Palygorskite-Derived Ternary Fluoride with 2d Ion Transport Channels for Ampere Hour-scale Li-S Pouch Cell with High Energy Density.

Although various excellent electrocatalysts/adsorbents have made notable progress as sulfur cathode hosts on the lithium-sulfur (Li-S) coin-cell level, high energy density (W G ) of the practical Li-S pouch cells is still limited by inefficient Li-ion transport in the thick sulfur cathode under low electrolyte/sulfur (E/S) and negative/positive (N/P) ratios, which aggravates the shuttle effect and sluggish redox kinetics. Here we develop a new ternary fluoride MgAlF 5 ·2H 2 O with ultrafast ion conduction-strong polysulfides capture integration. MgAlF 5 ·2H 2 O has an inverse Weberite-type crystal framwork, in which the corner-sharing [AlF 6 ]-[MgF 4 (H 2 O) 2 ] octahedra units extend to form two-dimensional Li-ion transport channels along the [100] and [010] directions, respectively. Applied as the cathode sulfur host, the MgAlF 5 ·2H 2 O lithiated by LiTFSI (lithium salt in Li-S electrolyte) acts as a fast ionic conductor to ensure efficient Li-ion transport to accelerate the redox kinetics under high S loadings and low E/S and N/P. Meanwhile, the strong polar MgAlF 5 ·2H 2 O captures polysulfides by chemisorption to suppress the shuttle effect. Therefore, a 1.97 A h-level Li-S pouch cell achieves a high W G of 386 Wh kg -1 . This work develops a new-type ionic conductor, and provides unique insights and new hosts for designing practical Li-S pouch cells. This article is protected by copyright. All rights reserved.