Catalytic performance of graphene doped with M@S1N3 for lithium-sulfur batteries

Lithium-sulfur batteries represent a potential energy storage to alternative traditional lithium-ion batteries, yet the sluggish kinetics of the sulfur reduction reaction (SRR) currently hinders their practical application. To improve the reaction kinetics of Li-S batteries, it is necessary to research and develop high-activity catalysts. For example, single-atom catalysts (SACs) can promote the redox process of Li 2 S and slow down the “shuttle effect” of polysulfides . Based on the experimentally synthesized and widely used Fe@S 1 N 3 doped graphene material, this work systematically calculated the catalytic properties of M@S 1 N 3 (M = Sc, Ti, Cr, Fe, Co, Ni, Cu, Zn, Y, Zr, and Ru) doped grahpenes as the cathode material . The results show that S-metal chemical has a key role in the adsorption and activation on SACs. Furthermore, the kinetics of the lithiation process and the behaviour during Li 2 S delithiation are compared for each SAC to find materials with promising applications in charge/discharge process. Finally, it found that Ru@S 1 N 3 has the best cycling performance among the calculated materials and the highest catalytic activity, which is closest to the ideal electrocatalysts . This study presents a detailed computational analysis lithium polysulfides (LiPS S ) adsorption and conversion on the SAC cathode, as a guide for the experimental development of efficient catalysts. Ru@S 1 N 3 has the limiting potential closest to the ideal value for the adsorption of *LiS, with a relatively low calculated energy barrier for Li 2 S decomposition. Electronic structure analysis reveals that the modulation mechanism of each SAC is mainly based on S-metal bonding.