The thousands of abandoned, inactive, and
operating mines present serious potential risks to human health and the
environment. The extraction and processing of metals, non-metal minerals and
coal, result in the generation of large quantities of contaminated solid
wastes, wastewater and air emissions which cause significant environmental
impacts, including groundwater and surface water contamination, soil erosion
and soil contamination.
The legacies of past uranium mining and
milling activities continue to be a cause of concern and require assessment and
remedial action. Over the next several decades, a large investment will have to
be committed to clean up sites contaminated with hazardous waste and petroleum
products. This commitment will result in a continuing demand for site
remediation services and technologies, which implies more research needs.
The special risks associated with uranium
mining in the past were mostly addressed to workers mines. Over the past
decades, these concerns for worker health and safety have been the driving
force for gradually tighter controls and improved work and safety practices.
Only in relatively recent times, however, impacts on public health and on the
wider natural environment, related to uranium mining, have been received the
deserved attention. In the case of the natural environment, these concerns
include the risk of environmental degradation, contamination and ecosystem
biodiversity, aesthetics, access to land and future land beneficial use.
The important routes of contamination have
been identified as a basis for determining the modelling approach and the
radionuclides of major concern were identified in each one of the compartments
based on their chemical, physical and radiological properties. Each compartment
represents an environmental media: air, soil, water, vegetation and biota. A
radionuclide transfer model through the food chain is also incorporated.
When modelling contaminant release and
transport mechanisms for each environmental compartment, the major output
chosen is often the contaminant concentration in each exposition point selected
(for instance, breathing air zone, superficial soil and well water). This will
allow the assessment of doses, if an additional exposure scenery is created.
The objective is to quantify the potential exposure levels of the hazard at the
receptor location answering to these main questions: what is the contaminant
concentration in the exposition point? How much of a contaminant do people
inhale or ingest during a specific period of time? Is the situation acceptable?
The undisturbed uranium ores contain low
concentrations of the decay daughters of uranium and thorium radionuclides in
equilibrium with the parental materials. In the uranium mineral processing some
of the radionuclides are not dissolved during the leaching process, which
breaks down the equilibrium chains of the uranium decay, remaining in the
tailings at their original activities. The expressions used to estimate the activity
for each one of the radionuclides in the tailings results from the successive
radioactive decays for the two uranium decay series, the uranium series 238U
(4n + 2) and the actinium series 235U (4n + 3).
The basic equations of diffusion were used
for estimating the theoretical values of the radon flux from the 226Ra
content in the waste material. The fundamentals of the conceptual model are
based in the principles of diffusion across a porous medium, which allows the
mathematical description of the radon transport through the waste and the
cover.
Radon migration to the surface is a complex
process controlled mainly by porosity, and moisture, leading the cover
efficiency in attenuating the radon flux. This efficiency depends on the
capacity of the cover material for keeping the diffusion so slow that radon
decays to another non-gaseous nuclide, becoming trapped by the cover system. The
algorithm incorporates the radon attenuation originated by an arbitrary cover
system placed over the radioactive waste disposal. As an alternative, it can be
estimated the thickness of the cover that allows a radon flux inferior to the
acceptable one.
The contaminant concentration released is
estimated by a box model formulation which has implicit a mass balance
formulation. The box volume is defined by its length, width and the mixing
height. As a consequence of a steady state assumption, the pollutant
concentration is constant in time and the mass flow rate entering into the box
is equal to the flow rate leaving the box.
In the atmospheric transport a
two-dimensional model is used for calculating the flux diffusion from the radioactive
waste disposal, having as result the hazard concentration at a defined distance
from the soil (the breathing or mixing height) which will be the starting point
for the dispersion which can be considered either simultaneously in each wind
direction or only in the prevailing wind direction. The atmospheric dispersion
is modelled by a modified Gaussian plume equation which estimates the average
dispersion of the contaminants released from the source in each wind direction.
The plume dispersion model accounts for the gaseous contaminant transport from
the source area to a downwind receptor. The atmospheric transport is done at
wind-speed to a sampling position located at surface elevation and transverse
horizontal distance from the plume.
For the hydrologic transport a two-direction
model is proposed for simulating the contaminants release from the waste
disposal and its migration process through the soil to the groundwater. The
final result is the contaminant concentration in the groundwater as function of
the elapsed time, at a defined distance from the waste disposal, generally the
location where the exposition point is considered being represented by an
hypothetical well.
A leaching model based on a
sorption-desorption process is used for describing the contaminant release from
the waste disposal. The leachate concentration is determined by a distribution
or a partition coefficient which describes the relative transport speed of the
contaminant to the water existing in the pores; soil properties such as bulk
density, and water content; the extent of contamination, described by the
contaminated zone thickness, area, and the amount of contaminant in the source.
The transport for the dissolved
contaminants is considered to occur either in the vertical direction through
the unsaturated zone until an aquifer is reached either in the horizontal
direction, through the saturated zone flowing to an hypothetical well, where
the contaminants become accessible to humans or other forms of life. The
vertical flow is considered to be one-dimensional. It is assumed that there is
retardation during the vertical transport that is estimated assuming that the
adsorption-desorption process can be represented by a linear isotherm.
Movement and fate of radionuclides in
groundwater follow the transport components represented by the basic
diffusion/dispersion–advection equation with radioactive decay and retardation
for the radionuclide transport in the groundwater.
The radionuclides initially considered in
the model simulation were uranium, thorium, radium, polonium and lead but only
the results obtained for uranium and radium were included in the model exploration.
For the other radionuclides considered, the results were in accordance with the
expected based on the assumption that because of the slow rate of contamination
migration only the radionuclides with relatively long half-life are of
importance in the transport process. In addition, data on uranium and radium
activity in groundwater and superficial waters from the Urgeiriça site were
used in the model simulation comparing the model results with the measured
data.
The hydrologic model also quantifies the
superficial runoff and its transport to the superficial waters. The activity
present in this environmental compartment, superficial water, may be a
potential pathway to food chain contamination, either by the direct use of
streams waters or indirectly through the contaminated aquatic biota.
As a result, the hydrologic model estimates
the radionuclide activity concentration in each exposition point, namely in the
underground waters (represented by a well) and in the superficial waters
(represented by a streamlet).
Modelling the radionuclide transfer to
vegetation has implicit several processes which describes and quantify
mathematically the radionuclides transfer mechanisms, transport, absorption and
translocation to vegetation. The main goal is to develop a radionuclide
transfer model through food chain by the ingestion of contaminated vegetation.
This pathway can be quite significant because of the biological concentration
in the foodstuffs.
Vegetation may be contaminated through
direct deposition, root uptake or irrigation with contaminated water. The material
resuspension from superficial soil may occur due to the wind, rain or mechanical
factors, with later deposition onto vegetation surface.
A model was developed to describe each one
of these contamination pathways: root uptake, deposition and resuspension,
either from deposition either from irrigation with contaminated water from a
well. Radionuclides evolved in the transfer processes depends on the
contamination route, deposition or root uptake.
The different contamination processes were
combined in a global model for simulate the radionuclide transfer and estimate
the vegetation activity resulting from each one of the contamination processes.
The final output is the total concentration in the vegetation combining the
internal contamination with the external contamination.
The model is rather complex as it is
necessary to understand and transcribe to the conceptual model the interactions
between the contaminants (radionuclides or heavy metals) and the soil
components, vegetation, as well as the interactions between the contaminants
itself.
The conceptual model is based on the
assumption that each one of the transfer processes may have either origin in
soil either in the air. In the first case, the processes involved are
deposition (characterized by the deposition velocity), interception (described
by the interception factor) and retention (described by the weathering
half-live). In the second case, the radionuclide behaviour in soil and its
mobilization reflects the radionuclides physics and chemical properties, soil
properties, the type of vegetation and local hydrology and geology characteristics.
The next model will complete the previous
one by simulating the radionuclide transfer through the food chain resulting
from the cattle ingestion of contaminated vegetation.
Contamination of the trophic chain by
radionuclides released into the environment will be a component of human
exposure by transferring the radionuclides into animal products that are part
of the human diet. This can occur by first ingestion of contaminated pasture by
animals and then by ingestion of animal products contaminated (dairy or meat).
The relevant incorporation of the radionuclides into cow’s milk, for instance,
is usually due to the ingestion of contaminated pasture. This transfer process
is often called the pasture-cow-milk
exposure route.
A compartment dynamic model was developed
to describe mathematically the radionuclide behaviour in the pasture-cow-milk exposure route and
predict the activity concentration in each sub-compartment. The dynamic model
is defined by a system of linear differential equations with constant
coefficients describing the mass balance in different compartments taking in
account the fluxes in and out of the compartment and the radionuclides decay. For
each compartment, a transient mass balance equation defines the relations
between the inner transformations and the input and output fluxes. The fluxes
between the compartments are estimated with a transfer rate proportional to the
amount of the radionuclide in the compartment. The concentration within each
compartment is then transcribed to doses values based on a simplified exposure
pathway and a pre-defined critical group.
The first model considered for the transfer
through the food chain is relatively simple and classic and considers as
initial state a contaminated pasture that is consumed by a cow that produces a
certain quantity of milk. The transfer coefficients for soil and pasture
compartments are expressed as function of soil characteristics and ecological
parameters. A more sophisticated model is also described taking into account
the spread of the radionuclide within the cow by including the sub-compartments
involved: the gastrointestinal system (GIT), the plasma and the bones, in the
case of radium simulation.
The transfer coefficients for the
sub-compartments within the cow are combined with biological half-lives which
is the time taken for the radionuclide activity concentration in tissues or
milk be reduced by one half of its initial value.
A complete model simulation was already
done for radium and the model can also be applied to uranium, thorium, lead and
polonium depending on the availability of data.
For all sub-models at least one simulation
was done. The necessary parameters were adopted from different sources: some
parameters were adopted from measurements referring to a particular
contaminated site, the Urgeiriça Uranium tailings piles, and others were
adopted from published data. The unknown parameters were estimated from
available data or from literature references in cases where on-site data were
not available.