Regulation and synthesis of metal–organic frameworks through mixed-ligand strategy: A pathway to enhance adsorption of perfluoroalkyl acids

Abstract

Metal-organic frameworks (MOFs) have been regarded as extremely promising adsorbent materials, with the repetitive coordination assembly of inorganic metal ions and organic ligands constituting their reticular structure and abundant pores. Herein, a ligand mixing approach to synthesizing and regulating MOFs is provided. By mixing multiple solvents and adding modifiers, imidazole-based linkers can be prepared MOFs with mixed ligand components at room temperature. In this study, we prepared four mixed-ligand MOFs: Zn(aIM + bIM), Zn(mIM + bIM), Zn(aIM + mIM), and Zn(mIM + 2-mbIM). Series of characterizations by SEM, XRD, NMR, etc. confirmed the successful preparation of mixed-ligand MOFs, and they exhibited the different surface areas, pore sizes, and surface properties. And the adsorption capabilities for perfluoroalkyl acids (PFAAs) were compared among the prepared MOFs adsorbents. Among them, Zn(aIM + bIM) consisting of benzimidazole and imidazole-2-formaldehyde linker possessed the optimum adsorption performance, with an equilibrium adsorption capacity qe of 245 mg/g for perfluorobutyric acid, and the calculated maximum adsorption capacity qm of 439 mg/g. And for the other chain lengths of perfluoroalkyl acids, the adsorption results are also acceptable. The potential adsorption mechanism and the reasons for the performance enhancement are discussed based on relevant characterization and simulation. It was proved that the ligand mixing strategy can provide new insights into the development of high-performance MOFs adsorbents for addressing environmental concerns.