Rational Design of Metal-Doped Graphitic Materials for Enhanced Lithium–Sulfur Batteries

Atomically dispersed metal atoms within graphitic carbon have shown great potential in enhancing the performance of lithium–sulfur batteries (LSBs), though the fundamental principles to guide their rational design remain to be fully established. Here, we report a combined computational and experimental study demonstrating that a group of metals (Ti, V, Mo, and Nb) incorporated into graphitic carbon have promising catalytic properties due to three factors: strong binding with lithium sulfides, reduced redox overpotentials, and low kinetic barriers for Li–S bond activation. In contrast, metals such as Fe and Mn show moderate catalytic behavior, while Ni representing a third group of elements has worse performance. To validate these computational predictions, we synthesized and studied three representative metal elementsNb, Fe, and Nieach exhibiting distinct capabilities in binding LiPSs/Li2S and catalyzing polysulfide conversion with varying overpotentials and kinetic barriers. Among them, Nb delivered the most exceptional performance, including superior rate capability (679.3 mA h g–1 at 5 C), high capacity retention (837.5 mA h g–1), and a low capacity decay rate (0.023% per cycle) after 500 cycles at 1 C. This work demonstrates an effective strategy that combines theoretical screening and experimental validation in exploring atomically dispersed metal catalysts for LSBs.