Interface Stability in Solid-State Batteries

Richards, William D.; Miara, Lincoln J.; Wang, Yan; Kim, Jae Chul; Ceder, Gerbrand

doi:10.1021/acs.chemmater.5b04082

Cited by 1,652Advanced Battery Materials and TechnologiesAdvancements in Battery MaterialsThermal Expansion and Ionic Conductivity

Interface Stability in Solid-State Batteries

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Richards, William D., Miara, Lincoln J., Wang, Yan, Kim, Jae Chul, Ceder, Gerbrand·2016·Chemistry of Materials

DOI 10.1021/acs.chemmater.5b04082

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Abstract

Development of high conductivity solid-state electrolytes for lithium ion batteries has proceeded rapidly in recent years, but incorporating these new materials into high-performing batteries has proven difficult. Interfacial resistance is now the limiting factor in many systems, but the exact mechanisms of this resistance have not been fully explained - in part because experimental evaluation of the interface can be very difficult. In this work, we develop a computational methodology to examine the thermodynamics of formation of resistive interfacial phases. The predicted interfacial phase formation is well correlated with experimental interfacial observations and battery performance. We calculate that thiophosphate electrolytes have especially high reactivity with high voltage cathodes and a narrow electrochemical stability window. We also find that a number of known electrolytes are not inherently stable but react in situ with the electrode to form passivating but ionically conducting barrier layers. As a reference for experimentalists, we tabulate the stability and expected decomposition products for a wide range of electrolyte, coating, and electrode materials including a number of high-performing combinations that have not yet been attempted experimentally.

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Soft anions such as Te2- and I- readily permit cation transport but do not possess the requisite electrochemical (redox) stability for use as solid electrolytes; conversely, hard anions such as O2- and F- are redox-stable but bind cations strongly, and the resulting materials usually display limited ionic conductivity.
“This points to an interesting contraindication in materials design: soft anions such as Te2– and I– readily permit cation transport but do not possess the requisite electrochemical (redox) stability for use as solid electrolytes. Conversely, hard anions such as O2– and F– are redox-stable, but they bind cations strongly, and the resulting materials usually display limited ionic conductivity.”
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Authors: Richards, W. D., Miara, L. J., Wang, Y., Kim, J. C., & Ceder, G.
Affiliations: Massachusetts Institute of Technology (US)
Samsung Advanced Institute of Technology - USA , 255 Main Street, Suite 702 , , ,
Lawrence Berkeley National Laboratory (US)
Corresponding author: Ceder, Gerbrand
ORCID: Richards, William D.
Miara, Lincoln J.
Wang, Yan
Kim, Jae Chul
Ceder, Gerbrand
Venue: Chemistry of Materials
Publisher: American Chemical Society (ACS)
Published: 2015-12-07
Volume: 28
Issue: 1
Pages: 266-273
ISSN: 0897-4756 (ISSN-L)
1520-5002
DOI: 10.1021/acs.chemmater.5b04082
OpenAlex: W2237868774
Cited by: 1,652
References: 60
Citations by year: 2026: 156 · 2025: 188 · 2024: 181 · 2023: 199 · 2022: 204 · 2021: 196 · 2020: 173 · 2019: 141 · 2018: 112 · 2017: 74 · 2016: 28
FWCI: 33.24
Type: journal article
Language: en
Open access: hybrid
doi.org
Licence: other-oa
pubs.acs.org/page/policy/authorchoice_termsofuse.html (vor, 11 d)
Locations: Chemistry of Materials (publishedVersion, other-oa)
DSpace@MIT (Massachusetts Institute of Technology) (submittedVersion, cc-by-nc)
Funders: Samsung (NA)
Topics: Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
Physical Sciences › Materials Science › Materials Chemistry › Thermal Expansion and Ionic Conductivity
Keywords: solid-state batteries, solid electrolytes, interfacial resistance, interfacial stability, interfacial phase formation, high-voltage cathodes, electrochemical stability window, electrolyte decomposition products, lithium-ion batteries

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Interface Stability in Solid-State Batteries

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