Clay mineral weathering and contaminant dynamics in a caustic aqueous system II. Mineral transformation and microscale partitioning

Sunkyung Choi, Garry Crosson, Karl T. Mueller, Supapan Seraphin, Jon Chorover

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31 Scopus citations

Abstract

Microscopic and spectroscopic studies were conducted to assess mineral transformation processes in aqueous suspensions of illite (Il), vermiculite (Vm) and montmorillonite (Mt) that were subjected to weathering in a simulated high-level radioactive tank waste leachate (0.05 M AlT, 2 M Na+, 1 M NO3-, pH ∼14, Cs+ and Sr2+ present as co-contaminants). Time series (0 to 369 d) experiments were conducted at 298 K, with initial [Cs]0 and [Sr]0 concentrations from 10-5 to 10- mol kg-. Incongruent clay dissolution resulted in an accumulation of secondary aluminosilicate precipitates identified as nitrate-sodalite, nitrate-cancrinite and zeolite X, by molecular spectroscopy and electron microscopy (XRD, IR, NMR, SEM-EDS and TEM-EDS). Contaminant fate was dependent on competing uptake to parent clays and weathering products. TEM-EDS results indicated that high Il affinity for Cs was due to adsorption at frayed edge sites. The Il system also comprised Sr-rich aluminous precipitates after 369 d reaction time. In Mt systems, Cs and Sr were co-precipitated into increasingly recalcitrant spheroidal precipitates over the course of the experiment, whereas contaminant association with montmorillonite platelets was less prevalent. In contrast, Cs and Sr were found in association with weathered Vm particles despite the formation of spheroidal aluminosilicate precipitates that were comparable to those formed from Mt. dissolution.

Original languageEnglish (US)
Pages (from-to)4437-4451
Number of pages15
JournalGeochimica et Cosmochimica Acta
Volume69
Issue number18
DOIs
StatePublished - Sep 15 2005

ASJC Scopus subject areas

  • Geochemistry and Petrology

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