Long‐Cycling All‐Solid‐State Batteries Achieved by 2D Interface between Prelithiated Aluminum Foil Anode and Sulfide Electrolyte

Abstract

All‐solid‐state batteries (ASSBs) with alloy anodes are expected to achieve high energy density and safety. However, the stability of alloy anodes is largely impeded by their large volume changes during cycling and poor interfacial stability against solid‐state electrolytes. Here, a mechanically prelithiation aluminum foil (MP‐Al‐H) is used as an anode to construct high‐performance ASSBs with sulfide electrolyte. The dense Li–Al layer of the MP‐Al‐H foil acts as a prelithiated anode and forms a 2D interface with sulfide electrolyte, while the unlithiated Al layer acts as a tightly bound current collector and ensures the structural integrity of the electrode. Remarkably, the MP‐Al‐H anode exhibits superior lithium conduction kinetics and stable interfacial compatibility with Li6PS5Cl (LPSCl) and Li10GeP2S12 electrolytes. Consequently, the symmetrical cells using LPSCl electrolyte can work at a high current density of 7.5 mA cm−2 and endure for over 1500 h at 1 mA cm−2. Notably, ≈100% capacity is retained for the MP‐Al‐H||LPSCl||LiCoO2 full cell with high area loadings of 18 mg cm−2 after 300 cycles. This work offers a pathway to improve the interfacial and performance issues for the application of ASSBs.

Toward Ultrastable Metal Anode/Li6PS5Cl Interface via an Interlayer as Li Reservoir

“…According to the analysis details for Figure S12, it is concluded that, in all-solid-state batteries, the Pre In anode has the ability of improving interfacial compatibility and effective utilization of active Li, which is inseparable from the multifunctional interlayer formed on it. In comparison to other reports, ,,,− sulfide-based solid-state cells in this work show superior performances in view of the cycling life span, capacity retention, and areal current density (Figure e), which proves the effectiveness of a generated interlayer on the improvement of metal anode/LPSCl interface stability.…”

Covalent Organic Framework Based Lithium–Sulfur Batteries: Materials, Interfaces, and Solid‐State Electrolytes

“…Therefore, scientists are con-tinually searching for ion-conducting materials that may complement or replace existing materials to create energy storage devices for the next generation. [158,[164][165][166] Replacing liquid electrolytes with SSEs has been proposed to create all-solid-state Li-S batteries (ASSLSBs) as the optimal solution to the aforementioned difficulties; this has drawn considerable scientific interest. SSEs developed for Li-S batteries can be classified into three subcategories: inorganic, polymer, and composite.…”

“…By contrast, polymer and composite SSEs exhibit better flexibility, processability, and interfacial compatibility. [162,165] Thus, polymer and composite SSEs that possess higher ionic conductivity at ambient temperatures and better mechanical strength at elevated temperatures must be urgently developed. [18] COFs are a type of organic crystalline porous material that combine the properties of polymers and inorganic crystalline materials.…”

Solid‐State Electrolytes in Lithium–Sulfur Batteries: Latest Progresses and Prospects

“…Compared to the polymer electrolyte and oxide electrolyte, sulfide electrolytes show more potential in commercial applications, in virtue of its high conductivity (10 −2 S cm −1 at room temperature) and malleability. [84,156,157] However, its limited electrochemical window makes inevitable compatibility and c) Reproduced with permission. [149] Copyright 2018, American Chemical Society.…”