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

作者：Sun, Da; Zhou, Jianbin; Rao, Dewei; Zhu, Linqin; Niu, Shuwen; Cai, Jinyan; Fang, Yanyan; Liu, Yun; Liu, Xinmiao; Zang, Yipeng; Wu, Yishang; Xie, Yufang; Zhu, Zixuan; Niu, Di; Lu, Zheng; Pei, Zhibin^*; Wang, Gongming^*

来源：Sustainable Materials and Technologies, 2021, 28: e00271.

DOI：10.1016/j.susmat.2021.e00271

• Li-S batteries
• Doping
• Electron filling state
• Electrocatalysts
• Transition metals

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.

• 单位
  江苏大学