Measuring the buried interphase between solid electrolytes and lithium metal using neutrons

Westover, Andrew S.; Browning, Katie L.; Cannavó, Antonino; Gilles, Ralph; Vacik, Jiri; Browning, James F.; Paul, Neelima; Ceccio, Giovanni; Lavrentiev, Vasyl

doi:10.1039/d5ta05758b

Measuring the buried interphase between solid electrolytes and lithium metal using neutrons

Journal Article · Tue Sep 09 00:00:00 EDT 2025 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/d5ta05758b· OSTI ID:3002355

^[1]; Browning, Katie L. ^[1]; Cannavó, Antonino ^[2]; Gilles, Ralph ^[3]; Vacik, Jiri ^[4]; ^[1]; ^[3]; Ceccio, Giovanni ^[4]; Lavrentiev, Vasyl ^[4]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Technische Univ. München, Garching (Germany)
Czech Academy of Sciences (CAS), Rez (Czech Republic)

Interfaces are the key to next-generation high-energy batteries including solid-state Li metal batteries. In solid-state batteries, the buried nature of solid–solid electrolyte–electrode interfaces makes studying them difficult. Neutrons have significant potential to non-destructively probe these buried solid–solid interfaces. This work presents a comparative study using both neutron depth profiling (NDP) and neutron reflectometry (NR) to study a model lithium metal–lithium phosphorus oxynitride (LiPON) solid electrolyte system. In the NDP data, no distinct interphase is observed at the interface. NR shows a difference between electrodeposited, and vapor deposited LiPON–Li interfaces but finds both are gradient interphases that are less than 30 nm thick. Additional simulations of the LiPON–Li₂O–Li system demonstrate that NDP has an excellent resolution in the 50 nm–1 μm regime while NR has an ideal resolution from 0.1–200 nm with different sample requirements. Together NDP and NR can provide a complementary understanding of interfaces between Li metal and solid electrolytes across relevant length scales.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 3002355

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 41 Vol. 13; ISSN 2050-7488; ISSN 2050-7496

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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