Defects Engineering of Lightweight Metal–Organic Frameworks-Based Electrocatalytic Membrane for High-Loading Lithium–Sulfur Batteries

Abstract

The sluggish kinetics and shuttle effect of lithium polysulfide intermediates are the major issues that retard the practical applications of lithium-sulfur (Li-S) batteries. Herein, we introduce a defect engineering strategy to construct a defected-UiO-66-NH₂-4/graphene electrocatalytic membrane (D-UiO-66-NH₂-4/G EM) which could accelerate the conversion of lithium polysulfides in high sulfur loadings and low electrolyte/sulfur (E/S) ratio Li-S batteries. Metal-organic frameworks (UiO-66-NH₂) can be directionally chemical engraved to form concave octahedra with abundant defects. According to electrocatalytic kinetics and DFT calculations studies, the D-UiO-66-NH₂-4 architecture effectively provides ample sites to capture polysulfides <i>via</i> strong chemical affinity and effectively delivers electrocatalytic activity of polysulfide conversion. As a result, a Li-S battery with such an electrocatalytic membrane delivers a high capacity of 12.3 mAh cm^-2 (1013 mAh g^-1) at a sulfur loading up to 12.2 mg·_S cm^-2 under a lean electrolyte condition (E/S = 5 μL mg^-1-sulfur) at 2.1 mA cm^-2 (0.1 C). Moreover, a prototype soft package battery also exhibits excellent cycling stability with a maintained capacity of 996 mAh g^-1 upon 100 cycles.