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.