Abstract
The widespread use of imidacloprid (IMI) in pest control presents significant environmental challenges due to its persistence and low removal efficiency. This study introduces magnetic Covalent Organic Frameworks (COFs) functionalized with Fe₃O₄ nanoparticles (Fe₃O₄@HMN-COF, Fe₃O₄@MAN-COF, and Fe₃O₄@SIN-COF) as efficient adsorbents for IMI removal from water. These COFs, engineered with nitrogen-rich structures and extensive π-electron systems, achieve superior adsorption through π-π interactions, hydrophobic interactions, and hydrogen bonding. Characterization via FT-IR, XRD, and nitrogen sorption isotherms confirmed their high hydrophilicity, stability, and large surface areas. The magnetic properties of the COFs facilitated easy separation from water, enhancing practicality. Kinetic studies for all COFs indicated a pseudo-second-order model, suggesting chemisorption, with adsorption capacities of 600 mg/g for Fe₃O₄@HMN-COF, 480 mg/g for Fe₃O₄@MAN-COF, and 375 mg/g for Fe₃O₄@SIN-COF. Thermodynamic analyses revealed spontaneous and endothermic adsorption processes. Reusability tests showed minimal capacity loss over multiple cycles, underscoring their practical applicability. Practical tests in honey and fruit samples confirmed high efficacy, demonstrating the COFs' versatility. The study also optimized the photocatalytic degradation of imidacloprid using these COFs, with Fe₃O₄@HMN-COF achieving 98.5 % efficiency under optimal conditions (10 mg L(-1) IMI, 0.01 g catalyst dose, pH 11, 30 °C, UV light). These findings highlight the potential of magnetic COFs for sustainable environmental remediation of pesticide-contaminated water.