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The transport of U- and Th-series nuclides in a sandy unconfined aquifer

Tricca, A. and Wasserburg, G. J. and Porcelli, D. and Baskaran, M. (2001) The transport of U- and Th-series nuclides in a sandy unconfined aquifer. Geochimica et Cosmochimica Acta, 65 (8). pp. 1187-1210. ISSN 0016-7037. https://resolver.caltech.edu/CaltechAUTHORS:20131119-071952813

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Abstract

A comprehensive evaluation of the transport of U, Th, Ra, and Rn nuclides of the ^(238)U- and ^(232)Th-decay series in an unconfined sandy aquifer (Long Island, NY) was conducted. Groundwater data are compared with results of a theoretical transport model of weathering of aquifer grains and interaction with surface coatings to establish relationships between the concentrations of the radionuclide activities in the water and flow line distance. The data provide estimates for geochemical parameters including weathering rates and chemical reactivities in both the vadose zone and the aquifer. A theoretical treatment of the transport is presented that considers the reaction between the water and a reactive surface layer. It is found that a model with chemical exchange between the surface layer and the water for all species is not valid, and that the effects of saturation and “irreversible” precipitation of Th is required. The water table shows a relatively wide range in U activities, the only element in the U-Th series for which vadose zone input is significant in the aquifer. High weathering of U and recoil inputs of ^(234)U to the water occur in the upper 3 m of the vadose zone, while lower weathering and removal of U from the water occur below. The deeper aquifer has variable ^(238)U activities that can be accounted for by input from the vadose zone and is not a result of non-conservative behavior. The isotopic composition of U is shown to be directly related to the recoil rate relative to the weathering rate. The wide range of ^(238)U in the aquifer waters is a reflection of diverse vadose zone inputs, showing that dispersive mixing is not a dominant effect. The higher values of δ^(234)U in the aquifer reflect the recoil/weathering input ratios from within the aquifer where the weathering rate is lower than the vadose zone. Both high U activities and high δ^(234)U values cannot be obtained in the vadose zone or within reasonable flow distances in the aquifer. Radium isotopes are found to be in exchange equilibrium with the surface layer. ^(224)Ra, ^(228)Ra, and ^(226)Ra have comparable activities throughout the aquifer. In the vadose zone, the dominant input of Ra to groundwater is weathering and recoil. As found elsewhere, the ^(222)Rn in the water is a large fraction (∼5%) of the Rn produced in the aquifer rock. This cannot be due to Ra precipitation onto surface coatings in the aquifer as supported by present weathering with Th in exchange equilibrium with the surface layer. It is found that Th is saturated in the waters under oxidizing conditions so that the weathering input is irreversibly precipitating onto surfaces. However, it is shown that under somewhat reducing conditions, Th activities are much higher and the Th/U ratio in the solution is approximately that of the rock. We propose that under oxidizing conditions the source of Rn is a surface coating enriched in ^(232)Th and ^(230)Th. This Th was precipitated in an earlier phase during rapid dissolution of readily weathered phases that contain ∼10% of the U-Th inventory of the rock, with the associated U carried away in solution. Therefore, the previously precipitated ^(230)Th and ^(232)Th produce daughter nuclides in the surface coating which are the dominant contributors of Ra and Rn to the ground water. In particular, Rn is provided by very efficient losses (by diffusion or recoil) from the surface coating. This then does not require recent, large recoil losses from the parent rock or the presence of nanopores in the rock. The first data of both long-lived ^(232)Th and short-lived ^(234)Th and ^(228)Th in ground water is reported. The Th isotope activities indicate that desorption kinetics are slow and provide the first estimate, based on field data, of the Th desorption rate from an aquifer surface. The mean residence time of Th in the surface coating is ∼3000 y while in the water it is ∼1 h. Ra is in partition equilibrium with the aquifer surface layer. However, the strong fixation of Th on surface coatings is very susceptible to changes in oxidation state as is shown by a comparison of two adjacent aquifers. This makes it difficult to define with certainty the retentive characteristics in natural systems. In general, it is shown that the distributions of naturally occurring nuclides can be used to calculate values for transport parameters that are applicable to the transport of anthropogenic nuclides.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1016/S0016-7037(00)00617-7DOIArticle
http://www.sciencedirect.com/science/article/pii/S0016703700006177PublisherArticle
Additional Information:© 2001 Elsevier Science Ltd. Received March 24, 2000; accepted in revised form November 29, 2000. This work was supported by DOE grant DE-FG07 to 96ER14700. Field support from, and discussions with, J. Naidu, D. Paquette, and R. Lagatolla at BNL are appreciated. We acknowledge the extensive comments and suggestions by the reviewers that have greatly motivated us to improve the presentation. J. J. Morgan contributed to substantial improvement of the “chemistry” parts of the manuscript. The comments by M. Hoffmann on the role of bacterial action are greatly appreciated. The Brookhaven National Laboratories kindly provided access and support. Div. Contr. No. 8649(1041). Associate editor: T. Cerlings
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-FG07 96ER14700
Other Numbering System:
Other Numbering System NameOther Numbering System ID
Caltech Division of Geological and Planetary Sciences 8649
Lunatic Asylum Lab1041
Issue or Number:8
Record Number:CaltechAUTHORS:20131119-071952813
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20131119-071952813
Official Citation:A. Tricca, G.J. Wasserburg, D. Porcelli, M. Baskaran, The transport of U- and Th-series nuclides in a sandy unconfined aquifer, Geochimica et Cosmochimica Acta, Volume 65, Issue 8, 15 April 2001, Pages 1187-1210, ISSN 0016-7037, http://dx.doi.org/10.1016/S0016-7037(00)00617-7. (http://www.sciencedirect.com/science/article/pii/S0016703700006177)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:42544
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:19 Nov 2013 15:47
Last Modified:03 Oct 2019 05:59

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