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Environmental Stability of Schwertmannite: A Review

Überprüfung der Umweltstabilität von Schwertmannit-A

Estabilidad ambiental de la schwertmannita - una revisión

施氏矿环境稳定性-综述

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Abstract

Schwertmannite is sensitive to changes in geochemical, thermal, and microbial conditions. Changes in aqueous pH beyond its stability, i.e. pH 2.5–4.5, triggers its transformation to jarosite or goethite in highly acidic environments (pH ≤ 2.5), depending on the availability of jarosite-directing cations (Na+, NH4+, K+, etc.), while goethite is the common stable end product at pH > 7.5. Schwertmannite with degraded morphology can stably exist for years in oxic intermediate pH environments (pH 5.5–6.5), but the presence of trace amounts of Fe(II)aq yields goethite/lepidocrocite within a few hours, especially at pH ≥ 6.5. Hematite is the sole end product at ≥ 600 °C dry heating, with goethite and ferrihydrite as intermediate phases. Siderite, maghemite, and mackinawite form in anoxic microbial conditions due to dissimilatory reduction of Fe(III) and SO42− to Fe(II) and HS−, while orpiment forms from As(V)-rich schwertmannites. Sorbed contaminants enhance schwertmannite stability by restricting Fe(II)–Fe(III) electron transfer and microbial degradation by occupying surface sites. Although Fe(III) and sorbed ion mobilization typically has negligible effects on schwertmannite transformation, complete schwertmannite-SO4 release is likely in extreme conditions, and in microbial Fe(II)aq-rich media. Dissolution–reprecipitation and solid state transformation mechanisms broadly govern schwertmannite transformation.

Zusammenfassung

Schwertmannit reagiert empfindlich auf Veränderungen der geochemischen, thermischen und mikrobiellen Bedingungen. Es ist im pH-Bereich zwischen 2,5 und 4,5 stabil. Bei Änderung des pH-Wertes der wässrigen Lösung über den Stabilitätsbereich hinaus kommt es zur Umwandlung in Jarosit oder Goethit. Im stark sauren Bereich (pH ≤ 2,5) erfolgt abhängig von der Verfügbarkeit einwertiger Kationen (Na+, NH4+, K+ usw.) eine Umwandlung in Jarosit. Bei pH-Werten über 7,5 bildet sich Goethit als stabiles Endprodukt. Schwertmannit mit gestörter Gitterstruktur kann im oxischen und intermediären pH-Milieu (pH = 5,5 bis 6,5) jahrelang stabil existieren. Wenn Fe(II)aq in Spuren vorhanden ist, entsteht allerdings Goethit/Lepidokrokit innerhalb von Stunden. Ein pH-Wert ≥ 6,5 fördert diesen Prozess. Bei trockener Erwärmung von Schwertmannit auf über + 600 °C wird es über die Zwischenphasen Goethit und Ferrihydrit in Hämatit umgewandelt. Unter anoxischen Bedingungen bilden sich aufgrund der dissimilatorischen Reduktion von Fe(III) und SO42- zu Fe(II) bzw. HS- Siderit, Maghämit und Mackinawit. Aus As(V)-reichen Schwertmanniten bildet sich Auripigment. Die Stabilität von Schwertmannit wird durch Verunreinigungen verbessert. Diese beschränken den Fe(II)-Fe(III)-Elektronentransfer und den mikrobiellen Abbau durch Besetzung von Sorptionsplätzen an der Oberfläche. Meist sind die Auswirkungen von Fe(III) sowie der Mobilisierung von sorbierten Ionen bei der Schwertmannitumwandlung vernachlässigbar, aber eine vollständige Freisetzung von Schwertmannit-SO4 ist unter extremen Bedingungen sowie in mikrobiellen Fe(II)aq-reichen Medien wahrscheinlich. Die Umwandlung von Schwertmannit erfolgt durch die Mechanismen der Auflösung und Fällung sowie der Festkörperumwandlung.

Resumen

La schwertmannita es sensible a los cambios en las condiciones geoquímicas, térmicas y microbianas. Valores de pH más allá de su estabilidad (2,5-4,5) desencadenan su transformación en jarosita o goethita en ambientes altamente ácidos (pH≤2,5), dependiendo de la disponibilidad de cationes que dirigen la jarosita (Na+, NH4+, K+, etc.), mientras que la goethita es el producto final estable común a pH>7,5. La schwertmannita con morfología degradada puede existir de manera estable durante años en ambientes de pH intermedio óxico (pH 5,5-6,5) pero la presencia de trazas de Fe(II) acuoso produce goethita/lepidocrocita en pocas horas, especialmente a valores de pH≥6,5. La hematita es el único producto final a ≥600 °C de calentamiento seco, con goethita y ferrihidrita como fases intermedias. La siderita, la maghemita y la mackinawita se forman en condiciones microbianas anóxicas debido a la reducción disimilatoria de Fe(III) y SO42- a Fe(II) y HS-, mientras que el orpimento se forma a partir de schwertmannita rica en As(V). Los contaminantes absorbidos mejoran la estabilidad de la schwertmannita restringiendo la transferencia de electrones Fe(II)-Fe(III) y la degradación microbiana al ocupar los sitios de la superficie. Aunque la movilización del Fe(III) y de iones sorbidos tiene típicamente efectos insignificantes en la transformación de la schwertmannita, la liberación completa de schwertmannita-SO4 puede ocurrir bajo condiciones extremas y en medios ricos en Fe(II) acuoso con presencia microbiana. Los mecanismos de disolución-reprecipitación y de transformación de estado sólido gobiernan ampliamente la transformación de la schwertmannita.

抽象

施氏矿对地球化学、热和微生物环境变化比较敏感。当水体pH超过它的稳定性范围时,例如pH值2.5-4.5,它将转变黄钾铁矾或在强酸环境下(pH≤2.5)转变为针铁矿,转变依赖于Na+、NH4+、K+等黄钾铁矾指向阳离子,然而针铁矿是pH>7.5时常见的最终稳定产物。形态退化施氏矿可在pH中等的氧化环境中(pH 5.5-6.5)稳定存在数年,但微量Fe(II)aq的存在,尤其是pH≥6.5时,可使之数小时内变成针铁矿/纤铁矿。赤铁矿是≥600°C干热条件下唯一产物,针铁矿和水铁矿为其中间过渡相。在缺氧的微生物作用下,铁(III)和SO 2-4 异化还原为铁(II)和HS-,会生成菱铁矿、磁赤铁矿和四方硫铁矿,而富As(V)-施氏矿则变成雌黄。通过占据反应表面以限制Fe(II)-Fe(III)电子转移和微生物降解的方式,吸附污染物提高了施氏矿的稳定性。虽然铁(III)和吸附离子活性对施底矿转化影响甚微,但极端条件和微生物富铁(II)aqi介质中的完全的施氏矿SO4释放是可能的。总体上,溶解-再沉淀和固体状态转化的机理控制着施氏矿转变。

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Acknowledgements

University Grants Commission, India and Panjab University, Chandigarh, India are acknowledged for providing financial, administrative and technical support during preparation of this article. Editors and publishers of respective journals are acknowledged to provide copyright permission to reproduce selected figures. Thanks to the reviewers for their valuable inputs to improve the manuscript.

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    Susanta Paikaray

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Paikaray, S. Environmental Stability of Schwertmannite: A Review. Mine Water Environ 40, 570–586 (2021). https://doi.org/10.1007/s10230-020-00734-2

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