Design of Quasi‐MOF Nanospheres as a Dynamic Electrocatalyst toward Accelerated Sulfur Reduction Reaction for High‐Performance Lithium–Sulfur Batteries

Lithium-sulfur (Li-S) batteries are considered as one of the most promising next-generation rechargeable batteries owing to their high energy density and cost-effectiveness. However, the sluggish kinetics of the sulfur reduction reaction process, which is so far insufficiently explored, still impedes its practical application. Metal-organic frameworks (MOFs) are widely investigated as a sulfur immobilizer, but the interactions and catalytic activity of lithium polysulfides (LiPs) on metal nodes are weak due to the presence of organic ligands. Herein, a strategy to design quasi-MOF nanospheres, which contain a transition-state structure between the MOF and the metal oxide via controlled ligand exchange strategy, to serve as sulfur electrocatalyst, is presented. The quasi-MOF not only inherits the porous structure of the MOF, but also exposes abundant metal nodes to act as active sites, rendering strong LiPs absorbability. The reversible deligandation/ligandation of the quasi-MOF and its impact on the durability of the catalyst over the course of the electrochemical process is acknowledged, which confers a remarkable catalytic activity. Attributed to these structural advantages, the quasi-MOF delivers a decent discharge capacity and low capacity-fading rate over long-term cycling. This work not only offers insight into the rational design of quasi-MOF-based composites but also provides guidance for application in Li-S batteries.