Insights into the Enhanced Tetracycline Adsorption by Two-Dimensional Cu-Based Metal–Organic Framework

Accumulation of tetracycline (TC) in aquatic environments poses a significant threat to human health and ecosystems, driving the need for efficient removal technologies. Two-dimensional metal–organic frameworks (2D MOFs) are promising adsorbents due to their tunable structures and abundant active sites. In this work, three 2D MOFs, M3(HHTP)2 (M = Cu, Ni, Co), were synthesized via a solvothermal method. Among them, Cu3(HHTP)2 exhibited superior TC adsorption with a maximum capacity of 302.84 mg/g. The adsorption process, best described by the Langmuir isotherm and pseudo-second-order kinetic models, indicates chemisorption. Mechanistic investigations reveal that the high-activity coordination sites formed by Cu2+ due to Jahn–Teller distortion enable strong coordination with TC. This is identified as the key factor governing the differential adsorption performance among the three MOFs. Simultaneously, the surface functional groups facilitate hydrogen bonding, and the advantageous pore structure of the material itself, together forming a synergistic adsorption. This work not only elucidates the microscopic mechanism behind the efficient adsorption of TC by Cu3(HHTP)2 but also, through comparative analysis of isostructural MOFs, confirms the decisive role of metal center electronic structure in modulating the adsorption behavior of 2D MOFs. The insights gained from this study may serve as a reference for the design of 2D high-performance adsorbents.