A Chemical-Free Magnetophoretic Approach for Recovering Magnetic Particles in Microalgae Removal through Magnetic Separation

Abstract

Magnetic separation can swiftly remove many substances (e.g., biomolecules, cells, and viruses) from water. In algal bloom mitigation and biomass dehydration, magnetic particles (MPs) with proper surface modifications could effectively attract and remove algae from the impaired water body. It has long been expected to recover and reuse magnetic nanoparticles or particles to reduce the algal removal cost and potential adverse effects on the environment. This study evaluated the use of a tunable magnetic field to remove algae using functionalized MPs coated with polymers: polyethyleneimine (PEI), chitosan (CTS), and cetyltrimethyl ammonium bromide (CTAB), whose recovery and reuse were examined. The results show that PEI-coated MPs and CTS-coated MPs at the coating density of 2.3 g-cationic polymers·g-MPs-1 achieved higher removal efficiencies of 88.61 ± 9.12% and 73.19 ± 0.37%, respectively, toward a model algal cell (i.e., Scenedesmus obliquus) within a 5-min separation time. In contrast, CTAB-coated MPs and pristine MPs exhibited lower removal efficiencies (47.46 ± 0.3% and 52.69 ± 0.44%, respectively). Furthermore, the removal efficiency of PEI-coated MPs was further improved to over 95% under pH 7, the highest magnetic field of 40 mT, and algogenic organic matter-free conditions. Adsorption kinetics and isotherm analysis revealed that chemical and physical interactions drive the adsorption of a monolayer of algal cells on the surface of magnetic particles. Atomic force microscopy and quartz crystal microbalance confirmed a strong adhesion force and rate between functionalized MPs and algae, which affect both algal removal efficiency and MPs recovery from algae-MPs aggregates. The extended Derjaguin−Landau−Verwey−Overbeek (EDLVO) theory predicted a strong attractive force between algae and cationic polymer-coated MPs, which supported the enhanced algal removal. Finally, almost 99% of the four MPs could be recovered from separated algae-MPs aggregates within 30 s under the strong magnetic field and exhibited excellent magnetic responsiveness and reusability in further separation cycles. This study establishes a foundation for coagulant-free algae removal and enables the potential sustainable separation processes.