A Theoretical Study of Porphyrin‐Based Covalent Organic Framework as an Effective Catalytic Material for Li‐S Batteries—A Comparative Study of Sulfur Reduction Reaction

ABSTRACT The creation of effective cathode materials remains a significant obstacle to the advancement of Lithium‐Sulfur (Li‐S) battery technology. Nowadays, Covalent Organic Frameworks (COFs) are used to anchor electrodes in Li‐S batteries due to their high pore size and self‐design ability. Identifying the ideal anchoring electrodes that effectively restrain the shuttle effect and slow redox reaction is still in the pioneering stage. Therefore, the systematic investigation of the porphyrin‐based COFs with the species Li 2 S n ( n = 1, 2, 4, 6, and 8) through density functional theory (DFT) calculations is taken into account. The key aspect of the study includes the calculation of adsorption energy, charge transfer, electronic properties, diffusion, and Sulfur Reduction Reaction (SRR). In order to study the shuttle effect, the long‐chain polysulfides has been incorporated with the solvent where, the interaction enhances their stabilization, as indicated by the variation in adsorption behavior. Also, the lower Gibbs free energy of SRR indicates a thermodynamically favorable conversion of S 8 to Li 2 S. Consequently, these insights highlight the catalytic efficiency of porphyrin‐based COFs for improving performance in Li‐S batteries.