Regeneration can effectively restore the adsorption capacity of adsorbents, enabling sustainable adsorption–desorption–adsorption cycles to be maintained. The regeneration of waste adsorbents has been extensively documented. However, there is few research on the adsorption properties and the mechanism after regeneration. The regeneration of aluminum-based phosphorus-inactivation agent (Al-PIA) and recovery of phosphate from Al-PIA were achieved in the previous study. Therefore, this study determined the mechanism and effects of Al-PIA recycling on phosphate removal, following regeneration for 30 min using 0.75 mol/L hydrochloric acid. Results show that the rate of adsorption by regenerated aluminum-based phosphorus-inactivation agent (Re-Al-PIA) was faster within the first 15 h, reaching equilibrium at around 50 h, with the rate-determining step being intraparticle diffusion. The adsorption saturation concentration of Re-Al-PIA was 6.92 mg/g, with phosphate adsorption occurring via a spontaneous, heat-absorbing, and chaotic process. Regeneration restored the phosphate removal capacity of Al-PIA. Al-PIA maintained its initial phosphate adsorption capacity after three cycles. The phosphate removal mechanisms of Re-Al-PIA were physical adsorption, electrostatic adsorption, surface precipitation, and ligand exchange. Regeneration provided favorable physical conditions for phosphate adsorption, enhancing the electrostatic adsorption capacity of the material while also restoring surface precipitation and ligand exchange for phosphate removal. These results can provide theoretical basis and technical support for the practical application of Al-PIA regeneration and a reference method for regeneration of the other phosphate removal materials.
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