Electrochemically induced fracture in LLZO: How the interplay between flaw density and electrostatic potential affects operability

Monismith, Scott; Qu, Jianmin; Dingreville, Rémi

doi:10.1016/j.jpowsour.2023.232646

Electrochemically induced fracture in LLZO: How the interplay between flaw density and electrostatic potential affects operability

Journal Article · Tue Jan 10 23:00:00 EST 2023 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2023.232646· OSTI ID:2311726

^[1]; Qu, Jianmin ^[2]; ^[3]

Tufts Univ., Medford, MA (United States)
Tufts Univ., Medford, MA (United States); Stevens Institute of Technology, Hoboken, NJ (United States)
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Fracture and short circuit in the Li₇La₃Zr₂O₁₂ (LLZO) solid electrolyte are two key issues that prevent its adoption in battery cells. In this paper, we utilize phase-field simulations that couple electrochemistry and fracture to evaluate the maximum electric potential that LLZO electrolytes can support as a function of crack density. In the case of a single crack, we find that the applied potential at the onset of crack propagation exhibits inverse square root scaling with respect to crack length, analogous to classical fracture mechanics. Here, we further find that the short-circuit potential scales linearly with crack length. In the realistic case where the solid electrolyte contains multiple cracks, we reveal that failure fits the Weibull model. The failure distributions shift to favor failure at lower overpotentials as areal crack density increases. Furthermore, when flawless interfacial buffers are placed between the applied potential and the bulk of the electrolyte, failure is mitigated. When constant currents are applied, current focuses in near-surface flaws, leading to crack propagation and short circuit. We find that buffered samples sustain larger currents without reaching unstable overpotentials and without failing. Our findings suggest several mitigation strategies for improving the ability of LLZO to support larger currents and improve operability.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003525

OSTI ID:: 2311726

Report Number(s):: SAND--2023-12251J

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Vol. 559; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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