Hydrogen‐Bonded Organic Framework Derived 2D N, O Co‐Doped Carbon Nanobelt with Tunable Pseudocapacitive Contribution for Efficient Capacitive Deionization

Abstract Defect engineering is recognized as an attractive method for modulating the electronic structure and physicochemical characteristics of carbon materials. Exploiting heteroatom‐doped porous carbon with copious active sites has attracted great attention for capacitive deionization (CDI). However, traditional methods often rely on the utilization of additional heteroatom sources and strong corrosive activators, suffering from low doping efficiency, insufficient doping level, and potential biotoxicity. Herein, hydrogen‐bonded organic frameworks (HOFs) are employed as precursors to synthesize N, O co‐doped porous carbon via a simple and green reverse defect engineering strategy, achieving controllable heavy doping of heteroatoms. The N, O co‐doping triggers significant pseudocapacitive contribution and the surface pore structure supports the formation of the electric double layer. Therefore, when HOF‐derived N, O co‐doped carbon is used as CDI electrodes, a superior salt adsorption capacity of 32.29 ± 1.42 mg g −1 and an outstanding maximum salt adsorption rate of 10.58 ± 0.46 mg g −1 min −1 at 1.6 V in 500 mg L −1 NaCl solution are achieved, which are comparable to those of state‐of‐the‐art carbonaceous electrodes. This work exemplifies the effectiveness of the reverse nitrogen‐heavy doping strategy on improving the carbon structure, shedding light on the further development of rational designed electrode materials for CDI.