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DOE OSTI · 3024491

Chemical and Structural Insights into Solid Electrolyte Interphase Evolution for Sodium Metal Electrodes

Lo, Chang-An [Stony Brook Univ., NY (United States)] (ORCID:0009000672713028)·Singla, Aditya [Purdue Univ., West Lafayette, IN (United States)]·Kankanallu, Varun R. [Stony Brook Univ., NY (United States)] (ORCID:0000000209545803)·Yen, Dean [Stony Brook Univ., NY (United States)]·Vishnugopi, Bairav S. [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0009000263579358)·Gann, Eliot [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000155708880)·Wiegart, Lutz [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000344178479)·Mukherjee, Partha P. [Purdue Univ., West Lafayette, IN (United States)]·Jaye, Cherno [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)]·Wąsik, Patryk [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)]·Chen-Wiegart, Yu-chen Karen [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000344452159)
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Abstract

The solid electrolyte interphase (SEI) critically governs the reversibility of sodium metal batteries, through dynamically mediating ion transport and interfacial reactions. However, its kinetic evolution under operating conditions, and how it influences interfacial stability, remains poorly understood. Here, in this study, we reveal that the SEI undergoes coupled chemical and mechanical changes during sodium plating and stripping, leading to spatial and temporal heterogeneity that drives interfacial degradation. Synchrotron operando grazing-incidence wide-angle X-ray scattering and soft X-ray absorption spectroscopy capture the sequential formation and dissolution of inorganic SEI phases (NaF, NaH, NaOH, Na 2 PO 3 F), accompanied by depth-dependent alterations in organic SEI components. Mesoscale modeling connects this evolving SEI heterogeneity to localized current density fluctuations and stress accumulation at the Na interface, identifying pathways to electrically isolated sodium formation. These findings show that SEI instability fundamentally limits reversibility in sodium metal batteries, and that controlling SEI chemistry–mechanics coupling is essential to achieving its durability.

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36 MATERIALS SCIENCE

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Lo, Chang-An [Stony Brook Univ., NY (United States)] (ORCID:0009000672713028), Singla, Aditya [Purdue Univ., West Lafayette, IN (United States)], Kankanallu, Varun R. [Stony Brook Univ., NY (United States)] (ORCID:0000000209545803), Yen, Dean [Stony Brook Univ., NY (United States)], Vishnugopi, Bairav S. [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0009000263579358), Gann, Eliot [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000155708880), Wiegart, Lutz [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000344178479), Mukherjee, Partha P. [Purdue Univ., West Lafayette, IN (United States)], Jaye, Cherno [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)], Wąsik, Patryk [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)], Chen-Wiegart, Yu-chen Karen [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000344452159). 2026-03-05. Chemical and Structural Insights into Solid Electrolyte Interphase Evolution for Sodium Metal Electrodes. https://doi.org/10.1021/acsenergylett.5c03538

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