Low-Bandgap Se-Deficient Antimony Selenide as a Multifunctional Polysulfide Barrier toward High-Performance Lithium-Sulfur Batteries

The shuttling behavior and sluggish conversion kinetics of the intermediate lithium polysulfides (LiPSs) represent the main obstructions to the practical application of lithium-sulfur (Li-S) batteries. Herein, an anion-deficient design of antimony selenide (Sb2Se3-x) is developed to establish a multifunctional LiPS barrier toward the inhibition of polysulfide shuttling and enhancement of battery performance. The defect chemistry in the as-developed Sb2Se3-x promotes the intrinsic conductivity, strengthens the chemical affinity to LiPSs, and catalyzes the sulfur electrochemical conversion, which are verified by a series of computational and experimental results. Attributed to these unique superiorities, the obtained LiPS barrier efficiently promotes and stabilizes the sulfur electrochemistry, thus enabling excellent Li-S battery performance, e.g., outstanding cyclability over 500 cycles at 1.0 C with a minimum capacity fading rate of 0.027% per cycle, a superb rate capability up to 8.0 C, and a high areal capacity of 7.46 mAh cm(-2) under raised sulfur loading. This work offers a defect engineering strategy toward fast and durable sulfur electrochemistry, holding great promise in developing practically viable Li-S batteries as well as enlightening the material design of related energy storage and conversion systems.