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Millennial-scale diffusive migration of solutes in thick clay-rich aquitards: evidence from multiple environmental tracers

Migration diffuse à l’échelle millénaire de solutés dans des aquitards épais riches en argile: démonstration avec traceurs environnementaux multiples

Migración difusiva a escala milenaria de solutos en acuitardos gruesos ricos en arcilla: evidencias a partir de trazadores múltiples ambientales

厚层富粘土质弱透水层中污染物千年尺度的扩散迁移: 多种环境示踪剂证据

Escala milenar da migração difusiva de solutos em aquitardos espessos ricos em argila: evidência a partir de traçadores ambientais múltiplos

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Abstract

High-resolution one-dimensional profiles of naturally occurring environmental tracers (3H, δD, δ18O, 14C-DIC, 14C-DOC, 36Cl, 4He, and major ions) and hydraulic data were used to study residence times, transport mechanisms, and sources of pore water and solutes in an aquitard system in Saskatchewan, Canada. The aquitard system consisted of 80 m of plastic clay-rich Battleford till discomformably overlying 77 m of Late Cretaceous plastic marine clay. Individual tracers independently revealed molecular diffusion as the dominant transport mechanism in the unoxidized nonfractured till and clay. Transport modeling indicated that late Pleistocene-age pore water at 35–55 m below ground was emplaced 15–30 thousand years Before Present (ka BP) during till deposition and ice retreat. The late Holocene climatic transition was estimated to have occurred 7–12 ka BP. Differences in the timing of events determined with different tracers were attributed to inaccuracies in transport parameters and boundary condition assumptions. This study showed that solute transport in clay-rich aquitards can be accurately predicted for time scales beyond 20 ka, and proved such aquitards are suitable for long-term isolation of most wastes.

Résumé

Des profils haute résolution unidimentionnels avec traceurs environnementaux naturels (3H, δD, δ18O, 14C-DIC, 14C-DOC, 36Cl, 4He, et ions majeurs) et des données hydrauliques ont été utilisés pour étudier les temps de séjour, le mécanismes de transfert et l’origine de l’eau et des solutés inclus dans les pores d’un système aquitard du Saskatchewan, Canada. L’aquitard est constitué par 80 m de tillite de Battleford riche en argile plastique, discordante sur 77 m d’argile plastique marine du Crétacé supérieur. Les traceurs indiquent chacun la diffusion moléculaire comme moyen de transport dominant dans l’argile non fracturée et non oxydée de la tillite. La modélisation du transport indique que l’eau est contemporaine du dépôt des tillites à 35–55 m de profondeur durant retrait des glaciers au Pléistocène supérieur il y a 15 à 30 ka. On estime que la transition holocène tardive s’est déroulée il y a 7 à 12 ka. Les différences dans la chronologie des évènements établie avec les traceurs ont été attribuées à des imprécisions liées aux paramètres de migration et hypothèses sur les conditions aux limites. Cette étude a montré que le transport de solutés dans des aquitards riches en argile peut être prévu avec précision pour des échelles de temps au-delà de 20 ka, prouvant que de tels aquitards conviennent pour le confinement à long terme de la plupart des déchets.

Resumen

Se usaron perfiles unidimensionales de alta resolución de trazadores ambientales que naturalmente existen (3H, δD, δ18O, 14C-DIC, 14C -DOC, 36Cl, 4He, y iones mayoritarios) y datos hidráulicos, para estudiar los tiempos de residencia, mecanismos de transporte y fuentes de agua poral y solutos en un sistema acuitardo en Saskatchewan, Canada. El sistema acuitardo consistía en 80 m del till Battleford plástico rico en arcilla que yace discordantemente sobre 77 m de arcilla plástica marina del Cretácico Tardío. Independientemente los trazadores individuales revelaron a la difusión molecular como un mecanismo de transporte dominante en el till no fracturado y no oxidado y en la arcilla. El modelado del transporte indicó que el agua poral de edad Pleistocena tardía en los 35–55 m debajo del terreno se instaló 15–30 mil años antes del presente (ka AP) durante la depositación del till y la retracción del hielo. Se estima que la transición climática del Holoceno tardío ocurrió 7–12 ka AP. Las diferencias en los tiempos de estos eventos determinados con diferentes trazadores se atribuyeron a inexactitudes en los parámetros de transporte y en las supuestas condiciones de contorno. Este estudio mostró que el transporte de soluto en acuitardos ricos en arcillas pueden ser predichos con precisión para escalas de tiempo más allá de 20 ka, y probó que tales acuitardos son apropiados para el aislamiento a largo plazo de la mayoría de los residuos.

摘要

本文用环境示踪剂 (δ3H, δD, δ18O, 14C-DIC, 14C-DOC, 36Cl, 4He和主要离子) 和水文资料的高分辨率一维剖面, 研究位于加拿大Saskatchewan省某隔水层系统的地下水驻留时间, 运移机制以及孔隙水和溶质的来源. 该弱透水层系统由80m厚塑性富粘土的Battleford 冰碛物组成, 下伏77m厚上白垩系塑性海相粘土, 二者为不整合接触. 各示踪剂单独揭示, 在未氧化和无裂隙冰碛物和粘土中, 水的主要运移机制为分子扩散. 运移模型表明, 地下35–55m处的晚更新世孔隙水为冰川退缩和漂砾沉积期 (15–30 ka BP) 形成. 全新世的气候转变期应为7–12 ka BP. 不同示踪剂定出的年龄有所差异, 其原因为运移参数和边界条件假设的不确定性. 本研究表明, 在大于20 ka的尺度上, 可以准确预测厚层粘土弱透水层中的溶质运移, 证明这类弱透水层适于大多数废物的长期隔离.

Resumo

Perfis unidimensionais de alta resolução usando traçadores que ocorrem naturalmente no ambiente [3H, δD, δ18O, 14C-CID (Carbono Inorgânico Dissolvido), 14C –COD (Carbono Orgânico Dissolvido), 36Cl, 4He, e iões principais] e dados hidráulicos foram usados para o estudo dos tempos de residência, dos mecanismos de transporte, e das origens da água dos poros e dos solutos num sistema aquitardo em Saskatchewan, no Canadá. O sistema aquitardo consiste em 80 m de sedimentos glaciares (till) de Battleford, ricos em argila plástica, sobrepondo em desconformidade 77 m de argila plástica de origem marinha do Cretácico superior. Traçadores individuais revelaram, de modo independente, a difusão molecular como o mecanismo de transporte dominante na argila e no till não fracturados e não oxidados. A modelação de transporte indicou que a água localizada nos poros entre os 35 e os 55 m é do Plistocénico superior, e terá infiltrado há cerca de 15–30 mil anos atrás, durante a deposição do till e o recuo do gelo. Estima-se que a transição climática do Holocénico superior terá ocorrido há 7–12 mil anos atrás. As diferenças na calendarização dos eventos, determinadas por diferentes traçadores, foram atribuídas a inexactidões nos parâmetros de transporte e nas assumpções das condições de fronteira. Este estudo mostrou que o transporte de solutos nos aquitardos ricos em argila pode ser previsto com precisão para escalas de tempo com mais de 20 mil anos, e provou que estes aquitardos são apropriados para o isolamento, a longo prazo, da maioria dos resíduos.

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Acknowledgements

Long-term financial support was provided by the Natural Sciences and Engineering Research Council of Canada and Cameco Co. Ltd. through the NSERC-Cameco Research Chair, the Saskatchewan Potash Producers Association, and Environment Canada. The assistance of many collaborators and students who contributed to the papers upon which this one was based is gratefully acknowledged.

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  1. Department of Geological Sciences, University of Saskatchewan, 114 Science Place, Saskatoon, SK, S7N 5E2, Canada

    M. Jim Hendry

  2. Environment Canada, 11 Innovation Blvd., Saskatoon, SK, S7N 3H5, Canada

    L. I. Wassenaar

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  1. M. Jim Hendry
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Correspondence to M. Jim Hendry.

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Hendry, M.J., Wassenaar, L.I. Millennial-scale diffusive migration of solutes in thick clay-rich aquitards: evidence from multiple environmental tracers. Hydrogeol J 19, 259–270 (2011). https://doi.org/10.1007/s10040-010-0647-4

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