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

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. (C) 2021 Elsevier B.V. All rights reserved.