In Situ Synthesis of Organopolysulfides Enabling Spatial and Kinetic Co-Mediation of Sulfur Chemistry.

Abstract

Li-S batteries have been regarded as one of the most promising alternatives of the next-generation Li batteries. However, the dissolution and shuttling of lithium polysulfides lead to low cycle stability and low Coulombic efficiency, which intensively hinder the practical application of Li-S batteries. Herein, we propose a strategy to simultaneously promote the redox kinetics and inhibit the shuttle of lithium polysulfides, through in situ synthesis of insoluble organopolysulfides by adding a special additive. Attractively, the thus-formed insoluble organopolysulfides in the form of nanoparticle aggregates are also capable of adsorbing unconverted lithium polysulfides and hence effectively spatially suppress the shuttle effect. Furthermore, the organopolysulfides served as active redox mediators, showing faster redox kinetics of S chemistry than that of lithium polysulfides. As a result, the Li-S batteries showed impressive capacity, improved rate performance, and long cycling stability even under lean-electrolyte and high sulfur loading conditions.