DOE OSTI · 3017052
Interface morphogenesis with a deformable secondary phase in solid-state lithium batteries
Abstract
Here, 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.
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Yoon, Sun Geun [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000262228962), Vishnugopi, Bairav S. [Purdue Univ., West Lafayette, IN (United States)], Nelson, Douglas Lars [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000334290547), Yong, Adrian Xiao Bin [Univ. of Illinois at Urbana-Champaign, IL (United States)] (ORCID:0000000206912380), Wang, Yingjin [California Institute of Technology (CalTech), Pasadena, CA (United States)] (ORCID:0009000212393422), Sandoval, Stephanie Elizabeth [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000208955237), Thomas, Talia A. [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000305086045), Cavallaro, Kelsey Anne [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000250669883), Shevchenko, Pavel [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)] (ORCID:000000027847472X), Alsaç, Elif Pınar [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000242559676), Wang, Congcheng [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000291562310), Singla, Aditya [Purdue Univ., West Lafayette, IN (United States)] (ORCID:000000034229605X), Greer, Julia R. [California Institute of Technology (CalTech), Pasadena, CA (United States)] (ORCID:0000000296751508), Ertekin, Elif [Univ. of Illinois at Urbana-Champaign, IL (United States)], Mukherjee, Partha P. [Purdue Univ., West Lafayette, IN (United States)], McDowell, Matthew T. [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000155523456). 2025-06-05. Interface morphogenesis with a deformable secondary phase in solid-state lithium batteries. https://doi.org/10.1126/science.adt5229
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