Journal
CHEMICAL GEOLOGY
Volume 564, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.chemgeo.2020.120054
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Funding
- College of Arts and Sciences (Strategic Research Initiative Seed Fund)
- Department of Geosciences (MSU)
- Laboratory Directed Research and Development (LDRD) program of Los Alamos National Laboratory (LANL) [20180007DR]
- National Nuclear Security Administration of the U.S. Department of Energy [89233218CNA000001]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
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This study evaluated the immobilization of uranium in calcite under varied redox conditions, finding that tetravalent uranium was absorbed by calcite at a higher rate than hexavalent uranium by up to four orders of magnitude. It was estimated that a few milligrams of calcite crystallization under reduced hydrothermal conditions could immobilize all dissolved uranium in a UO2-saturated solution.
This work evaluated the immobilization of uranium (U) through incorporation into calcite under reduced and oxidized conditions. We investigated how much U could be entrapped by calcite crystallizing in chloride solutions in autoclaves at temperatures from 162 to 300 degrees C. The oxidation state of U was set by controlling oxygen fugacity via redox buffers. Uranium was introduced into calcite growth media as a solid oxide compound or U aliquot. We found the uptake of tetravalent U by calcite is higher than that of hexavalent U by up to four orders of magnitude. We estimate that crystallization of a few mg of calcite immobilizes all dissolved U when 1 kg of solution is saturated with UO2 under reduced hydrothermal conditions.
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