What dictates soft clay-like lithium superionic conductor formation from rigid salts mixture

Journal Article · 27 October 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-42538-2 · OSTI ID:2203999

Gupta, Sunny ; Yang, Xiaochen; Ceder, Gerbrand

Abstract Soft clay-like Li-superionic conductors, integral to realizing all-solid-state batteries, have been recently synthesized by mixing rigid-salts. Here, through computational and experimental analysis, we clarify how a soft clay-like material can be created from a mixture of rigid-salts. Using molecular dynamics simulations with a deep learning-based interatomic potential energy model, we uncover the microscopic features responsible for soft clay-formation from ionic solid mixtures. We find that salt mixtures capable of forming molecular solid units on anion exchange, along with the slow kinetics of such reactions, are key to soft-clay formation. Molecular solid units serve as sites for shear transformation zones, and their inherent softness enables plasticity at low stress. Extended X-ray absorption fine structure spectroscopy confirms the formation of molecular solid units. A general strategy for creating soft clay-like materials from ionic solid mixtures is formulated.

• Research Organization: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
• Sponsoring Organization: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
• Grant/Contract Number: AC02-05CH11231; SC0012704
• OSTI ID: 2203999
• Journal Information: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723
• Publisher: Nature Publishing GroupCopyright Statement
• Country of Publication: United Kingdom
• Language: English