Magnetically nanorized seaweed residue for the adsorption of methylene blue in aqueous solutions

Abstract

The cost-effective and green separation of dye pollutants from wastewater is of great importance in environmental remediation. Industrial seaweed residue (SR), as a low-cost cellulose source, was used to produce carboxylated nanorized-SR (NSR) via oxalic acid (OA)–water pretreatments followed by ultrasonic disintegration. Fourier transform infrared spectroscopy, X-ray polycrystalline diffraction, nitrogen isotherms, scanning electron microscopy, transmission electron microscopy, vibrating sample magnetometry, X-ray photoelectron spectrometry, particle charge detection, zeta potential and retro titration experiments were utilized to explore the physiochemical properties of samples. The NSRs with carboxyl content of 4.58–6.73 mmol g⁻¹ were prepared using 10–60% OA–water pretreatment. In the case of 20% OA–water pretreatment, the highest NSR yield (73.9%) and nanocellulose content (80.2%) were obtained. Through self-assembly induced by the electrostatic interaction, magnetic NSR composite adsorbents (MNSRs) were prepared with the combination of NSR and Fe₃O₄ nanoparticles (NPs). The carboxylated NSR with negative charge demonstrated good affinity for Fe₃O₄ NPs. The Fe₃O₄ NPs were perfectly microencapsulated with the NSR when the NSR/Fe₃O₄ mass ratio was higher than 1/1. The adsorption properties of the MNSR for methylene blue (MB) removal from aqueous solution were investigated. The adsorbent with NSR/Fe₃O₄ mass ratio of 1/1 (MNSR1/1) exhibited optimum performance in terms of the magnetic properties and adsorption capacity. The MNSR1/1 showed high adsorption ability in a pH ≥7 environment. According to the Langmuir fitting, the maximum adsorption capacity of MNSR1/1 for MB reached 184.25 mg g⁻¹. The adsorption of MB complies with the pseudo-second-order kinetic model. MNSR1/1 still maintained good adsorption properties after the fifth cycle of adsorption–desorption. MNSR1/1 could selectively adsorb cationic dye (i.e., MB and methyl violet) from wastewater, with hydrogen bonding and electrostatic interaction as the main force.