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硫化物诱导酸性矿山排水中铁猛矿中铬的再分配:影响和机制。

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

机构信息

School of Chemistry and Environmental Engineering, Hanshan Normal University, Chaozhou 521041, China.

The Ministry of Education Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters, School of Environment and Energy, South China University of Technology, Guangzhou 510006, China.

出版信息

Sci Total Environ. 2022 Nov 20;848:157863. doi: 10.1016/j.scitotenv.2022.157863. Epub 2022 Aug 4.

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 SO 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 and ∼1.58 to ∼0.12 mg L 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, FeS), iron oxides (FeO, FeO), 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.

摘要

铁硫循环通常与水铁矿的形成和命运有关,水铁矿特别适合作为酸性矿山排水 (AMD) 中重金属和类金属的清除剂。然而,S(-II)与结构内并入的 Cr(VI)之间的相互作用仍然难以捉摸。本工作通过结合 XRD、SEM、FTIR、TEM 和 XPS 表征的溶解实验,提供了有关 S(-II)改变 pH 值、Cr 负载和 S(-II)浓度后诱导水铁矿转化的详细信息。我们的结果发现,硫化物的存在显著降低了酸性条件下水铁矿的稳定性。三种水铁矿样品的反应活性取决于结构内并入的 Cr(VI)含量,并遵循 Sch > 0.13Cr-Sch > 0.17Cr-Sch 的顺序。高浓度的 S(-II)和低浓度的 Cr 掺杂有利于 Fe 和 SO 从水铁矿中释放。通过提高 S(-II)浓度和 pH 值,降低了 Cr 的迁移率,导致 0.13Cr-Sch 和 0.17Cr-Sch 的 Cr 浓度分别为约 1.39 至约 0.10mg/L 和约 1.58 至约 0.12mg/L。结合表征结果,针铁矿是主要的次生相,与硫化物矿物 (FeS、FeS)、铁氧化物 (FeO、FeO) 和 CrFe 矿物一起构成了块状矿物表面。取代的 Cr 显著抑制了硫化物对水铁矿的还原转化,并导致纤铁矿的形成。因此,我们得出结论,一个由三个阶段组成的转化机制控制了水铁矿向针铁矿的部分转化。这一发现为受还原物质影响的铁矿物生物地球化学过程提供了新的认识,这些还原物质控制着 AMD 污染区中固定污染物的迁移和归宿。

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