CO2 mineralization is a promising technology to achieve a waste-to-resource chain by integrating CO2 sequestration and alkaline solid waste utilization. Amino acids as a multifunctional reagent was proposed to avoid the extensive consumption of acid and alkaline reagents in traditional processes. However, the detailed interaction between Ca-bearing minerals and amino acids are still not fully understood, as well as migration pathways of metal impurities. To fill these gaps, this paper investigated the leaching and carbonation behaviors of Ca2+ and metal impurities of a typical coal fly ash (CFA) at various reagent types, reagent concentrations and leaching temperatures, thereby exploring the fate of these metal impurities. Results showed that the leaching and carbonation of Ca2+ was influenced by various aspects such as initial pH, reagent pKa, complexation, and pH buffering. The CaCO3 products obtained from glycine (Gly) and alanine (Ala) were vaterite due to the stabilizing effect of these amino acids on vaterite preventing it from converting to calcite. The optimal reaction conditions were 1.0 M Gly and leaching temperature of 35 °C with 26.63 % leaching efficiency, 56.08 % carbonation efficiency, and 42.6 g/kg vaterite yield. In addition, Ala induced an unexpected high leaching efficiency of Cd (75.79 %), Pb (76.08 %), and Zn (41.62 %), respectively, indicating promising mitigation of the environment risk of leached residue and valuable metal recovery from CFA. Although Gly displayed limited metal leaching efficiency at 1.0 M and 25 °C, increasing leaching temperature induced a remarkable enhancement of Cd and Pb leaching, which were 88.54 % and near 100 % at 35 °C, indicating promising mitigation of the environment risk of leached CFA. However, the high binding affinity of amino acids to impurity metals led to the low purity of CaCO3 product. This study derives the migration pathways of various metal ions during the mineralization and utilization of CFA, making it of great significance for the resource management and utilization of solid wastes.
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