Abstract
Acid mine drainage (AMD) contains rare earth element (REE) concentrations several orders of magnitude higher than those of the rest of natural waters and could be a secondary source of REEs. In arid to semiarid climates with a long dry season, the precipitation of efflorescent sulfates constitutes a transient storage of REEs. The REE partition among the Al–Fe–Mg–Ca sulfates formed by the evaporation to dryness of six different AMDs was investigated by statistical methods and by selective dissolution. The chemical composition of the evaporitic salts showed that only three principal components (PCs) could explain more than 80% of the variability in the six samples analyzed. PC1 was associated with Ca and light REEs and interpreted as gypsum, whereas PC2 was associated with Y and heavy REEs, which were not clearly associated with a major sulfate. Finally, PC3 included Mg, Fe and several transition metals (Cu, Ni, Co, Mn and Zn) and was interpreted as Fe(II)-Mg sulfates. Selective dissolution of the salt mixtures with solutions saturated in the major sulfates revealed that the REEs were only retained in gypsum and were practically absent from the rest of the sulfates. The incorporation of REEs into gypsum decreased from Pr-Nd to La and Lu and was strictly ruled by the differences in their atomic radii and that of Ca in eight-fold coordination. However, gypsum concentrated less than 20% of the REE inventory (< 1% for Sc); the rest probably formed one or more unidentified trace minerals. This indicates that gypsum may not be an efficient way to concentrate REEs from AMD.
Zusammenfassung
Saures Grubenwasser (Acid Mine Drainage, AMD) enthält Seltene Erden (REE) in Konzentrationen, die um mehrere Größenordnungen höher sind als die der übrigen natürlichen Wässer und könnte eine sekundäre Quelle für REEs sein. In ariden bis semiariden Klimaten mit einer langen Trockenzeit stellt die Ausfällung von effloreszierenden Sulfaten eine vorübergehende Speicherung von REEs dar. Die REE-Verteilung unter den Al-Fe-Mg-Ca-Sulfaten, die durch die Verdunstung zur Trockenheit von sechs verschiedenen AMDs gebildet wurden, wurde mit statistischen Methoden und durch selektives Auflösen untersucht. Die chemische Zusammensetzung der evaporitischen Salze zeigte, dass nur drei Hauptkomponenten (PC) mehr als 80% der Variabilität in den sechs analysierten Proben erklären konnten. PC1 war mit Ca und leichten REEs assoziiert und wurde als Gips interpretiert, während PC2 mit Y und schweren REEs assoziiert war, die nicht eindeutig mit einem Hauptsulfat in Verbindung gebracht werden konnten. PC3 schließlich enthielt Mg, Fe und mehrere Übergangsmetalle (Cu, Ni, Co, Mn und Zn) und wurde als Fe(II)-Mg-Sulfate gedeutet.
Selektives Auflösen der Salzmischungen mit Lösungen, die in den Hauptsulfaten gesättigt waren, ergab, dass die REEs nur im Gips zurückgehalten wurden und in den restlichen Sulfaten praktisch nicht vorhanden waren. Der Einbau von REEs in Gips nahm von Pr-Nd zu La und Lu ab und wurde streng durch die Unterschiede in ihren Atomradien und dem von Ca in achtfacher Koordination bestimmt. Allerdings konzentrierte Gips weniger als 20 % des REE-Inventars (< 1 % für Sc); der Rest bildete wahrscheinlich ein oder mehrere nicht identifizierte Spurenminerale. Dies deutet darauf hin, dass Gips möglicherweise kein effizienter Weg ist, um REEs aus AMD zu konzentrieren.
抽象的
酸性矿井废水 (AMD) 的稀土元素 (REE) 浓度比其它天然水体高几个数量级, 有望成为稀土元素的次生来源。在干旱至半干旱气候的漫长旱季, 风化硫酸盐沉淀不断储存稀土元素。通过统计和选择性溶解方法, 研究了由六种不同酸性矿井废水 (AMD) 蒸发至干燥而成的硫酸铝-铁-镁-钙盐的稀土元素 (REE) 分离。蒸发盐的化学成分显示, 仅有的三个主成分 (PCs) 可以解释六种分析样品80%以上变化。主成分1 (PC1) 与钙 (Ca) 和轻稀土元素相关, 被解释为石膏; 主成分2 (PC2) 与钇 (Y) 和重稀土元素相关, 与主要硫酸盐关系不明确。最后, 主成分3 (PC3) 包括镁 (Mg) 、铁 (Fe) 和几种过渡金属 (铜Cu、镍Ni、钴Co、锰Mn和锌Zn), 被解释为硫酸铁 (II) -镁盐。选择性盐溶液与主要硫酸盐饱和溶液的混合揭示, 稀土元素 (REE) 只保留在石膏中, 其余硫酸盐中几乎没有。混入石膏的稀土元素 (REE) 从镨-钕到镧和镥减少, 严格由它们原子半径的不同和钙的8倍配位体的差异来决定。然而, 石膏仅浓缩了不到20%的稀土元素 (REE) 存量 (Sc < 1%), 其余形成了一种或多种不明的微量矿物。研究表明, 石膏还不是浓缩酸性矿井废水 (AMD) 中稀土元素 (REE) 的有效方法。
Resumen
El drenaje ácido de minas (DAM) contiene concentraciones de elementos de tierras raras (ETR) varios órdenes de magnitud superiores a las del resto de las aguas naturales y podría ser una fuente secundaria de ETR. En climas áridos o semiáridos con una larga estación seca, la precipitación de sulfatos eflorescentes constituye un almacenamiento transitorio de REEs. La partición de REE entre los sulfatos de Al-Fe-Mg-Ca formados por la evaporación hasta sequedad de seis DAM diferentes fue investigada por métodos estadísticos y por disolución selectiva. La composición química de las sales evaporíticas mostró que sólo tres componentes principales (PC) podían explicar más del 80% de la variabilidad en las seis muestras analizadas. La PC1 estaba asociada al Ca y a los REEs ligeros y se interpretó como yeso, mientras que la PC2 estaba asociada al Y y a los REEs pesados, que no estaban claramente asociados a un sulfato mayor. Finalmente, la PC3 incluía Mg, Fe y varios metales de transición (Cu, Ni, Co, Mn y Zn) y se interpretó como sulfatos de Fe(II)-Mg. La disolución selectiva de las mezclas de sales con soluciones saturadas en los principales sulfatos reveló que los REEs sólo se retenían en el yeso y estaban prácticamente ausentes del resto de los sulfatos. La incorporación de los REEs en el yeso disminuyó desde el Pr-Nd hasta el La y el Lu y se rigió estrictamente por las diferencias de sus radios atómicos y el del Ca en coordinación óctuple. Sin embargo, el yeso concentró menos del 20% del inventario de REE (< 1% para el Sc); el resto probablemente formó uno o más minerales traza no identificados. Esto indica que el yeso no es una forma demasiado eficiente para concentrar los REE del DAM.
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Acknowledgements
This work was funded by the European EIT-Raw Materials MORECOVERY and the Spanish SCYRE (CGL2016-78783-C2-R) projects. F. Macías was funded by the R&D FEDER Andalucía 2014-2020 programme through the project RENOVAME (FEDER; UHU-1255729). The authors thank M. Cabañas, R. Bartrolí, and N. Moreno (IDAEA-CSIC) for their analytical assistance, and two anonymous reviewers for their constructive comments.
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Ayora, C., Carrero, S., Bellés, J. et al. Partition of Rare Earth Elements Between Sulfate Salts Formed by the Evaporation of Acid Mine Drainage. Mine Water Environ 41, 42–57 (2022). https://doi.org/10.1007/s10230-021-00803-0
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DOI: https://doi.org/10.1007/s10230-021-00803-0