Room-temperature synthesis of covalent organic frameworks with dual functional groups for high-performance adsorption of diclofenac sodium from aqueous solution

Abstract

Diclofenac sodium (DCF) are commonly found in ambient waterways due to its widespread use, and this poses significant risks to both human health and ecosystems. In this study, we have designed and synthesized a series of imine-linked covalent organic frameworks (COFs) with dual functional groups using a triple assembly strategy. Specifically, the platform molecules 2,5-dimethoxyterephthalaldehyde (DMTP), 2,5-dihydroxyterephthalaldehyde (DHTP), and 1,3,5-tris(4-aminophenyl)benzene (TAPB) were employed for the direct fabrication of COFs through Schiff base condensation reactions. As a proof of concept, three room-temperature synthesized COFs (COF TAPB-DMTP-[OH]n, where n represents the molar mass of DHTP, with n values of 0.02, 0.03, and 0.04) were used for DCF adsorption from water. The adsorption isotherms, kinetics, pH effects, ionic strength, co-existing ions, and COF regeneration for DCF were thoroughly investigated. The incorporation of methoxy (-OMe) and hydroxyl (-OH) groups serves as a functional strategy to facilitate hydrogen bonding interactions with DCF molecules. Consequently, the developed COFs, featuring an ultrahigh surface area and mesoporous structure, demonstrated a maximum adsorption capacity of 413.2mg/g and a rate constant k2 of 0.0435g/mg/min, which exceeds the performance of the majority of previously described adsorbents. The adsorption capacity toward DCF remained nearly unchanged after five regeneration cycles of the COF. Furthermore, the self-prepared adsorbent demonstrated efficient adsorption of DCF from real environmental water, indicating its potential for practical DCF removal applications.