Abstract
At a test site consisting of a storage pond and connected artificial aquifer, the long-time behaviour of gadopentetic acid (Gd-DTPA) was compared with the classic tracer bromide (Br–) in a 70-day dual-tracer experiment. The mixed tracer solution was injected into the oligotrophic pond, which is separated from the aquifer by an infiltration bank. The water drained from the aquifer was returned to the pond together with additional fresh groundwater, causing reduced concentrations of Gd-DTPA and Br– in the system. Transmetallation of Gd-DTPA by rare earth elements and yttrium was negligible but Cu2+ and Ni2+ might have played a role. Adsorption and/or biodegradation of Gd-DTPA were negligible. The decline of Gd-DTPA/Br ratios by 18% in the pond over 68 days was caused by reversible sorption of Br– in the aquifer, which caused variation of Br– background. Thus, Br– behaves less conservatively than Gd-DTPA in the aquifer. Comparison of both proves the suitability of Gd-chelates as tracers in hydrological studies. The advantage of Gd-DTPA as a tracer is that natural Gd3+ in water can continuously be monitored by analysing the suite of naturally occurring rare-earth elements. Thus, stable organic Gd-chelates are determinable with high precision at very low concentrations.
Résumé
Sur un site test constitué d’un bassin de rétention connecté à un aquifère artificiel, le comportement long terme de l’acide gadopentetic (Gd-DTPA) a été comparé avec le traceur classique Brome (Br-) au cours d’une expérience traçage double de 70 jours.
On a injecté les traceurs dans le bassin oligotrophe, séparé de l’aquifère par une berge perméable. L’eau drainée de l’aquifère était retournée dans le bassin avec un de l’eau douce additionnelle, causant une réduction de la concentration de Gd-DTPA et Br- dans le système. La substitution de GD-DTPA par des terres rares et yttrium était négligeable mais Cu2+ et Ni2+ peuvent avoir joué un rôle. L’adsorption et/ou la biodegradation de Gd-DTPA étaient négligeables. Le déclin des rations Gd-DTPA/Br jusqu’à 18% dans le bassin en 68 jours a été causée par l’adsorption réversible de Br- par l’aquifère, qui a provoqué une variation du fond Br-. Ainsi, Br- se comporte moins conservativement que Gd-DTPA dans l’aquifère. La comparaison des deux montre que les chélates de Gd sont des traceurs appropriés aux études hydrogéologiques. L’avantage de Gd-DTPA en tant que traceur est que le GD3+ peut être contrôlé de façon continue en analysant le cortège des terres rares naturellement présentes dans l’eau. Ainsi, les chélates organiques stables de Gd sont analysables avec haute précision à des concentrations très basses.
Resumen
En un sitio de prueba que consistió en una laguna de almacenamiento y un acuífero artificial conectado, se comparó el comportamiento a largo plazo del ácido gadopentético (Gd-DTPA) con el trazador clásico bromuro (Br-) en un experimento de trazador doble durante 70 días. La solución mixta de trazador se inyecta en la laguna oligotrófica, la cual está separada del acuífero por un banco de infiltración. El agua drenada desde el acuífero fue devuelta a la laguna conjuntamente con agua dulce subterránea adicional, reduciendo las concentraciones de Gd-DTPA y de Br– en el sistema. La transmetalación de Gd-DTPA por elementos de tierras raras e ytrio fue despreciable, pero Cu2+ y Ni2+ podría haber jugado un papel importante. La adsorción y/o biodegradación del Gd-DTPA fueron despreciables. La reducción de las relaciones Gd-DTPA/Br en un 18% en la laguna durante 68 días fue producida por la adsorción reversible de Br– en el acuífero, lo que causó la variación del Br– de fondo. Por lo tanto, el Br– se comporta de forma menos conservadora que el Gd-DTPA en el acuífero. La comparación de ambos prueba la adecuación de los quelatos de Gd como trazadores en los estudios hidrológicos. La ventaja de Gd-DTPA como trazador es que el Gd3+ natural en el agua puede ser monitoreado continuamente mediante el análisis de la secuencia de elementos de las tierras raras que ocurren naturalmente. Por lo tanto los quelatos de Gd estables orgánicamente pueden ser determinados con alta precisión en concentraciones muy bajas.
Resumo
Num ensaio de campo consistindo numa lagoa de armazenamento com ligação hidráulica a um aquífero artificial foi comparado o comportamento, ao longo do tempo, do ácido gadopentético (Gd-DTPA) com o marcador clássico brometo (Br–), numa experiência de duplo traçador, num período de 70 dias. A solução mista marcadora foi injectada numa lagoa oligotrófica, a qual se encontrava separada do aquífero por um banco infiltrante. A água drenada do aquífero foi devolvida para a lagoa com um adicional de água doce subterrânea, provocando a redução das concentrações de Gd-DTPA e Br– no sistema. A transmetalação de Gd-DTPA por elementos de terras raras e ítrio foi insignificante, mas o Cu2+ e o Ni2+ podem ter desempenhado um papel relevante. A adsorção e/ou biodegradação de Gd-DTPA foram insignificantes. O declínio de 18% nos índices Gd-DTPA/Br na lagoa após 68 dias foi causado pela sorção reversível do Br– no aquífero, o que causou variação do Br– de fundo. Assim, o Br– manifesta um comportamento menos conservador do que Gd-DTPA no aquífero. A comparação de ambos comprova a adequação de quelatos de Gd como traçadores em estudos hidrológicos. A vantagem do Gd-DTPA como marcador é que o Gd3+ natural na água pode ser monitorizado continuamente através da análise do conjunto de elementos de terras raras de ocorrência natural. Assim, os quelatos orgânicos estáveis de Gd são determináveis com alta precisão em concentrações muito baixas.
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Acknowledgements
The authors thank the German Environmental Protection Agency for assisting in the fieldwork and Schering AG for providing Gd-DTPA. The assistance of E. Püringer and B. Richert during sampling, and C. Wiesenberg and B. Zander for preparation of the waters for ICP-MS measurements, is greatly appreciated. We also acknowledge the constructive comments of F. Elbaz-Poulichet, L. Leduc and an anonymous reviewer.
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Dulski, P., Möller, P. & Pekdeger, A. Comparison of gadopentetic acid (Gd-DTPA) and bromide in a dual-tracer field experiment. Hydrogeol J 19, 823–834 (2011). https://doi.org/10.1007/s10040-011-0713-6
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DOI: https://doi.org/10.1007/s10040-011-0713-6