Using magnetite-based nanocomposite adsorbents to remove and recycle phosphate from wastewater is crucial for controlling eutrophication and ensuring the sustainable use of phosphorus resources. However, the weak structural stability between magnetite and adsorptive nanoparticles often reduces phosphate removal efficiency in real-world applications. This instability primarily results from the loss of adsorptive nanoparticles from the magnetite surfaces, particularly when metal oxide nanoparticles are used for phosphate removal and recycling. In this study, we present a top-down approach that involves lattice locking magnesium iron oxide nanoparticles to the magnetite core, preventing magnesium loss from the magnetite surfaces. These nanocomposites exhibit exceptional performance in both phosphate recycling and removal, with a maximum adsorption capacity of 101.8 mg P·g−1. Excellent adsorption performance is also observed even in the presence of competing anions at phosphate-to-competing ion molar ratios of 1:5, 1:25, and 1:100, as well as dissolved organic matter, across a broad pH range of 4–10. The adsorbent also demonstrated minimal magnesium release during regeneration and in acidic conditions. Microscopic and spectroscopic analyses reveal that surface precipitation is the primary mechanism of phosphate removal in the magnesium-containing shells. The findings of this study address the current limitations of magnetite nanocomposites in phosphate removal, paving the way for the development of highly stable and sustainable nanocomposites for various chemical removal and recycling applications in wastewater treatment.
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