode during delithiation. We also find detrimental cracks at the silicon/ solid electrolyte interface that form due to local reaction competition between neighboring domains of different sizes. Continuum phase-field damage modeling quantifies stress-driven channel cracking and shows that the lithiated silicon stress state is critical for determining the extent of interfacial fracture. This work reveals the mechanisms that govern SSBs compared to conventional lithium-ion batteries and provides guidelines for engineering chemomechanically resilient electrodes for high-energy batteries.

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Research Organization:: Georgia Institute of Technology, Atlanta, GA (United States)

Sponsoring Organization:: National Aeronautics and Space Administration (NASA); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2481398

Alternate ID(s):: OSTI ID: 2481251

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 12 Vol. 9; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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