Direct correlation between void formation and lithium dendrite growth in solid-state electrolytes with interlayers

Raj, V and Venturi, V and Kankanallu, VR and Kuiri, B and Viswanathan, V and Aetukuri, NPB (2022) Direct correlation between void formation and lithium dendrite growth in solid-state electrolytes with interlayers. In: Nature Materials .

PDF nat_mat_2022.pdf - Published Version Restricted to Registered users only Download (2MB) | Request a copy

Abstract

Solid-state Li-ion batteries with lithium anodes offer higher energy densities and are safer than conventional liquid electrolyte-based Li-ion batteries. However, the growth of lithium dendrites across the solid-state electrolyte layer leads to the premature shorting of cells and limits their practical viability. Here, using solid-state Li half-cells with metallic interlayers between a garnet-based lithium-ion conductor and lithium, we show that interfacial void growth precedes dendrite nucleation and growth. Specifically, void growth was observed at a current density of around two-thirds of the critical current density for dendrite growth. Computational calculations reveal that interlayer materials with higher critical current densities for dendrite growth also have the largest thermodynamic and kinetic barriers for lithium vacancy accumulation at their interfaces with lithium. Our results suggest that interfacial modification with suitable metallic interlayers decreases the tendency for void growth and improves dendrite growth tolerance in solid-state electrolytes, even in the absence of high stack pressures. © 2022, The Author(s), under exclusive licence to Springer Nature Limited.

Item Type:	Journal Article
Publication:	Nature Materials
Publisher:	Nature Research
Additional Information:	The copyright for this article belongs to the Nature Research.
Keywords:	Current density; Ions; Lithium-ion batteries; Solid-State Batteries, Dendrite growth; Electrolyte layers; Higher energy density; Liquid electrolytes; Lithium anode; Lithium dendrite; Metallic interlayer; Solid-state electrolyte; Void growth; Voids formation, Solid electrolytes
Department/Centre:	Division of Chemical Sciences > Solid State & Structural Chemistry Unit
Date Deposited:	30 Sep 2022 04:47
Last Modified:	30 Sep 2022 04:47
URI:	https://eprints.iisc.ac.in/id/eprint/76858

Actions (login required)

View Item