Layered double Hydroxides-MXene heterointerfaces with abundant anion vacancies expediting sulfur redox kinetics for High‑Performance Lithium–Sulfur batteries

Abstract

Lithium-sulfur batteries (LSBs) are increasingly seen as advanced battery systems of great promise, owing to their exceptional energy density and cost-effectiveness. Yet, designing efficient electrocatalysts that can both effectively mitigate the diffusion of soluble lithium polysulfides (LiPSs) and enhance redox kinetics still remains a significant challenge, particularly at high sulfur loadings and lean electrolyte conditions. In this work, we develop NiCo-layered double hydroxides (NiCo-LDHs) nanosheets featuring abundant oxygen vacancies (Vo), anchored on Ti3C2-MXene nanosheets (denoted as Vo-LDHs-MXenes), tailored specifically for high-performance LSBs. The heterointerfaces between MXenes and Vo-LDHs modify the electronic structure and enhance the catalytic activity of the LDHs and MXenes, yielding multifunctional synergistic effects. Our theoretical and electrochemical analyses indicate that the Vo-LDHs-MXenes heterostructures exhibit enhanced affinity for LiPSs and superior catalytic performances compared to individual LDHs. This improvement facilitates the efficient adsorption and conversion of LiPSs, as well as the nucleation and decomposition of Li2S. Consequently, the cell with the Vo-LDHs-MXenes modified separator delivers stable cycling performances with a high initial specific capacity of 938.9 mAh/g over 300cycles at 1.0C and good rate capabilities. Notably, it still achieves a high initial areal capacity of 6.09 mAh cm−2 under a high sulfur loading of 6.7 mg cm−2 and low electrolyte/sulfur (E/S) ratio of 6.0 μL mg−1 over 50cycles.