11

Testing Amendments for Increasing Soil

Availability of Radionuclides
Nicholas R. Watt

Summary
Phytoextraction has been shown to be potentially feasible for some radionuclides. It is,
however, likely that soil amendments will be needed to make contaminant radionuclides
sufficiently available for plant uptake over the long time-scales likely to be required for
phytoextraction. A method is described here for investigating the effect of soil amend-
ments on the long-term uptake of 137Cs in a laboratory trial. The method described uses
large containers filled with artificially contaminated soil, which are harvested at 8-wk
intervals and then replanted. Consideration is also given to applying this method to other
radionuclides.

Key Words: Phytoextraction; phytoremediation; soil amendment; radionuclide; 137Cs.

1. Introduction
Phytoextraction of radionuclides has been shown to be at least theoretically
feasible for a number of elements including isotopes of U (1), Sr (2,3), and Cs
(4–7). However, although plants have been shown to readily remove some
radionuclides under certain conditions (1,8), it would appear that availability
of radionuclides for plant uptake may be the rate-limiting step for contaminant
removal (8). Two possible reasons for the limited availability of radionuclides
for plant uptake are (1) the chemical species found in the soil is unsuitable for
plant uptake (9) and (2) fixation of the radionuclide to the substrate as is the
case, for example, for 137Cs (10). Some amendment of soil availability may,
therefore, be necessary if phytoextraction is to become a practically useful
remediation technology for radionuclides (11,12). Future investigations of the
potential for phytoextraction to remediate radioactively contaminated soils

From: Methods in Biotechnology, vol. 23: Phytoremediation: Methods and Reviews

Edited by: N. Willey © Humana Press Inc., Totowa, NJ

131
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will therefore need to examine the effects of soil amendments on reducing

remediation times.
Given the relatively slow removal of ions from soils by plants, time-scales
for phytoextraction of radionuclides are likely to be measured in years. However,
phytoextraction trials reported in the literature where soil amendments have
been used have tended to utilize time-scales of less than 12 wk (4–7), hence
little is known about the potential performance of soil amendment-assisted
phytoextraction over practical time-scales. Furthermore, the herbaceous plants
that might be useful in phytoextraction systems will require repeated planting
and harvesting, at least in the case of 137Cs. Although the literature contains
many examples of 137Cs uptake over long time-scales following weapons test-
ing and the Chernobyl accident, repeated planting and harvesting data are rarely
reported.
The current limited knowledge of the effects of soil amendments on the long-
term behavior of radionuclides in phytoextraction systems suggests that it
would be inappropriate to establish trials of the use of soil amendments at field
sites. First, there is a risk of mobilizing the radionuclide off-site and second, in
the United Kingdom, for example, regulatory approval may be unlikely to be
forthcoming for such trials. Furthermore, the complexities of interpreting
results from field sites suggest that controlled laboratory experiments represent
a sensible starting point for investigations into the longer term phytoextraction
of radionuclides combined with the use of soil amendments.
Here, a method is described for investigating the effects of soil amendments
on 137Cs uptake by herbaceous plants grown under a repeated cropping regime.
137Cs is of particular interest at radioactively contaminated sites in the United

Kingdom because it is a high-yield fission product and has a relatively long

half-life (~30 yr) (8). Details are provided in the notes as to how the method
might be adapted for other radionuclides.

2. Materials
2.1. Soil
Soil used in experiments can be either soil sampled from contaminated sites
or, where this is not practically possible or experimentally desirable, clean soil
with radionuclides added (see Note 1). Where clean soil is employed the
radionuclide being investigated will have to be applied in aqueous form. The
limits on the activities used in the experiment will vary depending on local labo-
ratory rules. Sufficient activity should be applied to ensure that measurable
quantities of the radionuclide are removed by the particular plant species being
used (see Note 2), within limits that ensure that dose rates to laboratory workers
are kept as low as reasonably practicable.
Increasing Soil Availability of Radionuclides 133

2.2. Soil Amendments

Soil amendments can be selected from a wide range of chemical compounds
(see Note 3). As a starting point for investigations of 137Cs phytoextraction,
monovalent cations including NH4, Cs, and K can be used. Where an amend-
ment can degrade over time consideration should be given to the most appro-
priate application regime.
2.3. Plant Species
Although any herbaceous plant species could potentially be used in this
experiment, as a starting point a species that is known to possess reasonably
high uptake should be selected to ensure that measurable quantities of the con-
taminant are taken up by the plant. For example, in the case of 137Cs, Beta
vulgaris (leaf beet) is a suitable species (see Note 4).

3. Methods
3.1. Experimental Setup
1. Four open-topped plastic containers (approximate dimensions 40 u 60 cm and
equipped with drainage holes), are filled with a quantity of the soil to be investi-
gated to a depth marginally greater than the rooting depth of the plant (see Note 5).
The containers are placed in trays to prevent cross-contamination of the treatments
and leaching of any radioactive solution.
2. Where clean soil is the starting point, each container is contaminated with suffi-
cient 137Cs in a deionized water solution to provide a soil 137Cs-activity concen-
tration of approx 4 Bq/g (see Note 6). The soil is then thoroughly mixed using a
trowel, and samples are taken from throughout the soil and analyzed for 137Cs con-
tent to ensure a heterogeneous 137Cs distribution. Following addition of the 137Cs,
the soil is allowed to stand for 4 wk to allow for equilibration of the 137Cs with the
substrate. Where soil is used from a contaminated site, mixing and sampling is still
carried out to ensure the distribution of activity is heterogeneous.
3. The soil amendments being investigated are then applied to the containers in suf-
ficient quantify to be uniformly distributed throughout the soil (see Note 7).

3.2. Growing and Harvesting Plants

1. B. vulgaris var. Swiss chard “Fordhook Giant” seeds are broadcast into each con-
tainer by hand. The containers are then covered with cling film to encourage ger-
mination and placed on a bench equipped with supplementary lighting (mean PAR
200 Pmol/m/s) for 16 h each day (see Fig 1). Following germination the cling
film is removed and the containers are watered with deionized water to keep them
in a sufficiently moist state for plant growth but not to a level such that the amend-
ment or radionuclide solution is flushed from the soil.
2. The position of the containers is rotated at weekly intervals so that each container
occupies each position on the bench for 2 wk during each harvest period.
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Fig. 1. Experimental arrangement for a 137Cs phytoextraction trial using four experi-
mental treatments.

3. At 8-wk intervals the aerial plant parts are harvested, weighed, placed in
envelopes, and dried for 48 h in an oven at 80°C. The dried plant material is then
ground to a powder in a boiling tube, transferred to a 70-mm diameter plastic pot,
and weighed. Samples are analyzed for 137Cs content with the plastic pot in
contact with the end-cap of a high-purity Ge detector for 3600 s (see Note 8).
4. Following harvesting, the soil in the containers is turned over using a hand trowel
and watered with deionized water. Where degradable soil amendments are being
used, these are replenished as appropriate. The containers are then replanted with
B. vulgaris and the harvest and planting regime is repeated for as long as is
required for the experiment.
5. Concurrently with the plant growth in the containers, four 12-cm diameter plastic
plant pots are prepared that duplicate the experimental treatments in all respects
except that they do not contain any 137Cs. This allows the concentrations of the soil
amendments to be determined in 137Cs-free solutions (see Note 9). Samples are
taken from each pot at intervals throughout the experiment and analyzed using
standard techniques for the soil amendment in question, for example, for NH4
and NO3–, conductivity detection can be used.
4. Notes
1. The type of soil used will depend on the purpose of the experiment. For work
based on actual contaminated sites, soil from the site being investigated should be
Increasing Soil Availability of Radionuclides 135

used. This may not always be possible if activity levels, and hence dose rates, are
too high to permit the soil to be moved into a laboratory or greenhouse environ-
ment. For general investigations concerning the effectiveness of amendments for
a particular radionuclide, consideration should be given to using a soil which does
not significantly reduce plant availability, for example, an organic soil for isotopes
of Cs. For some radionuclides, aging processes are an important factor in their
availability for plant uptake over time. In particular, where artificially contami-
nated soils are used, experimenters will need to consider over what time-period the
radionuclide should be allowed to “age” after application and before planting
takes place. Care will need to be taken when applying the results from experiments
using artificially contaminated soils to field applications.
2. Depending on existing knowledge of uptake by a particular species for a given
radionuclide in a given substrate, it may be useful to conduct pot experiments to
ensure that measurable levels of the radionuclide can be removed.
3. Soil amendments could potentially be almost any chemical compound. Selection
will depend in part on the mechanism of improving plant uptake of the radio-
nuclide in question. For example, amendments could be targeted at desorbing the
radionuclide from the soil (for example, monovalent cations, and 137Cs), increas-
ing the solubility of a radionuclide, or chelating the radionuclide (for example,
EDTA and Pb). In addition, there are many agrochemicals that have been devel-
oped to affect soil processes, especially for some plant nutrients, and much is
known about the behavior and use of these compounds in soils. Future research
efforts should consider testing compounds from the wide range of agrochemicals
available. Some agrochemicals do not have a direct effect on nutrient availability,
rather they increase the persistence of other agrochemicals, for example, nitrifica-
tion inhibitors can maintain a higher NH4 concentration in the soil, which is of
interest to 137Cs phytoextraction.
4. The choice of plant species may be constrained by the ability of a particular
species to grow in the soil being tested and an understanding of the uptake char-
acteristics of the species considered for the trial. Approaches to aid species selec-
tion include considering species that are indigenous to the contaminated site, in
the United Kingdom for example, using the Natural History Museum’s Postcode
Plant Database (8) and in other countries regional/national equivalents, or select-
ing species from higher taxonomic groups that are known to have higher uptake
of the radionuclide being investigated. For example, in the case of 137Cs, the
Caryophyllidae clade has been shown to include species with high-uptake charac-
teristics for 137Cs including B. vulgaris (13).
5. The size of, and number of, containers used will depend on the number of treat-
ments being investigated and the space available, which can be limited for
experiments involving radionuclides. The volume of soil in the container
should be large enough to allow root growth to be uninhibited by the container
over the duration of the harvesting period. For manual handling purposes, con-
sideration should be given to the weight of the container when filled with wet
soil.
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6. A soil-activity concentration of approx 4 Bg/g137Cs should be sufficient for meas-

urable quantities of 137Cs to be taken up by plants over a time-scale of some
months while keeping the radiation dose as low as reasonably practicable. Suitable
adjustments will need to be made for other radionuclides. Low soil-activity con-
centrations allow the performance of phytoextraction to be assessed at contami-
nant concentrations that might be expected to be difficult to remediate and to
establish whether a body of soil can be remediated to levels that are below regu-
latory concern for a particular radionuclide.
7. It may be useful in experiments designed to simulate field trials to consider the
unit of application in agricultural terms especially where amendments are agro-
chemicals. For example, for trials involving 137Cs, NH4 can be applied in quanti-
ties equivalent to 300 kg/ha.
8. Where it is difficult to estimate the uptake of a radionuclide by plants from soils
containing low radionuclide-activity concentrations, more sensitive analytical
techniques may need to be used. For example, for 137Cs uptake at soil-activity con-
centrations of approx 4 Bq/g, a high-purity Ge detector has been used for the
analysis because it is a more sensitive technique than a NaI (Tl) detector (14). In
practice, the sensitivity of the detector will need to be considered in conjunction
with the number of samples that can be processed in each batch. NaI (Tl) detec-
tors found in some laboratories can be capable of processing many more samples
in a batch than high -purity Ge detectors.
9. Measurement of soil-amendment concentrations over time are of interest and may
be of particular importance where amendments degrade over time, as is the case with
some nitrification inhibitors (for example, dicyandiamide), or where the amendment
is itself taken up by the plant. This presents a practical difficulty where facilities are
not available to perform chemical analysis of radioactive samples. Furthermore,
these techniques can be expensive to source from external laboratories. Attempts
should therefore be made to replicate the conditions found in each experimental
treatment as closely as possible but without any radionuclides being present.

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