Interface Morphogenesis with a Deformable Secondary Phase in Solid-State Lithium Batteries
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1.
Georgia Institute of Technology
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2.
Purdue University West Lafayette
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3.
University of Illinois Urbana-Champaign
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4.
California Institute of Technology
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5.
Argonne National Laboratory
Abstract
The complex and uncontrolled morphological evolution of lithium metal at the interface with solid-state electrolytes limits performance of solid-state batteries, leading to inhomogeneous reactions and contact loss. Inspired by biological morphogenesis, we introduce a new interfacial self-regulation concept in which a deformable secondary phase dynamically aggregates at the interface in response to local electro-chemo-mechanical stimuli, serving to enhance contact. Stripping of a lithium electrode containing 5-20% redox-inactive sodium domains causes spontaneous sodium accumulation across the interface, with the sodium undergoing local plastic deformation as lithium is removed to attain intimate electrical contact without blocking transport channels. This process, characterized with operando X-ray tomography and electron microscopy, mitigates void formation and substantially improves battery cycling performance at the low stack pressures needed for practical applications. The counterintuitive strategy of adding inactive alkali metal to improve performance demonstrates that interfacial self-regulation is a promising pathway to efficient solid-state batteries.
Copyright and License
The content is available under CC BY NC 4.0
Conflict of Interest
Some of the authors are inventors on a patent application related to the materials.
Funding
Support is acknowledged from the Defense Advanced Research Projects Agency Morphogenic Interfaces (MINT) Program under Cooperative Agreement number 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 U.S. Department of Energy (DOE) Office of Science user facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.
Contributions
Conceptualization: S.G.Y., M.T.M.; Methodology: S.G.Y., B.S.V., A.X.B.Y., M.T.M.; Formal analysis: S.G.Y., B.S.V., D.L.N., A.X.B.Y., S.E.S., P.S., A.S., J.R.G., E.E., P.P.M., M.T.M.; Investigation: S.G.Y., D.L.N., Y.W., S.E.S., T.A.T., K.A.C., P.S., E.P.A., C.W.; Validation: S.G.Y., J.R.G., E.E., M.T.M.; Visualization: S.G.Y., M.T.M.; Writing – Original Draft: S.G.Y.; Writing – Review & Editing: S.G.Y., J.R.G., E.E., P.P.M., M.T.M.; Supervision: M.T.M.; Funding acquisition: M.T.M.; Project administration: M.T.M.
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Additional details
- Defense Advanced Research Projects Agency
- Morphogenic Interfaces (MINT) Program HR00112220028
- National Science Foundation
- ECCS-2025462
- Office of Science
- DE-AC02- 06CH11357
- Caltech groups
- Division of Engineering and Applied Science (EAS)
- Publication Status
- Submitted