Solid/Solid Interfacial Architecturing of Solid Polymer Electrolyte–Based All‐Solid‐State Lithium–Sulfur Batteries by Atomic Layer Deposition

Abstract

Solid polymer electrolytes (SPEs)-based all-solid-state lithium-sulfur batteries (ASSLSBs) have attracted extensive research attention due to their high energy density and safe operation, which provide potential solutions to the increasing need for harnessing higher energy densities. There is little progress made, however, in the development of ASSLSBs to improve simultaneously energy density and long-term cycling life, mostly due to the "shuttle effect" of lithium polysulfide intermediates in the SPEs and the low interfacial compatibility between the metal lithium anode and the SPE. In this work, the issues of solid/solid interfacial architecturing through atomic layer deposition of Al 2 O 3 on poly(ethylene oxide)-lithium bis(trifluoromethanesulfonyl)imide SPE surface are effectively addressed. The Al 2 O 3 coating promotes the suppression of lithium dendrite formation for over 500 h. ASSLSBs fabricated with two layers of Al 2 O 3 -coated SPE deliver high gravimetric/areal capacity and Coulombic efficiency, as well as excellent cycling stability and extremely low self-discharge rate. This work provides not only a simple and effective approach to boost the electrochemical performances of SPE-based ASSLSBs, but also enriches the fundamental understanding regarding the underlying mechanism responsible for their performance.

Inhibition of Polysulfide Shuttles in Li–S Batteries: Modified Separators and Solid‐State Electrolytes

“…To inhibit polysulfide shuttle and improve the interfacial stability, researchers have added inorganic fillers in PEO‐based solid polymer electrolytes such as Al 2 O 3 , [ 184,209 ] SiO 2 , [ 210 ] ZrO 2 , [ 211 ] nanoclay, [ 212,213 ] and MOF. [ 214 ]…”

A Decade of Progress on Solid‐State Electrolytes for Secondary Batteries: Advances and Contributions

“…[63] In contrast, Liu et al reported that an active Li surface grafted with double-block polymer brushes (DPB) to form a high Li + -conductivity polymeric interfacial layer (Figure 11d), [43] while Fan et al coated Al 2 O 3 onto an electrolyte surface by atomic layer deposition (Figure 11e). [193] Additionally, a self-healing adaptive buffer layer (an ABL consisting of low molecular-weight polypropylene carbonate, PEO and Li salt) (Figure 11f) and Pt metal, by magnetron sputtering (Figure 11g), were also proposed to stabilize the Li anode/polymer electrolyte interface. [42,194] Clearly, stable interfaces between the Li anode and polymer electrolyte can be successfully achieved by creating protective layers on the surface of the electrolyte or Li anode before (e.g., deposition or polymerization) and during (e.g., reacting with additives in the electrolyte) battery operation.…”

“…Reproduced with permission. [193] Copyright 2019, Wiley-VCH. f) The interface contact of Li/polymer electrolyte with or without ABL layer before and after electrochemical cycle.…”

Designing composite solid-state electrolytes for high performance lithium ion or lithium metal batteries

“…For example, solid/solid interfacial architecturing through atomic layer deposition of Al 2 O 3 on the SPE surface could suppress the "shuttle effect" of lithium polysulde intermediates in the SPE and increase the interfacial compatibility between the metal lithium anode and the SPE. 189 Considering the unique advantages of SSEs, some perspectives presented herein are based on CSSEs.…”