Novel MOF(Zr)-on-MOF(Ce) adsorbent for elimination of excess fluoride from aqueous solution

Herein, we used a one-pot method to fabricate a novel MOF-on-MOF adsorbent, namely MOF(Zr)-on-MOF(Ce). The adsorbent demonstrated a high maximum fluoride-ions capture capacity of 164.47 mg g^-1. The morphology, elemental distribution, pore size distribution, and thermal stability were studied using SEM-EDS, XRD, BET, and TGA. The influence of the temperature, solution pH, fluoride concentration, and coexisting ions was explored using intermittent experiments. The results suggested that MOF(Zr)-on-MOF(Ce) had a fast capture rate for fluoride. MOF(Zr)-on-MOF(Ce) maintained an excellent fluoride removal performance over a wide pH range with an initial fluoride concentration of 20 mg L^-1. The optimal effect was obtained at a pH of 4, but a high removal efficiency of 94% was maintained even at a pH of 9. Interference experiments showed that only the PO₄^3- had an adverse inhibition influence. The field experiments demonstrated that MOF(Zr)-on-MOF(Ce) can keep the safety threshold levels of fluoride in drinking water. The Langmuir and pseudo-second order kinetic models were well fitted for the defluoridation process, demonstrating that the adsorption of fluoride ions on MOF(Zr)-on-MOF(Ce) was dominated by monolayer chemisorption. With the further characterization and kinetic thermodynamic studies indicates that the removal mechanism involves ion exchange, electrostatic interactions and complexation effect.