2D Sandwich‐Like α‐Zirconium Phosphate/Polypyrrole: Moderate Catalytic Activity and True Sulfur Confinement for High‐Performance Lithium–Sulfur Batteries

Abstract Although lithium–sulfur batteries are promising environmentally friendly and low‐cost energy storage devices with high energy densities, many obstacles such as poor conductivity, volume expansion and the “shuttle effect” still limit their large‐scale commercialization. In this work, a 2D sandwich‐like α‐ZrP/polypyrrole (α‐ZrP/PPy) material with a nanosheet structure was designed as a sulfur host. The material can provide unique ion transfer channels for the rapid transfer of Li + ions and catalytically promote the conversion of lithium polysulfides (LiPSs). Moreover, the α‐ZrP nanosheets provides a true covalent anchor for sulfur species, whereas the PPy builds a physical barrier and forms a conductive network for accelerating the electron transport and promoting the electrochemical performance. In addition, the moderate catalytic activity and true sulfur confinement effect of α‐ZrP were confirmed by experiments and theoretical calculations. The α‐ZrP/PPy@S cathode exhibits a highly reversible capacity of 727.2 mAh g −1 even at a high current density of 5 C, offering a novel cathode material for high performance Li–S batteries.