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

• 成果类型: Article
• 署名作者: Yoon, Sun Geun; Vishnugopi, Bairav S.; Nelson, Douglas Lars; Yong, Adrian Xiao Bin; Wang, Yingjin; Sandoval, Stephanie Elizabeth; Thomas, Talia A.; Cavallaro, Kelsey Anne; Shevchenko, Pavel; Alsac, Elif Pinar; Wang, Congcheng; Singla, Aditya; Greer, Julia R.; Ertekin, Elif; Mukherjee, Partha P.; McDowell, Matthew T.
• 署名单位: University System of Georgia; Georgia Institute of Technology; Purdue University System; Purdue University; Purdue University in Indianapolis; University System of Georgia; Georgia Institute of Technology; University of Illinois System; University of Illinois Urbana-Champaign; University of Illinois System; University of Illinois Urbana-Champaign; California Institute of Technology; United States Department of Energy (DOE); Argonne National Laboratory; University of Illinois System; University of Illinois Urbana-Champaign
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-11755
• DOI: 10.1126/science.adt5229
• 发表日期: 2025-06-05
• 页码: 1062-1068
• 关键词: initio molecular-dynamics; total-energy calculations; elastic band method; mechanical-properties; interphase formation; mixed conductors; self-diffusion; alloy-anode; li; electrolytes

摘要

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.