This study investigated whether a combined application of hydroxyapatite and ferrihydrite could immobilize lead and antimony in shooting range soil in which the level of lead contamination is markedly higher than that of antimony. In addition, we evaluated the stability of lead and antimony immobilized by the combined application with varying soil pH. The levels of water-soluble lead and antimony for the combined application were lower than those of single applications of hydroxyapatite or ferrihydrite, indicating that the combined application could suppress the levels of water-soluble lead and antimony by 99.9% and 95.5%, respectively, as compared with the levels in shooting range soil without immobilization material. The amounts of residual lead and amorphous Fe/Al oxide-bound antimony fractions in sequential extraction increased with a decrease in the exchangeable and carbonate lead fractions as well as in non-specifically bound and specifically bound antimony fractions. The alteration of lead and antimony phases to chemically more stable ones as a result of the combined application would result in the suppression of their mobility. The stability of immobilized lead and antimony in the combined application was equal to that of lead with a single application of hydroxyapatite and that of antimony with a single application of ferrihydrite within neutral to alkaline pH conditions, respectively. Therefore, this study suggests that the combined application of hydroxyapatite and ferrihydrite can simultaneously immobilize lead and antimony in shooting range soil with neutral to alkaline pH.

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This study combined the original unsaturated-column-percolation test with X-ray diffraction (XRD) analysis to understand how lead is transformed into lead-insoluble phase and immobilized by hydroxyapatite during lead migration in the water-unsaturated soil of different lead mobilities. The amounts of lead migrated from the soils without hydroxyapatite ranged from 4 to 46%, depending on the lead mobilities of soils. On the other hand, those of soils with hydroxyapatite were greatly suppressed by > 95% as compared with those without hydroxyapatite. The XRD analysis showed that the amounts of lead transformed into pyromorphite were compatible with those of lead migrated from the soil irrespective of the different lead mobilities. To the best of our knowledge, this study provides the first experimental evidence that lead migration can induce lead to transform into pyromorphite in the water-unsaturated soil. In addition, this study quantitatively demonstrates that the amount of lead migrated is almost equal to that of lead formed into pyromorphite. Thus, it was found that even if soluble lead remains after the application of immobilization material, it would be immobilized by the material during the lead migration as long as adequate material is applied to the soil.

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