In this work, a new hydrogel poly(2-hydroxyethyl methacrylate-co-polyethylene glycol methacrylate-co-itaconic acid) poly(HEMA-PEG6MA-IA) covalently crosslinked with Fe3O4 nanoparticles functionalized with 3-(trimethoxysilyl)propyl methacrylate organosilane (TMSPM) was prepared by free radicals, named Fe3O4-TMSPM/HG. FTIR-ATR, TGA, XRD, and TEM experiments were utilized to explore the Fe3O4-TMSPM/HG nanocomposite hydrogel. Swelling studies were also carried out in water, in different pH media, and then used in the adsorption of the cationic dye methylene blue (MB) from aqueous media. The factors controlling the adsorption process such as pH, dose, contact time, initial MB concentration, and temperature were investigated. The maximum MB adsorption capacity (270.27 mg/g) using Fe3O4-TMSPM/HG was obtained under the best conditions pH 8, dose 0.5 mg/mL, contact time 24 h, and ambient laboratory temperature (≈15 °C). The kinetic and isothermal experiments showed that the adsorption of MB followed the pseudo-second-order and Langmuir models. The effect of temperature on the adsorption capacity is related to the swelling, since the Fe3O4-TMSPM/HG nanocomposite hydrogel exhibit temperature-responsive. After 5 adsorption–desorption cycles, the adsorption decreased by 19 mg/g compared to the initial adsorption capacity. All the experimental results show that the prepared Fe3O4-TMSPM/HG nanocomposite hydrogel has the potential to be applied as an adsorbent for MB dye.
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