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Clay Minerals; September 2002; v. 37; no. 3; p. 497-508; DOI: 10.1180/0009855023730048
© 2002 Mineralogical Society of Great Britain and Ireland
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Research Paper

Tritium accumulation in structures of clay minerals

E. A. KALINICHENKO1, R. A. PUSHKAROVA2, P. FENOLL HACH-ALÍ3,* and A. LÖPEZ-GALINDO3

1 Institute of Geochemistry, Mineralogy and Ore Formation, Palladin Av. 34, 03680 Kiev, Ukraine, 2 State Scientific Centre of Environmental Radiogeochemistry, Palladin Av. 34a, 03680 Kiev, Ukraine; and 3 Instituto Andaluz de Ciencias de la Tierra. CSIC – Universidad de Granada, Avda. Fuentenueva, s/n, 18002 Granada, Spain

* E-mail: pfenoll{at}goliat.ugr.es

(Received 12 January 2001; revised 17 January 2002)

Tritium accumulation in clay minerals (kaolinite, montmorillonite, palygorskite) was studied experimentally over a one year contact with tritiated water (initial activity 1.67x109 Bq/m3) under room conditions, and was compared to theoretical calculations. The amounts of tritium ions in bound water and structural hydroxyls were measured by the activity of water fractions released at characteristic temperatures determined on the basis of the mineral DTA patterns. Experiments showed that after a 400 day contact with tritiated water, tritium exchange rates ({theta}) were highest in palygorskite ({theta}a = 0.42 in bound water and {theta}s = 0.51 in the structure) compared to montmorillonite ({theta}a = 0.15 and {theta}s = 0.11, respectively) and kaolinite ({theta}a = 0.34 and {theta}s = 0.02, respectively). This could be due to different tritium concentrations in the solution near the bound-water layers, and also to certain features of the mineral structures, most of the kaolinite structural hydroxyls not interacting directly with bound HTO molecules.

Tritium accumulation in these minerals, under room conditions, can be described by a relatively simple two-stage isotope exchange model in which tritium ions first migrate from the solution to the bound layers and then substitute the protons of the structural hydroxyls. Rate constants for both stages of this isotope exchange were calculated on the basis of the experimental data.

KEYWORDS: tritium accumulation, clay minerals, hydrogen isotope exchange kinetics and mechanisms






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