Regulating the electron filling state of d orbitals in Ta-based compounds for tunable lithium‑sulfur chemistry

Abstract Building the fundamental relation between the polysulfides adsorption on cathode additives and Li S chemistry kinetics is critical for the rational design of efficient and reliable Li S batteries. Herein, we reveal that Li S chemistry kinetics can be well regulated by manipulating the electron-filling state of d orbitals in Ta2O5. The prepared S@N-Ta2O5/rGO with moderate N contents delivers the lowest polarization for LiPSs conversion and the highest specific capacity of 1252.8 mAh g−1 at 0.2C. More importantly, the theoretical analysis unravel that the enhanced electrochemical performance is mainly originated from the orbital-induced adsorption modulation. This work could offer a powerful platform to manipulate the Li S chemistry by orbital engineering for high-performance Li S batteries.