Interfacial synergy in twinborn CoS₂/CoS_1.097 heterojunction to promote sulfur conversion kinetics in lithium-sulfur batteries

The rational design of sulfur hosts is essential for mitigating the shuttle effect of lithium polysulfides (LiPSs) and improving the sluggish conversion kinetics of sulfur during multi-step phase transition. Herein, twinborn CoS₂/CoS_1.097 heterojunctions encapsulated in N-doped hollow carbon polyhedrons and in-situ generated CNTs (CoS₂/CoS_1.097@NC/CNT) were elaborately synthesized and utilized as the electrocatalysts in sulfur cathodes. The CoS₂/CoS_1.097 heterojunction provides abundant chemisorption sites that facilitate the formation of chemical bonds with polysulfides, thereby effectively adsorbing LiPSs. More importantly, the spontaneously generated internal electric field at the CoS₂/CoS_1.097 interface accelerates electron transfer, which promotes the reversible transformation between LiPSs and Li₂S. Additionally, the hollow carbon polyhedrons and grafted CNTs not only effectively confine sulfur, but also provide extra buffer space for the sulfur evolution reaction. Benefiting from these characteristics, the battery assembled with CoS₂/CoS_1.097@NC/CNT/S cathode exhibits a remarkable initial capacity of 1454.4 mAh g⁻¹ at 0.1C, excellent rate capability of 674.7 mAh g⁻¹ at 4C, and outstanding capacity retention of 604.7 mAh g⁻¹ over 500 cycles at 2C (∼73.1 % of initial capacity).