Electron and Ion Co-Conductive Catalyst Achieving Instant Transformation of Lithium Polysulfide towards Li2 S.

Most of the catalysts in lithium sulfur (Li-S) batteries present low electronic conductivity and the lithium polysulfides (LiPSs) must diffuse onto the surface of the carbon materials to achieve their conversion reaction. It is a significant challenge to achieve the instantaneous transformation of LiPSs to Li2 S in Li-S batteries to suppress the shuttle effect of LiPSs. Herein, a unique electron and ion co-conductive catalyst of carbon-coated Li1.4 Al0.4 Ti1.6 (PO4 )3 (C@LATP) is developed, which not only possesses strong adsorption to LiPSs, but, more importantly, also promotes the instantaneous conversion reaction of LiPSs to Li2 S. The C@LATP nanoparticles as catalytic active sites can synchronously and efficiently provide both Li ions and electrons to facilitate the conversion reaction of LiPSs. The conversion reaction path of LiPSs using C@LATP changes from traditional "adsorption-diffusion-conversion" to novel "adsorption-conversion," which effectively lowers the decomposition barrier of Li2 S6 and promotes faster conversion of LiPSs. The shuttle effect of LiPSs is considerably suppressed and utilization of sulfur is greatly improved. The Li-S batteries using C@LATP present excellent rate, cycling, and self-discharge properties. This work highlights the significance of electron and ion co-conductive solid-state electrolytes for the instantaneous transformation of LiPSs in advanced Li-S batteries.

Integrated Structure of Cathode and Double-Layer Electrolyte for Highly Stable and Dendrite-Free All-Solid-State Li-Metal Batteries.

All-solid-state batteries have become the most potential next-generation energy-storage devices. However, it is quite difficult to simultaneously achieve a single solid-state electrolytes (SSEs) layer with both dendrite-free Li metal plating and low interfacial resistance between the cathode and SSEs. Herein, an integrated structure of cathode and double-layer solid electrolyte membrane (IS-CDL) is designed, which greatly improves the interfacial contact and suppresses the Li dendrite growth. The first "polymer in ceramic" solid electrolyte layer (SL1) consists of 80 wt % Li1.4Al0.4Ti1.6(PO4)3 (LATP) nanoparticles and 20 wt % polyethylene oxide (PEO), and the second polymer electrolyte layer is PEO-based solid electrolyte layer (SL2). The SL1 with high mechanical properties can hinder the growth of Li dendrites and reduce the interfacial resistance with the cathode. The SL2 can inhibit the side reaction between the Li metal and LATP. The Li symmetric cells with sandwich-type hierarchical electrolyte (SL2/SL1/SL2) can stably cycle over 3200 h at 0.1 mA cm-2 at 45 °C. The obtained all-solid-state LiFePO4-IS-CDL/Li batteries present a capacity of 142.6 mA h g-1 at 45 °C with the capacity retention of 91.7% after 100 cycles, and all-solid-state NCM811-IS-CDL/Li batteries deliver a specific capacity of 175.5 mA h g-1 at 60 °C. This work proposes an effective strategy to fabricate all-solid-state lithium batteries with high electrochemical performance.