Sulfide-induced repartition of chromium associated with schwertmannite in acid mine drainage: Impacts and mechanisms

Abstract

The cycling of Fe/S is often related to the formation and fate of schwertmannite which is particularly suitable as a scavenger for heavy metals and metalloids in acid mine drainage (AMD). However, the interactions between reactivity of S(-II) and schwertmannite with structurally incorporated Cr(VI) remain elusive. This work evaluated dissolution experiments in combination with XRD, SEM, FTIR, TEM, and XPS characterization to provide detailed information regarding the transformation of schwertmannite induced by S(-II) following changes in pH, Cr loading, and S(-II) concentration. Our results found that the presence of sulfide significantly decreased the stabilization of schwertmannite under acidic conditions. The reactivity of the three schwertmannite samples depended on the contents of Cr(VI) that were structurally incorporated and followed the order Sch > 0.13Cr-Sch > 0.17Cr-Sch. High S(-II) concentrations and low Cr doping favored the release of Fe and SO42− from schwertmannite. Attenuation of Cr mobility occurred via elevating the S(-II) concentrations and pH values resulting in Cr concentrations spanning ∼1.39 to ∼0.10 mg L−1 and ∼1.58 to ∼0.12 mg L−1 for 0.13Cr-Sch and 0.17Cr-Sch, respectively. Combining the results of characterization, goethite was the dominant end product constituted secondary phase together with sulfide minerals (FeS, FeS2), iron oxides (Fe3O4, Fe2O3), and CrFe minerals on the bulk mineral surface. The substituted Cr significantly inhibited the reductive transformation of schwertmannite by sulfide and led to the formation of lepidocrocite. Thus, we concluded that a three-stage transformation mechanistic pathway governed partial conversion of schwertmannite to goethite. This finding provides new understanding of the biogeochemical processes of iron minerals affected by reducing substances that control the transport and fate of immobilizing contaminants in an AMD-polluted area.