Pilot-scale natural carbonation of waste paper fly ash for stabilization of Ba and Pb

The increase in energy valorization of paper sludge and biomass waste through incineration results in a rise in waste paper fly ash (WPFA), often perceived as hazardous and requiring specific treatment. In this study, natural carbonation technology at a pilot scale was employed to mitigate the hazardous nature of WPFA by enhancing the stabilization of metal and metalloid trace elements (MMTE), particularly barium (Ba) and lead (Pb) leaching. Natural carbonation of WPFA was found to be optimal at a water/solid ratio of 0.3 L/kg under natural temperature and humidity conditions. Batch leaching tests based on thermodynamic equilibrium were used to assess MMTE solubility concerning pH in both non-carbonated and carbonated WPFA at natural pH. After 7 days of natural carbonation, the leaching concentration of Ba and Pb was below the legal limit in France. The concentration of Ba and Pb in carbonated samples decreased by 98.5% and 98%, respectively. Analyses using thermogravimetry, X-ray diffraction, scanning electron microscopy, and energy-dispersive spectroscopy demonstrated the increased formation and quantity of calcite (CaCO₃) with longer carbonation times, along with the formation of new minerals as BaCO₃ and PbCO₃, confirming the immobilization of these elements post-carbonation. The leaching behavior and release potential of carbonated WPFA were further evaluated using the four-stage sequential extraction procedure proposed by the European Commission’s Bureau of Reference (BCR). The speciation of Ba and Pb shifted significantly from the soluble substance (F1) at 17.6% and 14.8%, respectively, to the carbonate fraction (F2) at 0.49% and 0.02% after 90 days of carbonation. The percolation water collected during the carbonation process adheres to discharge standards into the sea.