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Title: Influence of Acidic and Alkaline Waste Solution Properties on Uranium Migration in Subsurface Sediments

Abstract

This study shows that acidic and alkaline wastes co-disposed with uranium into subsurface sediments has significant impact on changes in uranium retardation, concentration, and mass during downward migration. For uranium co-disposal with acidic wastes, significant rapid (i.e., hours) carbonate and slow (i.e., 100s of hours) clay dissolution resulted, releasing significant sediment-associated uranium, but the extent of uranium release and mobility change was controlled by the acid mass added relative to the sediment proton adsorption capacity. Mineral dissolution in acidic solutions (pH 2) resulted in a rapid (< 10 h) increase in aqueous carbonate (with Ca2+, Mg2+) and phosphate and a slow (100s of hours) increase in silica, Al3+, and K+, likely from 2:1 clay dissolution. Infiltration of uranium with a strong acid resulted in significant shallow uranium mineral dissolution and deeper uranium precipitation (likely as phosphates and carbonates) with downward uranium migration of three times greater mass at a faster velocity relative to uranium infiltration in pH neutral groundwater. In contrast, mineral dissolution in an alkaline environment (pH 13) resulted in a rapid (< 10 h) increase in carbonate, followed by a slow (10s to 100s of hours) increase in silica concentration, likely from montmorillonite, muscovite, and kaolinite dissolution. Infiltrationmore » of uranium with a strong base resulted in uranium-silicate precipitation (presumed Na-boltwoodite) but also desorption of natural uranium on the sediment due to the high ionic strength solution, or 60% greater mass with greater retardation compared with groundwater. Overall, these results show that acidic or alkaline co-contaminant disposal with uranium can result in complex depth- and time-dependent changes in uranium dissolution/precipitation reactions and uranium sorption, which alter the uranium migration mass, concentration, and velocity.« less

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1094938
Report Number(s):
PNNL-SA-96107
830403000
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Contaminant Hydrology, 151:155-175
Additional Journal Information:
Journal Name: Journal of Contaminant Hydrology, 151:155-175
Country of Publication:
United States
Language:
English
Subject:
uranium; subsurface contamination; acid waste; alkaline waste

Citation Formats

Szecsody, James E., Truex, Michael J., Qafoku, Nikolla, Wellman, Dawn M., Resch, Charles T., and Zhong, Lirong. Influence of Acidic and Alkaline Waste Solution Properties on Uranium Migration in Subsurface Sediments. United States: N. p., 2013. Web. doi:10.1016/j.jconhyd.2013.05.009.
Szecsody, James E., Truex, Michael J., Qafoku, Nikolla, Wellman, Dawn M., Resch, Charles T., & Zhong, Lirong. Influence of Acidic and Alkaline Waste Solution Properties on Uranium Migration in Subsurface Sediments. United States. https://doi.org/10.1016/j.jconhyd.2013.05.009
Szecsody, James E., Truex, Michael J., Qafoku, Nikolla, Wellman, Dawn M., Resch, Charles T., and Zhong, Lirong. 2013. "Influence of Acidic and Alkaline Waste Solution Properties on Uranium Migration in Subsurface Sediments". United States. https://doi.org/10.1016/j.jconhyd.2013.05.009.
@article{osti_1094938,
title = {Influence of Acidic and Alkaline Waste Solution Properties on Uranium Migration in Subsurface Sediments},
author = {Szecsody, James E. and Truex, Michael J. and Qafoku, Nikolla and Wellman, Dawn M. and Resch, Charles T. and Zhong, Lirong},
abstractNote = {This study shows that acidic and alkaline wastes co-disposed with uranium into subsurface sediments has significant impact on changes in uranium retardation, concentration, and mass during downward migration. For uranium co-disposal with acidic wastes, significant rapid (i.e., hours) carbonate and slow (i.e., 100s of hours) clay dissolution resulted, releasing significant sediment-associated uranium, but the extent of uranium release and mobility change was controlled by the acid mass added relative to the sediment proton adsorption capacity. Mineral dissolution in acidic solutions (pH 2) resulted in a rapid (< 10 h) increase in aqueous carbonate (with Ca2+, Mg2+) and phosphate and a slow (100s of hours) increase in silica, Al3+, and K+, likely from 2:1 clay dissolution. Infiltration of uranium with a strong acid resulted in significant shallow uranium mineral dissolution and deeper uranium precipitation (likely as phosphates and carbonates) with downward uranium migration of three times greater mass at a faster velocity relative to uranium infiltration in pH neutral groundwater. In contrast, mineral dissolution in an alkaline environment (pH 13) resulted in a rapid (< 10 h) increase in carbonate, followed by a slow (10s to 100s of hours) increase in silica concentration, likely from montmorillonite, muscovite, and kaolinite dissolution. Infiltration of uranium with a strong base resulted in uranium-silicate precipitation (presumed Na-boltwoodite) but also desorption of natural uranium on the sediment due to the high ionic strength solution, or 60% greater mass with greater retardation compared with groundwater. Overall, these results show that acidic or alkaline co-contaminant disposal with uranium can result in complex depth- and time-dependent changes in uranium dissolution/precipitation reactions and uranium sorption, which alter the uranium migration mass, concentration, and velocity.},
doi = {10.1016/j.jconhyd.2013.05.009},
url = {https://www.osti.gov/biblio/1094938}, journal = {Journal of Contaminant Hydrology, 151:155-175},
number = ,
volume = ,
place = {United States},
year = {Thu Aug 01 00:00:00 EDT 2013},
month = {Thu Aug 01 00:00:00 EDT 2013}
}