Hydrogen‐Bonded Organic Framework to Upgrade Cycling Stability and Rate Capability of Li‐CO2 Batteries

Abstract Elaborately designed multifunctional electrocatalysts capable of promoting Li + and CO 2 transport are essential for upgrading the cycling stability and rate capability of Li‐CO 2 batteries. Hydrogen‐bonded organic frameworks (HOFs) with open channels and easily functionalized surfaces hold great potential for applications in efficient cathodes of Li‐CO 2 batteries. Herein, a robust HOF S (HOF‐FJU‐1) is introduced for the first time as a co‐catalyst in the cathode material of Li‐CO 2 batteries. HOF‐FJU‐1 with cyano groups located periodically in the pore can induce homogeneous deposition of discharge products and accommodate volumetric expansion of discharge products during cycling. Besides, HOF‐FJU‐1 enables effective interaction between Ru 0 nanoparticles and cyano groups, thus forming efficient and uniform catalytic sites for CRR/CER. Moreover, HOF‐FJU‐1 with regularly arranged open channels are beneficial for CO 2 and Li + transport, enabling rapid redox kinetic conversion of CO 2 . Therefore, the HOF‐based Li‐CO 2 batteries are capable of stable operation at 400 mA g −1 for 1800 h and maintain a low overpotential of 1.96 V even at high current densities up to 5 A g −1 . This work provides valuable guidance for developing multifunctional HOF‐based catalysts to upgrade the longevity and rate capability of Li‐CO 2 batteries.