Lead-chlorine synergistic immobilization mechanism in municipal solid waste incineration fly ash (MSWIFA)-based magnesium potassium phosphate cement
Journal of Hazardous Materials(2023)
摘要
The high chlorine (Cl) and lead (Pb) content characteristics of municipal solid waste incineration fly ash (MSWIFA) pose environmental risks and hinder resource utilization. Herein, an MSWIFA-based magnesium potassium phosphate cement (MKPC) preparation strategy was developed, which allowed the MSWIFA recycling and the Pb-Cl synergistic immobilization without the washing pretreatment. The compressive strength of the resulting 10 wt% MSWIFA-based MKPC was 28.44 MPa, with over 99.2% reduction in leaching toxicity of Pb and Cl. The high-angle annular dark field scanning transmission electron microscope (HAADF-STEM) and X-ray absorption spectroscopy (XAS) analyzes showed that Pb, phosphate and Cl- formed Pb5(PO4)3Cl in MKPC. In-situ X-ray diffraction (XRD) tests showed that Pb3(PO4)2 was gradually transformed to Pb5(PO4)3Cl through a dissolution-precipitation process. The formation energy, Bader charge, charge density difference and density of states (DOS) of Pb5(PO4)3Cl were analyzed by first-principles calculations, confirming that Pb5(PO4)3Cl was more thermodynamically stable than Pb3(PO4)2 and PbCl2 and that electronic interactions between Pb-p, O-p, P-p and Cl-p orbits were the origin of Pb-Cl synergistic immobilization. This work provides a new strategy for the resource utilization of MSWIFA without washing pretreatment, and provides an in-depth understanding of the Pb-Cl synergistic immobilization mechanism.
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关键词
Municipal solid waste incineration fly ash,Magnesium potassium phosphate cement,Heavy metal,Synergistic immobilization,First-principles calculation
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