A computational study on bifunctional 1T-MnS with an adsorption-catalysis effect for lithium-sulfur batteries

• Published in: Physical chemistry chemical physics : PCCP 2023-08, Vol.25 (3), p.2546-2556
• Main Authors: Duan, Shaorong, Liu, Mingyi, Cao, Chuanzhao, Liu, Haitao, Ye, Meng, Duan, Wenhui
• Format: Article
• ISSN: 1463-9076; 1463-9084
• DOI: 10.1039/d3cp01633a

Lithium-sulfur (Li-S) batteries are promising rechargeable energy storage systems with a high energy density, environmental friendliness and low cost. However, the commercialization process of Li-S batteries has been seriously hindered by the shuttling of lithium polysulfides (LiPSs) and the sluggish kinetics of conversion reaction among sulfur species. In this work, the adsorption-catalysis performance of five transition metal disulfide 1T-MS 2 (M = Mn, V, Ti, Zr, and Hf) surfaces is investigated by evaluating the adsorption energy of sulfur species, Li-ion diffusion energy barrier, decomposition energy barrier of Li 2 S, and the Gibbs free energy barrier of the sulfur reduction reaction based on first-principles calculations. Our results show that the sulfiphilicity of 1T-MS 2 plays an important role in the adsorption behavior of short-chain sulfur species, in addition to lithiophilicity. Remarkably, among the five 1T-MS 2 materials, our results confirm that 1T-TiS 2 and 1T-VS 2 show excellent adsorption-catalysis performance and it is predicted that 1T-MnS 2 is an even better candidate catalyst to inhibit the shuttle effect and accelerate delithiation/lithiation kinetics. Moreover, the outstanding performance of 1T-MnS 2 persists in a solvent environment and under strain modulation. Our results not only demonstrate that 1T-MnS 2 is an excellent potential catalyst for high-performance Li-S batteries, but also provide great insights into the adsorption-catalysis mechanism during the cycling process. 1T-MnS 2 exhibits excellent adsorption-catalysis activity for Li-S batteries, which can enhance the adsorption for polysulfides and accelerate the oxidation of Li 2 S and sulfur reduction reaction.