Covalent integration of electroactive β-ketoenamine COFs with amino-functionalized CNTs for efficient capacitive deionization

Covalent organic frameworks (COFs) are attractive electrode candidates for capacitive deionization (CDI), but their practical use is often restricted by sluggish electron transport and the limited accessibility of redox-active units. In this work, electroactive β $\beta$ -ketoenamine COF domains were covalently integrated with amino-functionalized carbon nanotubes (CNTs), producing a conductive core–shell hybrid with intimate interfacial coupling. Benefiting from the thin COF shell, the conductive CNT backbone, and the chemically anchored interface, the optimized electrode achieves a salt adsorption capacity of 87.38 mg g −1 and maintains stable regeneration behavior, outperforming the pristine COF and CNT controls. Electrochemical measurements and density functional theory (DFT) calculations indicate that the covalent COF/CNT junction redistributes interfacial charge, improves electronic communication, and decreases the barrier for Na + migration. These results highlight covalent interfacial integration as an efficient route for activating redox COFs and developing high-performance metal-free CDI electrodes. Download: Download high-res image (372KB) Download: Download full-size image