Investigation of the Nanocrystal CoS2 Embedded in 3D Honeycomb-like Graphitic Carbon with a Synergistic Effect for High-Performance Lithium Sulfur Batteries

摘要

Lithium sulfur (Li-S) batteries can offer great opportunities for the next-generation energy storage systems with tremendous energy density. However, challenges still exist in practical Li-S batteries including low sulfur utilization, and poor cycling stability and rate capability. Herein, we propose a novel hybrid catalyst structure by in situ implanting nanocrystal CoS2 in three-dimensional honeycomb-like hierarchical porous graphitic carbon (HPGC) for high-performance Li-S batteries. A unique synergistic absorption-catalysis-functional effect is demonstrated by comprehensive experimental and theoretical analysis: strong physical and chemical co-absorption effects are originated from the large quantity of microporous HPGC and the polar surface of metallic CoS2; the introduced nanocrystal CoS2 with a large specific area can impose an exceptional catalytic effect on the liquid-liquid, solid-liquid, and solid-solid phase redox reactions in Li-S batteries; the reaction dynamics are further guaranteed by the multifunctional properties of the HPGC backbone, including the capabilities in polysulfide sustention, reaction product transportation, electrolyte compensation, and efficiency in assisting diverse electrochemical reaction dynamics. In this way, our results not only develop a novel CoS2@HPGC structure, but also provide fundamental understanding on the catalytic dynamics during each reaction process. Moreover, we further propose the necessity and philosophy of the rational design of catalysts' special structure, which can fulfill the functional dynamics requirements of Li-S batteries, and can be promoted to other Li-S-related cathode design and composite catalytic structure design.