Micromechanism in All-Solid-State Alloy-Metal Batteries: Regulating Homogeneous Lithium Precipitation and Flexible Solid Electrolyte Interphase Evolution

Abstract

Sulfide-based solid-state electrolytes (SSEs) matched with alloy anodes are considered as promising candidates for application in all-solid-state batteries (ASSBs) to overcome the bottlenecks of the lithium (Li) anode. However, an understanding of the dynamic electrochemical processes on alloy anode in SSE is still elusive. Herein, in situ atomic force microscopy gives insights into the block-formation and stack-accumulation behaviors of Li precipitation on an Li electrode, uncovering the morphological evolution of nanoscale Li deposition/dissolution in ASSBs. Furthermore, two-dimensional Li–indium (In) alloy lamellae and the homogeneous solid electrolyte interphase (SEI) shell on the In electrode reveal the precipitation mechanism microscopically regulated by the alloy anode. The flexible and wrinkle-structure SEI shell further enables the electrode protection and inner Li accommodation upon cycles, elucidating the functional influences of SEI shell on the cycling behaviors. Such on-site tracking of the morphological evolution and dynamic mechanism provide an in-depth understanding and thus benefit the optimizations of alloy-based ASSBs.

Constructing a stable interface between the sulfide electrolyte and the Li metal anodeviaa Li+-conductive gel polymer interlayer

“…4c, after 30 cycles, the R SUM of the Li|LGPS|Li cell (70 kO) is greatly increased compared with that before cycle (Table S2, ESI †), indicating that a large number of poor ionic conductors were continuously produced on the Li-LGPS interface. 28,45,46 Conversely, the R SUM of the modified Li|GPI-LGPS-GPI|Li cell remains unchanged after cycling (Table S2, ESI †), again demonstrating that the GPI as the interlayer between the Li metal and LGPS can block significant interfacial reactions between the Li metal and LGPS, thus promising a higher electrochemical stability (Fig. 4d).…”

Air Stability and Interfacial Compatibility of Sulfide Solid Electrolytes for Solid‐State Lithium Batteries: Advances and Perspectives

“…Copyright 2020, American Chemical Society. b) Schematic diagrams of the dynamic evolution and interfacial mechanism of Li and Li x In [68] . Copyright 2021, American Chemical Society.…”

Characterizing Batteries by In Situ Electrochemical Atomic Force Microscopy: A Critical Review

“…Dynamic visualization of the Li deposition/dissolution was achieved by in situ EC‐AFM, via monitoring of the lateral interface between Li–In alloy anode and Li 10 GeP 2 S 12 (LGPS) SSE. [ 290 ] The Li‐In alloy anode with a high ionic diffusion coefficient and low ionic migration barrier induces the homogeneous formation of an SEI and 2D uniform growth of Li x In lamellae upon lithiation. The on‐site tracking of the morphological evolution and dynamic mechanism in these studies provides an in‐depth understanding of the electrode/SSE interfaces.…”