Lithium Polysulfide Catalytic Mechanism of AlN/InN Heterojunction by First-Principles Calculation

To solve the shuttling effect and transformations of LiPSs in lithium–sulfur batteries, heterostructures have been designed to immobilize LiPSs and boost their reversible conversions. In this paper, we have constructed AlN/InN heterojunctions with AlN with a wide band gap and InN with a narrow band gap. The heterojunctions show metallic properties, which are primarily composed of 2s, 2p N atoms and 5s, 5p In atoms. InN has relatively higher adsorptivity for LiPSs than AlN. Reaction profiles show that on the surface of AlN, there is a lower rate-limiting step than on that of InN, from S8 to Li2S6, and a higher rate-limiting step from Li2S4 to Li2S2, which is more favorable for InN during the reduction from Li2S4 to Li2S2. The heterojunction can realize the synergistic reaction of trapping–diffusion–conversion for LiPSs, in which AlN traps large Li2S8 and Li2S6, the heterojunction causes the diffusion of Li2S4, and InN completes the conversion of Li2S4 to Li2S.