Two-Dimensional Imide-Based Covalent Organic Frameworks with Tailored Pore Functionality as Separators for High-Performance Li–S Batteries

Modifying the separator of lithium-sulfur batteries (LSBs) is considered to be one of the most effective strategies for relieving the notorious polysulfide shuttle effect. Constructing a stable, lightweight, and effective LSB separator is still a big challenge but highly desirable. Herein, a stable and lightweight imide-based covalent organic framework (COF-TpPa) is facilely fabricated on reduced graphene oxide (rGO) through an oxygen-free solvothermal technique. With the directing effect of rGO and changing the side functional group of the monomer, the morphology and the pore tailoring of COF-TpPa can be simultaneously achieved and two-dimensional (2D) COF nanosheets with different functionalities (such as -SO₃H and -Cl) are successfully constructed on rGO films. The specific functional groups inside the COF's pore channels and the narrowed pore size result in efficient absorption and restriction of Li₂S_n for weakening the "shuttle effect". Meanwhile, the 2D COF nanosheets on the rGO is a favorable morphology for better exploiting pores inside the COF materials. As a result, the COF-SO₃H-modified separator, consisting of rGO and COF-TpPa-SO₃H, exhibits a high specific capacity (1163.4 mA h/g at 0.2 C) and a desirable cyclic performance (60.2% retention rate after 1000 cycles at 2.0 C) for LSBs. Our study provides a feasible strategy to rationally design functional COFs and boosts their applications in various energy storage systems.