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This study investigates and compares arsenic, As(V), removal from aqueous media using the water-stable zinc metal−organic frameworks (Zn-MOF-74) prepared via room-temperature precipitation (RT-Zn-MOF-74) and a solvothermal procedure (HT-Zn-MOF-74). The Zn-MOF-74 crystals possess average particle sizes of 66 nm and 144 μm for RT-Zn-MOF-74 and HT-Zn-MOF-74, respectively. Moreover, nanosized RT-Zn-MOF-74 exhibited a superior performance to HT-Zn-MOF-74. While the Brunauer− Emmett−Teller surface area of RT-Zn-MOF-74 was smaller than that of HT-Zn-MOF-74, higher adsorption uptake took place on the room-temperature-synthesized ones because of their small particle size and better dispersion. Adsorption isotherm studies showed that the Langmuir isotherm was effective for the adsorption of As(V) onto RT-Zn-MOF-74 and HT-Zn-MOF-74 with maximum adsorption uptake (q max ) values of 99.0 and 48.7 mg g −1 , respectively. These values exceed most reported maximum adsorption capacities at neutral pH. The thermodynamics of adsorption revealed a spontaneous endothermic process that is due to the substitution of adsorbed water molecules by arsenate in the pores of the MOF crystal. This was further investigated using plane-wave density functional theory calculations. This study constitutes direct evidence for the importance of tuning the size of the MOF crystals to enhance their properties.

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