The heterointerface effect to boost the catalytic performance of single atom catalysts for sulfur conversion in lithium-sulfur batteries.

Lithium-sulfur (Li-S) batteries are considered as one of the promising next-generation energy storage devices due to their characteristics of high energy density and low cost. However, the shuttle effect and sluggish conversion of lithium polysulfide (LiPs) have hindered their commercial applications. To address these issues, in our previous works, we have screened several highly efficient single atom catalysts (SACs) (MN 4 @G, M = V, Mo and W) with atomically dispersed transition metal atoms supported by nitrogen doped graphene based on high throughput calculations. Nevertheless, they still suffer from low loading of metal centers and unsatisfactory capability for accelerating the reaction kinetics. To tackle such problems, based on first-principles calculations, we systematically investigated the heterointerface effect on the catalytic performance of such three MN 4 @G toward sulfur conversion upon forming heterostructures with 5 typical two-dimensional materials of TiS 2 , C 3 N 4 , BN, graphene and reduced graphene oxide. Guided by efficient descriptors proposed in our previous work, we screened VN 4 @G/TiS 2 , MoN 4 @G/TiS 2 and WN 4 @G/TiS 2 possessing low Li 2 S decomposition barriers of 0.54, 0.44 and 0.41 eV, respectively. They also possess enhanced capabilities for catalyzing the sulfur reduction reaction as well as stabilizing soluble LiPs. More interestingly, the heterointerface can enhance the capability of the carbon atoms far away from the metal centers for trapping LiPs. This work shows that introducing a heterointerface is a promising strategy to boost the performance of SACs in Li-S batteries.