Interface morphogenesis with a deformable secondary phase in solid-state lithium batteries

Creators: Yoon, Sun Geun¹; Vishnugopi, Bairav S.²; Nelson, Douglas Lars¹; Yong, Adrian Xiao Bin³; Wang, Yingjin⁴; Sandoval, Stephanie Elizabeth¹; Thomas, Talia A.¹; Cavallaro, Kelsey Anne¹; Shevchenko, Pavel⁵; Alsaç, Elif Pınar¹; Wang, Congcheng¹; Singla, Aditya²; Greer, Julia R.⁴; Ertekin, Elif³; Mukherjee, Partha P.²; McDowell, Matthew T.¹

1. Georgia Institute of Technology
2. Purdue University West Lafayette
3. University of Illinois Urbana-Champaign
4. California Institute of Technology
5. Argonne National Laboratory

Abstract

The complex morphological evolution of lithium metal at the solid-state electrolyte interface limits performance of solid-state batteries, leading to inhomogeneous reactions and contact loss. Inspired by biological morphogenesis, we developed an interfacial self-regulation concept in which a deformable secondary phase dynamically aggregates at the interface in response to local electro-chemo-mechanical stimuli, enhancing contact. The stripping of a lithium electrode that contains 5 to 20 mole % electrochemically inactive sodium domains causes spontaneous sodium accumulation across the interface, with the sodium deforming to attain intimate electrical contact without blocking lithium transport. This process, characterized with operando x-ray tomography and electron microscopy, mitigates voiding and improves cycling at low stack pressures. The counterintuitive strategy of adding electrochemically inactive alkali metal to improve performance demonstrates the utility of interfacial self-regulation for solid-state batteries.

Copyright and License

© 2025 the authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original US government works. https://www.science.org/about/science-licenses-journal-article-reuse

Funding

Support is acknowledged from the Defense Advanced Research Projects Agency Morphogenic Interfaces (MINT) Program under cooperative agreement HR00112220028. The content of this article does not necessarily reflect the position of the policy of the government, and no official endorsement should be inferred. This work was performed in part at the Georgia Tech Institute for Matter and Systems, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), which is supported by the National Science Foundation (ECCS-2025462). This research used resources of the Advanced Photon Source, a US Department of Energy (DOE) Office of Science user facility operated for the DOE Office of Science by Argonne National Laboratory under contract DE-AC02-06CH11357. V. Sundaresan is acknowledged for helpful discussions.

Conflict of Interest

M.T.M. and S.G.Y. are inventors on US patent application 2024/0339624, which is related to the content in this article. All other authors declare no competing interests.

Supplemental Material

Materials and Methods; Supplementary Text; Figs. S1 to S25; Tables S1 to S8; References (50–100) (PDF)

Data S1 and S2 (ZIP)

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