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Title: Saturated Zone Colloid Transport

Abstract

This scientific analysis provides retardation factors for colloids transporting in the saturated zone (SZ) and the unsaturated zone (UZ). These retardation factors represent the reversible chemical and physical filtration of colloids in the SZ. The value of the colloid retardation factor, R{sub col} is dependent on several factors, such as colloid size, colloid type, and geochemical conditions (e.g., pH, Eh, and ionic strength). These factors are folded into the distributions of R{sub col} that have been developed from field and experimental data collected under varying geochemical conditions with different colloid types and sizes. Attachment rate constants, k{sub att}, and detachment rate constants, k{sub det}, of colloids to the fracture surface have been measured for the fractured volcanics, and separate R{sub col} uncertainty distributions have been developed for attachment and detachment to clastic material and mineral grains in the alluvium. Radionuclides such as plutonium and americium sorb mostly (90 to 99 percent) irreversibly to colloids (BSC 2004 [DIRS 170025], Section 6.3.3.2). The colloid retardation factors developed in this analysis are needed to simulate the transport of radionuclides that are irreversibly sorbed onto colloids; this transport is discussed in the model report ''Site-Scale Saturated Zone Transport'' (BSC 2004 [DIRS 170036]). Although itmore » is not exclusive to any particular radionuclide release scenario, this scientific analysis especially addresses those scenarios pertaining to evidence from waste-degradation experiments, which indicate that plutonium and americium may be irreversibly attached to colloids for the time scales of interest. A section of this report will also discuss the validity of using microspheres as analogs to colloids in some of the lab and field experiments used to obtain the colloid retardation factors. In addition, a small fraction of colloids travels with the groundwater without any significant retardation. Radionuclides irreversibly sorbed onto this fraction of colloids also transport without retardation. The transport times for these radionuclides will be the same as those for nonsorbing radionuclides. The fraction of nonretarding colloids developed in this analysis report is used in the abstraction of SZ and UZ transport models in support of the total system performance assessment (TSPA) for the license application (LA). This analysis report uses input from two Yucca Mountain Project (YMP) analysis reports. This analysis uses the assumption from ''Waste Form and In-Drift Colloids-Associated Radionuclide Concentrations: Abstraction and Summary'' that plutonium and americium are irreversibly sorbed to colloids generated by the waste degradation processes (BSC 2004 [DIRS 170025]). In addition, interpretations from RELAP analyses from ''Saturated Zone In-Situ Testing'' (BSC 2004 [DIRS 170010]) are used to develop the retardation factor distributions in this analysis.« less

Authors:
Publication Date:
Research Org.:
Yucca Mountain Project, Las Vegas, Nevada (US)
Sponsoring Org.:
US Department of Energy (US)
OSTI Identifier:
839520
Report Number(s):
ANL-NBS-HS-000031, REV 02
DOC.20041008.0007, DC41517; TRN: US0502957
DOE Contract Number:
AC28-01RW12101
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: 7 Oct 2004
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; AMERICIUM; COLLOIDS; FILTRATION; FRACTURES; LICENSE APPLICATIONS; MICROSPHERES; PERFORMANCE; PLUTONIUM; RADIOACTIVITY; RADIOISOTOPES; TESTING; TRANSPORT; WASTES; YUCCA MOUNTAIN

Citation Formats

H. S. Viswanathan. Saturated Zone Colloid Transport. United States: N. p., 2004. Web. doi:10.2172/839520.
H. S. Viswanathan. Saturated Zone Colloid Transport. United States. doi:10.2172/839520.
H. S. Viswanathan. Thu . "Saturated Zone Colloid Transport". United States. doi:10.2172/839520. https://www.osti.gov/servlets/purl/839520.
@article{osti_839520,
title = {Saturated Zone Colloid Transport},
author = {H. S. Viswanathan},
abstractNote = {This scientific analysis provides retardation factors for colloids transporting in the saturated zone (SZ) and the unsaturated zone (UZ). These retardation factors represent the reversible chemical and physical filtration of colloids in the SZ. The value of the colloid retardation factor, R{sub col} is dependent on several factors, such as colloid size, colloid type, and geochemical conditions (e.g., pH, Eh, and ionic strength). These factors are folded into the distributions of R{sub col} that have been developed from field and experimental data collected under varying geochemical conditions with different colloid types and sizes. Attachment rate constants, k{sub att}, and detachment rate constants, k{sub det}, of colloids to the fracture surface have been measured for the fractured volcanics, and separate R{sub col} uncertainty distributions have been developed for attachment and detachment to clastic material and mineral grains in the alluvium. Radionuclides such as plutonium and americium sorb mostly (90 to 99 percent) irreversibly to colloids (BSC 2004 [DIRS 170025], Section 6.3.3.2). The colloid retardation factors developed in this analysis are needed to simulate the transport of radionuclides that are irreversibly sorbed onto colloids; this transport is discussed in the model report ''Site-Scale Saturated Zone Transport'' (BSC 2004 [DIRS 170036]). Although it is not exclusive to any particular radionuclide release scenario, this scientific analysis especially addresses those scenarios pertaining to evidence from waste-degradation experiments, which indicate that plutonium and americium may be irreversibly attached to colloids for the time scales of interest. A section of this report will also discuss the validity of using microspheres as analogs to colloids in some of the lab and field experiments used to obtain the colloid retardation factors. In addition, a small fraction of colloids travels with the groundwater without any significant retardation. Radionuclides irreversibly sorbed onto this fraction of colloids also transport without retardation. The transport times for these radionuclides will be the same as those for nonsorbing radionuclides. The fraction of nonretarding colloids developed in this analysis report is used in the abstraction of SZ and UZ transport models in support of the total system performance assessment (TSPA) for the license application (LA). This analysis report uses input from two Yucca Mountain Project (YMP) analysis reports. This analysis uses the assumption from ''Waste Form and In-Drift Colloids-Associated Radionuclide Concentrations: Abstraction and Summary'' that plutonium and americium are irreversibly sorbed to colloids generated by the waste degradation processes (BSC 2004 [DIRS 170025]). In addition, interpretations from RELAP analyses from ''Saturated Zone In-Situ Testing'' (BSC 2004 [DIRS 170010]) are used to develop the retardation factor distributions in this analysis.},
doi = {10.2172/839520},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Thu Oct 07 00:00:00 EDT 2004},
month = {Thu Oct 07 00:00:00 EDT 2004}
}

Technical Report:

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  • The purpose of the Saturated Zone Colloid-Facilitated Transport Analysis and Modeling Report (AMR), as outlined in its Work Direction and Planning Document (CRWMS M&O 1999a), is to provide retardation factors for colloids with irreversibly-attached radionuclides, such as plutonium, in the saturated zone (SZ) between their point of entrance from the unsaturated zone (UZ) and downgradient compliance points. Although it is not exclusive to any particular radionuclide release scenario, this AMR especially addresses those scenarios pertaining to evidence from waste degradation experiments, which indicate that plutonium and perhaps other radionuclides may be irreversibly attached to colloids. This report establishes the requirementsmore » and elements of the design of a methodology for calculating colloid transport in the saturated zone at Yucca Mountain. In previous Total Systems Performance Assessment (TSPA) analyses, radionuclide-bearing colloids were assumed to be unretarded in their migration. Field experiments in fractured tuff at Yucca Mountain and in porous media at other sites indicate that colloids may, in fact, experience retardation relative to the mean pore-water velocity, suggesting that contaminants associated with colloids should also experience some retardation. Therefore, this analysis incorporates field data where available and a theoretical framework when site-specific data are not available for estimating plausible ranges of retardation factors in both saturated fractured tuff and saturated alluvium. The distribution of retardation factors for tuff and alluvium are developed in a form consistent with the Performance Assessment (PA) analysis framework for simulating radionuclide transport in the saturated zone. To improve on the work performed so far for the saturated-zone flow and transport modeling, concerted effort has been made in quantifying colloid retardation factors in both fractured tuff and alluvium. The fractured tuff analysis used recent data and interpretation from the C-wells reactive tracer testing complex in the saturated zone of Yucca Mountain. As no data regarding colloid transport have been developed by the Yucca Mountain Site Characterization Project (YMP) for the alluvial system, a theoretical analysis based on studies performed in other alluvial systems is developed. The parameters derived in this AMR are developed in a manner consistent with the PA methodology and can be readily integrated into that analysis.« less
  • Colloid retardation is influenced by the attachment and detachment of colloids from immobile surfaces. This analysis demonstrates the development of parameters necessary to estimate attachment and detachment of colloids and, hence, retardation in both fractured tuff and porous alluvium. Field and experimental data specific to fractured tuff are used for the analysis of colloid retardation in fractured tuff. Experimental data specific to colloid transport in alluvial material from Yucca Mountain as well as bacteriophage field studies in alluvial material, which are thought to be good analogs for colloid transport, are used to estimate attachment and detachment of colloids in themore » alluvial material. There are no alternative scientific approaches or technical methods for calculating these retardation factors.« less
  • The main purpose of this project was to improve the fundamental mechanistic understanding and quantification of long-term colloid mobilization and colloid-facilitated transport of radionuclides in the vadose zone, with special emphasis on the semi-arid Hanford site. While we focused some of the experiments on hydrogeological and geochemical conditions of the Hanford site, many of our results apply to colloid and colloid-facilitated transport in general. Specific objectives were (1) to determine the mechanisms of colloid mobilization and colloid-facilitated radionuclide transport in undisturbed Hanford sediments under unsaturated flow, (2) to quantify in situ colloid mobilization and colloid-facilitated radionuclidetransport from Hanford sediments undermore » field conditions, and (3) to develop a field-scale conceptual and numerical model for colloid mobilization and transport at the Hanford vadose zone, and use that model to predict long-term colloid and colloid- facilitated radionuclide transport. To achieve these goals and objectives, we have used a combination of experimental, theoretical, and numerical methods at different spatial scales, ranging from microscopic investigationsof single particle attachment and detachment to larger-scale field experiments using outdoor lysimeters at the Hanford site. Microscopic and single particle investigations provided fundamental insight into mechanisms of colloid interactions with the air-water interface. We could show that a moving air water interface (such as a moving water front during infiltration and drainage) is very effective in removing and mobilizing particles from a stationary surface. We further demonstrated that it is particularly the advancing air-water interface which is mainly responsible for colloid mobilization. Forces acting on the colloids calculated from theory corroborated our experimental results, and confirm that the detachment forces (surface tension forces) during the advancing air-water interface movement were stronger than during the receding movement. Theory indicates that, for hydrophilic colloids, the advancing interface movement generally exerts a stronger detachment force than the receding, except when the hysteresis of the colloid-air-water contact angle is small. These results of our study are particularly relevant for colloid mobilization and transport related to three process in the vadose zone at Hanford: (1) water infiltration into sediments during rainfall or snowmelt events, (2) groundwater fluctuations as caused by river stage fluctuations, and (3) steady-state, low-flow recharge in deep vadose zone sediments. Transient water flow, like during infiltration or groundwater level fluctuations, are most conducive for colloid mobilization, but even during steady-state, low-flow recharge, colloids can be mobile, although to a much lesser extent. The results of this project have led to a comprehensive and fundamental understanding of colloid transport and mobilization under unsaturated flow conditions at the Hanford site.« less
  • Natural groundwater colloids have been recognized as possible agents for enhancing the subsurface transport of strongly-sorbing radionuclides. To evaluate this mechanism, packed-bed column experiments were conducted comparing the simultaneous transport of dissolved plutonium (Pu), Pu sorbed onto natural colloids, 190-nm and 500-nm diameter fluorescent CML microspheres, and tritiated water in saturated alluvium. Experiments were conducted in two columns having slightly different porosities at two flow rates, resulting in average linear velocities (v{sub z}) of 0.6 to 3.65 cm/hr in one column and 0.57 to 2.85 cm/hr in the other. In all experiments, Pu associated with natural colloids transported through alluviummore » essentially unretarded, while dissolved Pu was entirely retained. These results were consistent with the strong sorption of Pu to alluvium and the negligible desorption from natural colloids, observed in separate batch experiments, over time scales exceeding those of the column experiments. Breakthroughs of natural colloids preceded tritiated water in all experiments, indicating a slightly smaller effective pore volume for the colloids. The enhancement of colloids transport over tritiated water decreased with v{sub z}, implying {approx} 40% enhancement at v{sub z} = 0. The 500-nm CML microspheres were significantly attenuated in the column experiments compared to the 190-nm microspheres, which exhibited slightly more attenuation than natural colloids.« less
  • This Analysis/Model Report (AMR) summarizes transport properties for the lower unsaturated zone hydrogeologic units and the saturated zone at Yucca Mountain and provides a summary of data from the Busted Butte Unsaturated Zone Transport Test (UZTT). The purpose of this report is to summarize the sorption and transport knowledge relevant to flow and transport in the units below Yucca Mountain and to provide backup documentation for the sorption parameters decided upon for each rock type. Because of the complexity of processes such as sorption, and because of the lack of direct data for many conditions that may be relevant formore » Yucca Mountain, data from systems outside of Yucca Mountain are also included. The data reported in this AMR will be used in Total System Performance Assessment (TSPA) calculations and as general scientific support for various Process Model Reports (PMRs) requiring knowledge of the transport properties of different materials. This report provides, but is not limited to, sorption coefficients and other relevant thermodynamic and transport properties for the radioisotopes of concern, especially neptunium (Np), plutonium (Pu), Uranium (U), technetium (Tc), iodine (I), and selenium (Se). The unsaturated-zone (UZ) transport properties in the vitric Calico Hills (CHv) are discussed, as are colloidal transport data based on the Busted Butte UZTT, the saturated tuff, and alluvium. These values were determined through expert elicitation, direct measurements, and data analysis. The transport parameters include information on interactions of the fractures and matrix. In addition, core matrix permeability data from the Busted Butte UZTT are summarized by both percent alteration and dispersion.« less