Study on the accelerated carbonation of MSWI fly ash under ultrasonic excitation: CO₂ capture, heavy metals solidification, mechanism and geochemical modelling

The current carbonation technology of municipal solid waste incineration fly ash (FA) has disadvantages such as low carbon sequestration efficiency, harsh conditions, and complicated equipment. An ultrasonic chemical method coupled with wet-carbonization technology is proposed. The effects of the FA ultrasonic carbonation (UC) method on CO2 capture, heavy metals (HMs) release and solidification were investigated, and geochemical model of FA was explored. The results showed that UC improved the CO2 capture capacity, and the carbonation efficiency increased from 14.1 % to 18.8 % because the ultrasonic physical and chemical excitation improved the mass transfer efficiency and strengthened the gas-liquid-solid three-phase carbonation reaction. UC inhibited the release of Pb and Zn into the liquid phase (0.002 mg/L and 0.004 mg/L) and increased the solidification efficiency of Pb and Zn in FA (99.99 % and 100 %) because free Pb and Zn converted carbonates completely. UC FA had a single component, small particle size, high degree of homogenization, and contained slender nano-CaCO3 crystals. The acid neutralization capacities of original FA, FA4, and FA9 were 10, 8, and 3 meq/g because the carbonation reaction neutralized the alkaline substance. The content of carbonate minerals was the highest in UC FA and the pH of carbonate-minerals controlled dissolution/precipitation was mainly between 6 and 10. The HMs were in a soluble state (pH < 6) and the amphoteric HMs were affected by soluble hydroxides, the leaching concentration increasing (pH > 10). Therefore, UC FA had the potential of economical, environmentally friendly, and resource-based applications when avoiding strong acid and alkali application scenarios.