High-Entropy MXene as Bifunctional Mediator toward Advanced Li–S Full Batteries

Abstract

The development of high-energy-density Li-S batteries (LSBs) is still hindered by the disturbing polysulfide shuttle effect. Herein, with clever combination between "high entropy" and MXene, an HE-MXene doped graphene composite containing multiple element quasi-atoms as bifunctional mediator for separator modification (HE-MXene/G@PP) in LSBs is proposed. The HE-MXene/G@PP offers high electrical conductivity for fast lithium polysulfide (LiPS) redox conversion kinetics, abundant metal active sites for efficient chemisorption with LiPSs, and strong lipophilic characteristics for uniform Li⁺ deposition on lithium metal surface. As demonstrated by DFT theoretical calculations, in situ Raman, and DRT results successively, HE-MXene/G@PP efficiently captures LiPSs through synergistic modulation of the cocktail effect and accelerates the LiPSs redox reaction, and the lattice distortion effect effectively induces the homogeneous deposition of dendritic-free lithium. Therefore, this work achieves excellent long-term cycling performance with a decay rate of 0.026%/0.031% per cycle after 1200 cycles at 1 C/2 C. The Li||Li symmetric cell still maintains a stable overpotential after 6000 h under 40 mA cm^-2/40 mAh cm^-2. Furthermore, it delivers favorable cycling stability under 7.8 mg cm^-2 and a low E/S ratio of 5.6 μL mg^-1. This strategy provides a rational approach to resolve the sulfur cathode and lithium anode problems simultaneously.