C9N4 and C2N6S3 monolayers as promising anchoring materials for lithium–sulfur batteries: weakening the shuttle effect via optimizing lithium bonds

The notorious polysulfide shuttle effect is a crucial factor responsible for the degradation of Li-S batteries. A good way to suppress the shuttle effect is to effectively anchor dissoluble lithium polysulfides (LPSs, Li2Sn) on appropriate substrates. Previous studies have revealed that Li of Li2Sn is prone to interact with the N of N-containing materials to form Li–N bonds. In this work, by means of density functional theory (DFT) computations, we explored the possibility to form Li bonds on ten different N-containing monolayers, including BN, C2N, C2N6S3, C9N4, a covalent triazine framework (CTF), g-C3N4, p-C3N4, C3N5, S-N2S, and T-N2S, by examining the adsorption behavior of Li2Sn (n = 1, 2, 3, 4, 6, 8) on these two-dimensional (2D) anchoring materials (AMs), and investigated the performance of the formed Li bonds (if any) in inhibiting the shuttle effect. By comparing and analyzing the nitrogen content, the N-containing pore size, charge transfer, and Li bonds, we found that the N content and N-containing pore size correlate with the number of Li bonds, and the formed Li–N bonds between LPSs and AMs correspond well with the adsorption energies of the LPSs. The C9N4 and C2N6S3 monolayers were identified as promising AMs in Li-S batteries. From the view of Li bonds, this work provides guidelines for designing 2D N-containing materials as anchoring materials to reduce the shuttle effect in Li-S batteries, and thus improving the performance of Li-S batteries.