DFT Simulation-Based Design of 1T-MoS₂ Cathode Hosts for Li-S Batteries and Experimental Evaluation

The main challenge in lithium sulphur (Li-S) batteries is the shuttling of lithium polysulphides (LiPSs) caused by the rapid LiPSs migration to the anode and the slow reaction kinetics in the chain of LiPSs conversion. In this study, we explore 1T-MoS₂ as a cathode host for Li-S batteries by examining the affinity of 1T-MoS₂ substrates (pristine 1T-MoS₂, defected 1T-MoS₂ with one and two S vacancies) toward LiPSs and their electrocatalytic effects. Density functional theory (DFT) simulations are used to determine the adsorption energy of LiPSs to these substrates, the Gibbs free energy profiles for the reaction chain, and the preferred pathways and activation energies for the slow reaction stage from Li₂S₄ to Li₂S. The obtained information highlights the potential benefit of a combination of 1T-MoS₂ regions, without or with one and two sulphur vacancies, for an improved Li-S battery performance. The recommendation is implemented in a Li-S battery with areas of pristine 1T-MoS₂ and some proportion of one and two S vacancies, exhibiting a capacity of 1190 mAh/g at 0.1C, with 97% capacity retention after 60 cycles in a schedule of different C-rates from 0.1C to 2C and back to 0.1C.