Two-Step Growth Mechanism of the Solid Electrolyte Interphase in Argyrodyte/Li-Metal Contacts

• DOI: 10.1021/acsami.4c02548
• Publication Date: 2024-05-03T10:04:10Z
• Authors: Gracie Chaney; Andrey Golov; Ambroise van Roek...; Javier Carrasco; Natalio Mingo
• Keywords: Interphase; Lithium metal

The structure and growth of the solid electrolyte interphase (SEI) region between an electrode is one most fundamental yet less well-understood phenomena in solid-state batteries. We present atomistic simulation SEI for currently promising electrolytes (Li6PS5Cl), based on ab initio-trained machine learning interatomic potentials, over 30,000 atoms during 10 ns, well beyond capabilities conventional molecular dynamics. This unveils a two-step mechanism: Li-argyrodite chemical reaction leading to formation amorphous phase, followed by kinetically slower crystallization products into 5Li2S·Li3P·LiCl solution. results support recent, experimentally founded hypothesis indirect pathway reduction. These findings shed light intricate processes governing evolution, providing valuable foundation design optimization next-generation