Integrated Interface Strategy toward Room Temperature Solid-State Lithium Batteries

Abstract

Solid-state lithium batteries have drawn wide attention to address the safety issues of power batteries. However, the development of solid-state lithium batteries is substantially limited by the poor electrochemical performances originating from the rigid interface between solid electrodes and solid-state electrolytes. In this work, a composite of poly(vinyl carbonate) and LiSnPS solid-state electrolyte is fabricated successfully via in situ polymerization to improve the rigid interface issues. The composite electrolyte presents a considerable room temperature conductivity of 0.2 mS cm, an electrochemical window exceeding 4.5 V, and a Li transport number of 0.6. It is demonstrated that solid-state lithium metal battery of LiFeMnPO (LFMP)/composite electrolyte/Li can deliver a high capacity of 130 mA h g with considerable capacity retention of 88% and Coulombic efficiency of exceeding 99% after 140 cycles at the rate of 0.5 C at room temperature. The superior electrochemical performance can be ascribed to the good compatibility of the composite electrolyte with Li metal and the integrated compatible interface between solid electrodes and the composite electrolyte engineered by in situ polymerization, which leads to a significant interfacial impedance decrease from 1292 to 213 Ω cm in solid-state Li-Li symmetrical cells. This work provides vital reference for improving the interface compatibility for room temperature solid-state lithium batteries.

Recent Progress of Hybrid Solid‐State Electrolytes for Lithium Batteries

“…[32] In-situ polymerization has been introduced to synthesize poly(vinyl carbonate)-Li 10 SnP 2 S 12 (PVCA-LSnPS), providing integrated interphase between electrodes and HSSE with dramatically decreased interfacial impendence. [33] Furthermore,t his HSSE delivers ah igh room temperature conductivity of 2 10 À4 Scm À1 ,a ne nlargede lectrochemical window of 4.5 Va nd improved lithium transference number of 0.6. The solid-state LiFe 0.2 Mn 0.8 PO 4 /HSSE/Li cell presents ah igh specific capacity of 130 mAh g À1 ands uperior cycling life over 140 cycles at 0.5 C, whichi se ven more stable than control cell based on liquid electrolyte.…”

“…Such change in composition would notably alter the ionic transport behavior as well as the mechanical properties. [33] Furthermore,t his HSSE delivers ah igh room temperature conductivity of 2 10 À4 Scm À1 ,a ne nlargede lectrochemical window of 4.5 Va nd improved lithium transference number of 0.6. Zhang and co-workers designed aL LZO incorporated poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP) HSSE, presenting high ionic con- [37] Reproduced with permission.…”

Intermolecular Chemistry in Solid Polymer Electrolytes for High‐Energy‐Density Lithium Batteries

“…Therefore, it can be speculated that although the bulk ion conduction of LLTO did not dominate ionic conductivity of CPE, the Li + in LLTO can provide continuous Li + hopping sites by Lewis acid–base interaction. Recently, poly(vinyl carbonate)/Li 10 SnP 2 S 12 (PVCA/LSnPS) was synthesized by in‐situ polymerization strategy . Density functional theory (DFT) analysis demenstrated that F − ions tended to be bound by LSnPS nanoparticles instead of PVCA.…”

Recent Progress in Organic–Inorganic Composite Solid Electrolytes for All‐Solid‐State Lithium Batteries

“…They also studied the effect of LGPS and LiTFSI components on interface for-mation within the composite electrolyte, and the resultss how that the electrolyte with 70 wt %L GPS-PEO( LiTFSI) prepared by meanso fb all-milling exhibits an enhanced Li + conductivity of 0.22 mS cm À1 .C ui et al fabricated ap oly(vinyl carbonate)-Li 10 SnP 2 S 12 (PVAC-LSPS) composite electrolyte throughi ns itu polymerization. [100] An integrated interface between electrodes and the composite electrolyte was built during the in situ polymerization process;t hus interface impendence was substantially decreased. Ther esulting composite electrolyte delivers a series of favorable electrochemical properties,i ncluding ah igh room-temperature ionic conductivity of 2 10 À4 Scm À1 ,awide electrochemical window of 4.5 V, improved Li + transport number of 0.6, and good compatibility with the Li-metal anode.T he Li/LiFe 0.2 Mn 0.8 PO 4 ASSB shows ah igh specific capacity of 130 mA hg À1 and outstanding cyclings tabilityo ver 140 cycles at 0.5 C. Villaluenga et al developedn onflammable glass-polymer hybrid single-ion-conducting composite electrolytes.…”