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Characterizing fluxes of trace metals related to dissolved and suspended matter during a storm event: application to a karst aquifer using trace metals and rare earth elements as provenance indicators

Caractérisation des flux des métaux en éléments tracés associés à la matière dissoute et en suspension au cours d’une crue: application à un aquifère karstique en utilisant des métaux traces et les terres rares comme indicateurs de provenance

Caracterización de los flujos de metales traza relacionados con la materia disuelta y en suspensión durante un evento de tormenta: aplicación a un acuífero kárstico usando metales traza y elementos de tierras raras como indicadores de procedencia

暴雨事件期间与溶解物质和悬浮物质相关的微量金属的通量特征描述:使用痕量金属和稀土元素作为出处指标应用于岩溶含水层

Caracterização dos fluxos de metais traços relacionados ao material dissolvido e em suspensão durante eventos de tempestade: aplicação em um aquífero cárstico usando metais traços e elementos de terras raras como indicadores de proveniência

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Abstract

The origin of suspended matter and colloids in karst aquifers during storm events is not well understood in spite of their potentially important role in the transport of poorly soluble inorganic, organic, and microbiological pollutants. This work aims to characterize the fluxes of trace metals related to dissolved and suspended matter during a storm event at the spring of a karst aquifer in the Jura Mountains in France that is mainly recharged by diffuse infiltration. Various natural tracers, including rare earth elements (REE), were used to identify the origin of the contributing dissolved and suspended fractions. The storm event was characterized by the temporally delayed arrival of two different fractions of suspended particulate matter (SPM). A first SPM peak corresponded to autochthonous conduit sediment mobilized by a piston effect at the beginning of the event. A second SPM peak, related to the arrival of allochthonous soil particulates, was characterized by elevated turbidity and high concentrations of K, Al, Fe, and Mn. In the dissolved fraction, this second SPM peak was accompanied by various poorly soluble trace elements, which were interpreted by the presence of nanoparticles and colloids (NPCs). The REE distribution patterns demonstrated that both the NPCs and the SPM were derived from soil particles whatever the storm stage. This suggests that the SPM of the first stage was reworked cave sediment from previous storms composed of residual clays and soil particles, which excludes authigenic precipitates (such as Fe-Mn oxyhydroxides and speleothems) as a significant source for autochthonous sediments.

Résumé

L’origine de la matière suspendue et des colloïdes dans les aquifères karstiques au cours des crues n’est pas bien comprise malgré leur rôle potentiellement important dans le transport de polluants inorganiqueset organiques peu solubles et polluants microbiologiques. Ce travail vise à caractériser les flux des éléments métalliques en trace liés à la matière dissoute et en suspension lors d’une crue à l’exutoire d’un aquifère karstique dans les montagnes du Jura en France, qui est principalement rechargé par infiltration diffuse. Différents traceurs naturels, y compris les terres rares (TR), ont été utilisés pour identifier l’origine des fractions dissoutes et en suspension. La crue a été caractérisée par une arrivée différée dans le temps de deux fractions différentes de matièresen suspension (MES). Un premier pic de MES correspondait au sédiment endogène du conduit mobilisé par un effet piston au début de l’événement. Un second pic de MES, associé à l’arrivée de particules exogènes, était caractérisé par une turbidité élevée et des concentrations élevées en K, Al, Fe et Mn. Dans la fraction dissoute, le second pic de MES était accompagné par différents éléments traces peu solubles, ce qui a été interprété par la présence de nanoparticules et de colloïdes (NPCs). Les modalités de distribution des MES montrent que les NPCs et MES proviennent tous les deux de particules de sol quel que soit le stade de l’événement. Cela suggère que les MES au début de l’événement proviennent de la remobilisation de sédiments déposés lors de crues précédentes, composés d’argiles résiduelles et de particules de sol, ce qui exclut des précipités endogènes (tels que des oxyhydroxydes de Fe-Mn et des spéléothèmes) comme une source significative de sédiments autochtones.

Resumen

El origen de la materia en suspensión y los coloides en los acuíferos kársticos durante los eventos de tormentas no está bien conocido a pesar de su papel potencialmente importante en el transporte de contaminantes inorgánicos, orgánicos y microbiológicos poco solubles. El objetivo de este trabajo es caracterizar los flujos de metales traza relacionados con la materia disuelta y en suspensión durante un evento de tormenta en el manantial de un acuífero kárstico en Jura Mountains en Francia, que se recarga principalmente por infiltración difusa. Se usaron varios trazadores naturales, incluidos los elementos de tierras raras (REE), para identificar el origen de las contribuciones de las fracciones disueltas y en suspensión. El evento de tormenta se caracterizó por la llegada temporalmente retrasada de dos fracciones diferentes de materia particulada en suspensión (SPM). Un primer pico de SPM correspondió a un sedimento de autóctono del conducto movilizado por un efecto de pistón al comienzo del evento. Un segundo pico de SPM, relacionado con la llegada de partículas de suelo alóctono, se caracterizó por una elevada turbidez y altas concentraciones de K, Al, Fe, y Mn. En la fracción disuelta, este segundo pico de SPM fue acompañado por varios oligoelementos poco solubles, que fueron interpretados por la presencia de nanopartículas y coloides (NPC). Los patrones de distribución REE demostraron que tanto los NPC como el SPM se derivaron de las partículas del suelo cualquiera que sea la etapa de la tormenta. Esto sugiere que el SPM de la primera etapa fue un sedimento retrabajado de tormentas previas compuesto de arcillas residuales y partículas de suelo, que excluye los precipitados autigénicos (como oxihidróxidos de Fe-Mn y espeleotemas) como fuente significativa de sedimentos autóctonos.

摘要

尽管岩溶含水层中的悬浮物质和胶体在溶解很差的无机、有机及微生物污染物搬运中可能扮演非常重要的角色,但暴雨事件期间岩溶含水层中的悬浮物质和胶体成因还不是了解的很清楚。本研究工作目的就是描述法国Jura山脉中一个主要有弥散入渗不及的岩溶含水层泉处暴雨事件期间与溶解物质和悬浮物质相关的微量金属通量的特征。各种天然示踪剂包括稀土元素用来确定溶解和悬浮物质的成因。暴雨事件的特征就是悬浮微粒物质两种不同部分的延迟达到。第一个悬浮微粒物质高峰相当于原地的通道沉积物,这个原地的通道沉积物由事件开始时的活塞效应激活。第二个悬浮微粒物质高峰与外来的土壤微粒相关,呈现的特征是浊度升高,以及K, Al, Fe和 Mn浓度升高。在溶解物质中,第二个悬浮微粒物质高峰伴随着各种溶解很差的微量元素,这些微量元素可通过纳米粒子和胶体的存在得到解译。稀土元素分布模式显示,无论在暴雨的什么阶段,纳米粒子和悬浮微粒物质都来源于土壤粒子。这表明第一阶段的悬浮微粒物质由先前的包含残余黏土和土壤颗粒的暴雨再沉积成洞穴沉积物,这些残余黏土和土壤颗粒不包括作为原地沉积物重要来源的自生沉淀物(如铁锰氢氧化合物及洞穴堆积物)。

Resumo

A origem de materiais em suspensão e coloides em aquíferos cársticos durante eventos de tempestade não é muito conhecida, apesar do seu papel potencialmente importante no transporte de poluentes inorgânicos, orgânicos e microbiológicos pouco solúveis. Este trabalho tem como objetivo principal a caracterização dos fluxos de metais traços relacionados com a matéria dissolvida e em suspensão durante eventos de tempestade em uma nascente em um aquífero cárstico nas Montanhas Jura, na França, que é principalmente recarregada por infiltração difusa. Vários traçadores naturais, incluindo elementos de terras raras (ETR) foram usados para identificar a origem das frações contribuintes dissolvidas e em suspensão. Eventos de tempestade são caracterizados pela chegada temporal de duas diferentes frações de material particulado em suspensão (MPS). O primeiro pico de MPS corresponde a um sedimento de conduto autóctone mobilizado pelo efeito pistão no inicio do evento. Um segundo pico do MPS, relacionado à chegada de partículas de solo alóctone, foi caracterizada pela turbidez elevada e altas concentrações de K, Al, Fe e Mn. Na fração dissolvida, o segundo pico de MPS foi acompanhado por vários oligoelementos pouco solúveis, que podem ser interpretados pela presença de nanopartículas e coloides (NPCs). Os padrões de distribuição dos ETR demonstraram que tantos os NPCs quanto o MPS são provenientes das partículas do solo, independentemente do estágio da tempestade. Isto sugere que o MPS do primeiro estágio foi retrabalhado em sedimentos de caverna em tempestades anteriores compostas por argilas residuais e partículas de solo, o que exclui precipitados autigênicos (como os oxi-hidróxidos de Fe-Mn e espelotemas) como fonte significativa de sedimentos autóctones.

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Acknowledgements

The authors wish to thank Bruno Régent for his indispensable collaboration during fieldwork. Christophe Loup, Nadia Crini, and Caroline Amiot are thanked for the laboratory analyses. We would also like to thank the municipality of the village of Epenoy for giving access to their drinking-water-supply station. The Jurassic Karst hydrogeological observatory is part of the INSU/CNRS national observatory for karstic aquifers, SNO KARST (http://www.sokarst.org). The present paper profited from fruitful discussions with various colleagues of this network. The constructive reviews of N. Goldscheider and an anonymous reviewer helped to improve an earlier version of the manuscript.

Funding

This work was carried out with the financial support of the Regional Council of Burgundy Franche-Comté and the French Geological Survey BRGM, which is kindly acknowledged.

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Authors and Affiliations

  1. Chrono-Environnement, UMR 6249 UBFC/CNRS, University of Burgundy Franche-Comté, 25000, Besançon, France

    Cybèle Cholet, Marc Steinmann & Sophie Denimal

  2. BRGM, University of Montpellier, 1039 rue de Pinville, 34000, Montpellier, France

    Cybèle Cholet & Jean-Baptiste Charlier

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  1. Cybèle Cholet
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  2. Marc Steinmann
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  3. Jean-Baptiste Charlier
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  4. Sophie Denimal
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Correspondence to Marc Steinmann.

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Cholet, C., Steinmann, M., Charlier, JB. et al. Characterizing fluxes of trace metals related to dissolved and suspended matter during a storm event: application to a karst aquifer using trace metals and rare earth elements as provenance indicators. Hydrogeol J 27, 305–319 (2019). https://doi.org/10.1007/s10040-018-1859-2

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  • DOI: https://doi.org/10.1007/s10040-018-1859-2

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