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Incorporation of Metals into Calcite in a Deep Anoxic Granite Aquifer

Journal article
Authors H. Drake
F. A. Mathurin
Thomas Zack
T. Schafer
N. M. W. Roberts
M. Whitehouse
A. Karlsson
C. Broman
M. E. Astrom
Published in Environmental Science & Technology
Volume 52
Issue 2
Pages 493-502
ISSN 0013-936X
Publication year 2018
Published at Department of Earth Sciences
Pages 493-502
Language en
Links doi.org/10.1021/acs.est.7b05258
Keywords rare-earth-elements, potential geological repository, fractured, crystalline rock, low-temperature calcite, la-icp-ms, trace-element, aqueous-solution, partition-coefficients, solution systems, stable-isotopes, Engineering, Environmental Sciences & Ecology
Subject categories Geology

Abstract

Understanding metal scavenging by calcite in deep aquifers in granite is of importance for deciphering and modeling hydrochemical fluctuations and water rock interaction in the upper crust and for retention mechanisms associated With underground, repositories for toxic wastes. Metal scavenging into calcite has generally been established in the laboratory or in natural environments that cannot be unreservedly applied to conditions in deep crystalline rocks, an environment of broad interest, for nuclear waste repositories. Here, we report a microanalytical study: of calcite precipitated over a period of 17 years from anoxic, low-temperature (14 degrees C), neutral (pH: 7.4-7.7), and brackish (Cl: 1700-7100 mg/L) groundwater flowing in fractures at >400 m depth in granite rock. This enabled assessment of the trace metal uptake by calcite under these deep-seated conditions. Aquatic speciation modeling was carried out to assess influence of metal complexation on the partitioning into calcite. The resulting environment-specific partition coefficients were for several divalent ions in line with values obtained in controlled laboratory experiments, whereas for several other ions they differed substantially. High absolute uptake of rare earth elements and U(IV) suggests that coprecipitation into calcite can be an important sink for these metals and analogousactinides in the vicinity of geological repositories.

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