In Situ-Constructed Li_xMoS₂ with Highly Exposed Interface Boosting High-Loading and Long-Life Cathode for All-Solid-State Li–S Batteries

Abstract

As the persistent concerns regarding sluggish reaction kinetics and insufficient conductivities of sulfur cathodes in all-solid-state Li–S batteries (ASSLSBs), numerous carbon additives and solid-state electrolytes (SSEs) have been incorporated into the cathode to facilitate ion/electron pathways around sulfur. However, this has resulted in a reduced capacity and decomposition of SSEs. Therefore, it is worth exploring neotype sulfur hosts with electronic/ionic conductivity in the cathode. Herein, we present a hybrid cathode composed of few-layered S/MoS₂/C nanosheets (<5 layers) that exhibits high-loading and long-life performance without the need of additional carbon additives in advanced ASSLSBs. The multifunctional MoS₂/C host exposes the abundant surface for intimate contacting sites, in situ-formed Li_xMoS₂ during discharging as mixed ion/electron conductive network improves the S/Li₂S conversion, and contributes extra capacity for the part of active materials. With a high active material content (S + MoS₂/C) of 60 wt% in the S/MoS₂/C/Li₆PS₅Cl cathode composite (the carbon content is only ∼3.97 wt%), the S/MoS₂/C electrode delivers excellent electrochemical performance, with a high reversible discharge capacity of 980.3 mAh g^-1 (588.2 mAh g^-1 based on the whole cathode weight) after 100 cycles at 100 mA g^-1. The stable cycling performance is observed over 3500 cycles with a Coulombic efficiency of 98.5% at 600 mA g^-1, while a high areal capacity of 10.4 mAh cm^-2 is achieved with active material loading of 12.8 mg cm^-2.

Keywords

all-solid-state lithium–sulfur batteries / conversion/intercalation / high-loading and long-life / low carbon content / mixed ionic/electronic conductivities

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