Effect of aggregation behavior on microplastic removal by magnetic Fe₃O₄ nanoparticles

Magnetic nanotechnologies have been shown to be an efficient approach to the reduction of microplastic (MP) pollution in aquatic environments. However, uncertainties remain regarding the relationship between particle stability and MP removal under varying water conditions, hindering the practical application of magnetic nanotechnologies for MP removal. Herein, the influence of particle aggregation behavior on nano-scale MP removal by Fe₃O₄ nanoparticles (FNPs) was investigated, by monitoring dynamic light scattering parameters and analyzing the microstructures of particle aggregates. Results showed that 83.1 %-92.9 % of MPs could be removed by FNPs within 1 h, and MP removal exhibited a high degree of Pearson correlation (R = 0.95; P = 0.04) with particle aggregation behavior mediated by the FNPs dosage. Furthermore, pH-dependent electrostatic interactions significantly influenced particle aggregation behavior and the removal of MPs. Under pH <6.7 conditions, electrostatic attraction between electropositive FNPs and electronegative MPs led to charge neutralization-induced aggregation and efficient removal MP performance. Under increasingly saline conditions, compression of the electrical double layer enhanced the self-aggregation behavior of MPs, weakening the electrostatic repulsion between FNPs and MPs under alkaline conditions. Therefore, salinity improved the MP removal efficiency, especially under alkaline conditions, with MP removal increasing from 4.47 % to 55.1 % when the mass fraction of NaCl was increased from 0 % to 1 %. These findings further our understanding of the effect of aggregation behavior on MP removal by FNPs and highlight the potential for magnetic nanotechnology application in the removal of nano-scale MPs from aquatic environments, while also providing valuable insights for the design of FNP-based materials.