A three-component magnetic material, namely, Fe3O4@SiO2@CaSiO3, which featuring an Fe3O4@SiO2 core and a layered porous CaSiO3 shell, was synthesized via precipitation and utilized as an adsorbent to remove Ag+ from wastewater. The structure, morphology, composition, and magnetic properties of this material were analyzed by a series of characterization techniques, and its adsorption efficiency, adsorption thermodynamics, kinetic characteristics, and recyclability were investigated in detail. The magnetic Fe3O4@SiO2@CaSiO3 composite possessed a core–shell structure, with a cotton-like morphology, a specific surface area of 75.97 m2·g−1, pore size of 11.4 nm, pore volume of 0.36 cm3·g−1, and magnetization saturation of 60.5 emu·g−1. The adsorption equilibrium data of Ag+ adsorption by Fe3O4@SiO2@CaSiO3 fitted the Redlich–Peterson model well, and the equilibrium adsorption capacity of the material for Ag+ reached 127.84 mg·g−1 at an initial concentration of 225 mg·L−1 and temperature of 293 K. Kinteic studies showed that the adsorption process conformed well to the pseudo-second-order model and reached equilibrium within 150 min. The adsorption process was endothermic, with an activation energy of 8.475 kJ·mol−1 and accompanied by AgO bonding and Ca2+ release. Therefore, the adsorption mechanism involved in Ag+ removal includes not only physisorption and ion exchange but also chemisorption, which is controlled by surface OH and O groups. The percentage of Ag+ removal tended to stabilize after five cycles of Fe3O4@SiO2@CaSiO3 reuse and but decreased by only 14.34%. Synthesized Fe3O4@SiO2@CaSiO3 exhibited excellent adsorption, regeneration, and magnetic separation performance. Thus, the synthesized Fe3O4@SiO2@CaSiO3 may potentially be applied to remove Ag+.
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