Pt-NbC Composite as a Bifunctional Catalyst for Redox Transformation of Polysulfides in High-Rate-Performing...

Accelerating the redox reaction of polysulfides via catalysis is an effective way to suppress the shuttling effect in lithium-sulfur (Li-S) cells. However, recent studies have mainly focused on the singular function of the catalyst, i.e., either oxidation or reduction of polysulfides. As such, the goal of rapid cycling of sulfur species remains to be highly desired. Herein, a Pt-carbide composite as a bifunctional catalyst was developed to simultaneously accelerate both the reduction of soluble polysulfides and the oxidation of insoluble Li₂S/Li₂S₂. Typically, a Pt-NbC composite was synthesized by growing Pt nanoparticles on the surface of NbC, and the resultant intimate interface in the hybrid is a key component for the bifunctional catalysis. During the reduction process, polysulfides could be grabbed on the surface of NbC via strong adsorption, and then these trapped polysulfides could be catalytically converted by Pt nanoparticles. During the oxidation process, both NbC and Pt exhibited catalytic activities for the dissolution of Li₂S. This process could lead to the renewal of the surface of the catalyst. By combining the sulfur cathode with a Pt-NbC-CNT (Pt-NbC anchored on a carbon nanotube)-coated separator, the cell was able to demonstrate a high initial capacity of 1382 mAh g^-1 at a current density of 0.2C. Furthermore, the cell was able to achieve an exceptional rate capability of 795 mAh g^-1 at 5C, and it was also able to show significantly inhibited self-discharge behavior. Thus, this work explores the catalyst design and the mechanism of a bifunctional catalyst for the performance enhancement in Li-S cells.