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Through
the Environmental Management Science
Program (EMSP), DOEs
Office of Environmental Management (EM) and Office
of Science (SC) collaborate to fund basic research to solve intractable
problems that threaten the successful closure of DOE sites. As one
of the programs within the Office
of Science and Technology, EMSP ensures that OSTs projects
cover the full spectrum of R&D. EMSPs Web site is at http://emsp.em.doe.gov.
Over the last 50 years, nuclear R&D programs have resulted in
releases of plutonium to both on- and off-site locations at several
western DOE facilities. Most plutonium and other actinides are tightly
bound to soil particles, but the particles themselves are subject
to redistribution. The major driver of risks to human health and the
environment for DOE facilities in arid and semiarid environments
is the mobility of these actinides in surface soils. Research indicates
that actinide redistribution is driven primarily not by chemical processes,
but by the physical and biological processes associated with ecosystem
dynamics. Surface disturbances that cause changes in vegetation and
upper soil profiles, such as fire, drought, tilling, and burrowing
animals, are critical processes for determining long-term mobility
of actinides in the environment.
Actinide mobility is an issue at Rocky
Flats and Hanford,
and there is increasing concern at other DOE facilities in dry regions
about the effect of environmental disturbances that increase mobility.
At all of these facilities, uncertainty in actinide mobility hinges
on the relative roles of three modes of transport: wind erosion, water
erosion, and vertical migration, each of which depends on multiple,
interrelated environmental factors. Because it is a fundamental factor
in remediation decisions and long-term stewardship strategies, understanding
actinide mobility is an Environmental Management Science Program priority
in the health, ecology, and risk category.
The vast majority of actinide contaminants at DOE sites are of low
concentration and sequestered in soils, so its worth asking
not how, but whether to clean them up. Physical removal
of the soils is costly, presents significant health risks to workers,
virtually destroys the contaminated ecosystem, and requires a licensed
disposal site. If the long-term risk from actinides in surface soils
were known to be sufficiently low, contaminants might better be left
in place; but this option would require assessments that took into
account low-frequency, high-impact disturbances that change thresholds
between significant and nonsignificant transport of soil contaminants.
Until sound technical data and knowledge are available to accurately
address long-term fate and effects of soil actinides, scientific,
regulatory, and public confidence in cleanup decisions will be limited.
 
A recently concluded EMSP project, led by Los
Alamos National Laboratorys David Breshears with participation
from researchers at Colorado State
University and the Carlsbad Environmental
Monitoring and Science Center of New
Mexico State University, is providing DOE with data and tools
to improve risk assessments, cut cleanup costs, and facilitate technology
transfer. After first developing advanced measurement techniques for
assessing the three pathways, the team assembled new data on each
pathway based on site-specific field and laboratory measurements at
three major DOE facilities and developed multipathway, multisite assessments
of mobility based on existing long-term transport models. The results
were integrated in new assessment tools that will provide the basis
for incorporating strong technical information into the cleanup decision-making
process.
Measurement of low levels of plutonium-239 contamination in the environment
requires radiochemical analysis and alpha spectrometry, which are
expensive, time-consuming, and destructive. In contrast, gamma spectrometry
is cost-effective, rapid, and capable of measuring activity levels
in situ. The project team determined that cesium-137 and americium-241,
two radionuclides readily measured via gamma spectrometry counting,
could reliably be used as tracers for plutonium in soil and applied
this finding to their studies of the three transport modes. Initial
studies focused on Hanford,
Rocky Flats, and the Waste
Isolation Pilot Plant, three semiarid DOE sites that differ in
climate, soils, vegetation, and actinide sources.
Risk assessments often estimate wind erosion based on averages of
reported data, which can obscure variations of several orders of magnitude.
Average values have a large degree of uncertainty and may not be accurate
for other DOE sites. The LANL-led research team quantified wind erosion
rates using spatially distributed, finely time-resolved aerosol measurements
and correlated them with meteorological and ground-cover conditions.
Project results show that episodic, high-wind events disproportionately
increase resuspension.
Measurements also yielded strong evidence that wind erosion rates
from sites disturbed by fire or overgrazing are significantly greater
than those from undisturbed sites. The results demonstrate the importance
of low-frequency thresholds and disturbances in ground cover in determining
actinide transport by wind erosion.
Water erosion is a second major process affecting contaminant transport,
but major knowledge gaps exist. Intense convection thunderstorms often
play a major role in generating runoff and erosion in these environments.
Soil types, vegetation, surface slope, and the amount and intensity
of rainfall are key factors governing runoff, erosion, and associated
transport of actinides; but quantitative data were lacking on specific
sites and the hydrologic effect of site disturbance on the process.
This study created simulated rainstorms at different levels of initial
soil water content to measure erosional losses of sediment and an
actinide surrogate from disturbed (burned) and control field plots
located near three DOE sites.
Results highlighted the large effect of burning as a disturbance on
contaminant transport and mobility via runoff and erosion. Average
erosion rates at both WIPP and Rocky Flats were about three times
higher from disturbed plots than from control plots, and activity
readings from disturbed plots exceeded those from paired control plots
by factors of 313. Soil texture also had a pronounced effect
on runoff and erosion, making associated actinide transport strongly
site-specific. Contrasts in vegetation and soil composition between
Rocky Flats and WIPP caused radionuclide transport to differ by a
remarkable factor of 12.
Because plutonium solubility is extremely low under normal environmental
conditions, vertical migration of actinides must result from downward
transport of soil particles through either cracks or the soil matrix
itself. Project researchers used an ingenious new measurement system
on soil columns collected from the field to investigate vertical migration
as a function of soil type, water percolation, and wetting/drying
cycles that promote cracks in soil profiles.
Soil columns were subjected to a series of wetting/drying cycles in
a drying oven that could induce soil cracking within weeks or months,
accelerating a process that might occur only annually in the field.
Soil cracking was far more pronounced in certain soils, probably due
to higher clay content. Collectively, the results highlight the impact
of low-frequency events, such as soil cracking, on vertical migration.
The researchers used existing models of long-term transport to conduct
a preliminary assessment for each of the three modes of transport.
Data for the three field sites were used to parameterize and run models
and to compare predictions with measured field data. Water erosion
is most sensitive to slope angle of the land and soil texture; wind
erosion is most sensitive to range vegetation type and amount; and
vertical migration is most sensitive to soil texture and land contour.
The relative importance of the three pathways was evaluated to predict
average long-term responses for a total of seven DOE sites in arid
and semiarid sites.
The project team also developed a transport model for simulating dynamic
contaminant transport in soils. The model provides a framework for
creating code in which the soil is represented by a matrix of adjoining
soil columns, each subdivided into layers. The design is easy to modify
to represent a transport process, add new transport pathways, or customize
for site-specific processes. The code lays the groundwork for future
modeling efforts to fully couple all three pathways and incorporate
low-frequency, high-impact contaminant transport events.
The projects measurement and assessment results offer several
payoffs for DOE. Field studies demonstrate that disturbances that
reduce ground cover, such as fire or heavy grazing, can increase wind
and water erosion by more than two orders of magnitude. These results
clarify the need to factor disturbance events and recovery rates into
long-term assessment of actinide mobility. Research found that infrequent,
extreme climatic and disturbance events greatly increase transport
rates on all three pathways relative to long-term averages, highlighting
the need to account for extremes in climate and disturbance that may
be brief but contribute most to long-term risks. Models indicate that
the relative importance of actinide transport by wind erosion, water
erosion, and vertical migration differs within sites and from site
to site by more than an order of magnitude. These resultssome
of the first multipathway, multisite estimates for DOE facilitiescan
be used to set priorities to improve risk assessments and remediation.
An important theme emerging from this project is that each of the
three pathways exhibits threshold responses to a suite of environmental
conditionsprecipitation intensity, wind velocity, wetting-drying
cycles, surface heterogeneity (vegetation and ground cover), and disturbances
that impact the surface heterogeneityresulting in nonlinear
increases in contaminant transport. These results highlight the importance
of finer-scale processes that could dominate the overall risk estimates
associated with the long-term mobility of actinides; but these processes
are not generally evaluated in concert and their threshold response
is largely unconsidered. Improved risk assessment for addressing remediation,
litigation, and long-term stewardship will require a more mechanistic
understanding and predictive capability of these processes.
Quantifying the thresholds that determine changes in the rates of
soil actinides transport from wind erosion, water erosion, and vertical
migration over longer time frames provides the basis for a scientifically
defensible risk assessment. Such an assessment may justify leaving
the contaminants in place, saving taxpayers billions of dollars. At
a minimum, a sound technical basis for cleanup decisions can help
increase stakeholder confidence in selected strategies and in plans
for long-term site stewardship.
For more information on this research, contact principal investigator
David Breshears, Los Alamos National Laboratory, (505) 665-2803, daveb@lanl.gov.
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