Conductive 1D Metal–Organic Frameworks DDA‐X (DDA = Hexacoordinated 1,5‐Diamino‐4,8‐Dihydroxy‐9,10‐Anthraceneedione, X = Co, Ni, and Cu) for Highly Efficient Sulfur Redox Kinetics in Lithium–Sulfur Batteries: A Density‐Functional Theory Study

Lithium–sulfur batteries (LiSBs) are considered as the prominent candidates for next‐generation energy storage systems. However, the commercial applications of LiSBs are impeded by shuttling effect and sluggish conversion kinetics of the lithium polysulfides (LiPSs). Herein, it is proposed that the 1D metal–organic framework (1D MOF) DDA‐X (DDA = hexacoordinated 1,5‐diamino‐4,8‐dihydroxy‐9,10‐anthraceneedione, X = Co, Ni, and Cu) can be a potential sulfur host material for LiSBs. Through the first‐principles calculations, it is revealed that the DDA‐X with excellent electronic conductivity mitigates the insulating properties of S‐based electrodes. Because of the significant synergistic effect based on the XS bond and the LiN bond, the DDA‐X can intensely interact with LiPSs and substantially prevent soluble LiPSs species into the electrolyte. Particularly, the battery with the DDA‐Co cathode has excellent electrocatalytic activity for the redox reaction of LiPSs, which has low Gibbs free energy barriers (0.398 eV) and Li 2 S decomposition energy barriers (1.45 eV) during the charge–discharge cycle, and it is due to the upshift of the d‐band center of Co in DDA‐Co. Through these findings, the application of the 1D MOF materials in high‐performance LiSBs is facilitated.