Sequestration of Sr-90 Subsurface Contamination in the Hanford 100-N Area by Surface Infiltration of a Ca-Citrate-Phosphate Solution

Szecsody, James E. ; Rockhold, Mark L. ; Oostrom, Martinus ; Moore, R. C. ; Burns, Carolyn A. ; Williams, Mark D. ; Zhong, Lirong ; Fruchter, Jonathan S. ; McKinley, James P. ; Vermeul, Vincent R. ; Covert, Matthew A. ; Wietsma, Thomas W. ; Breshears, Andrew T. ; Garc

关键词: APATITES;    BIODEGRADATION;    BUILDUP;    CITRATES;    CONTAMINATION;    DRAINAGE;    FLOW RATE;    GEOPHYSICS;    RIVERS;    SEDIMENTS;    SORPTION;    SPATIAL DISTRIBUTION;    TRANSPORT;    WATER;    WATER INFLUX Sr-90 in sediments;    Hanford 100N;    Ca-citrate-PO4 infiltration;    remediation;    Environmental Molecular Sciences Laboratory;   

DOI  :  10.2172/985589
RP-ID  :  PNNL-18303
PID  :  OSTI ID: 985589
Others  :  Other: 23593
Others  :  830403000
Others  :  TRN: US201112%%125

学科分类：地球科学(综合)

美国|英语

来源: SciTech Connect

【 摘 要 】

The objective of this project is to develop a method to emplace apatite precipitate in the 100N vadose zone, which results in sorption and ultimately incorporation of Sr-90 into the apatite structure. The Ca-citrate-PO4 solution can be infiltrated into unsaturated sediments to result in apatite precipitate to provide effective treatment of Sr-90 contamination. Microbial redistribution during solution infiltration and a high rate of citrate biodegradation for river water microbes (water used for solution infiltration) results in a relatively even spatial distribution of the citrate biodegradation rate and ultimately apatite precipitate in the sediment. Manipulation of the Ca-citrate-PO4 solution infiltration strategy can be used to result in apatite precipitate in the lower half of the vadose zone (where most of the Sr-90 is located) and within low-K layers (which are hypothesized to have higher Sr-90 concentrations). The most effective infiltration strategy to precipitate apatite at depth (and with sufficient lateral spread) was to infiltrate a high concentration solution (6 mM Ca, 15 mM citrate, 60 mM PO4) at a rapid rate (near ponded conditions), followed by rapid, then slow water infiltration. Repeated infiltration events, with sufficient time between events to allow water drainage in the sediment profile can be used to buildup the mass of apatite precipitate at greater depth. Low-K heterogeneities were effectively treated, as the higher residual water content maintained in these zones resulted in higher apatite precipitate concentration. High-K zones did not receive sufficient treatment by infiltration, although an alternative strategy of air/surfactant (foam) was demonstrated effective for targeting high-K zones. The flow rate manipulation used in this study to treat specific depths and heterogeneities are not as easy to implement at field scale due to the lack of characterization of heterogeneities and difficulty tracking the wetting front over a large subsurface area. However, the use of real-time surface and cross-borehole geophysics can be used to track the infiltrating Ca-citrate-PO4 front so some adjustments can be made in the infiltration rate to precipitate apatite in desired zones. In addition, the reactive transport code used in this study with field scale physical parameters for sediments can be used to evaluate infiltration strategies along with preliminary water infiltration tests at field scale.