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Advances in Phytotherapy Research, 2009: 139-149 ISBN: 978-81-308-0223-7


Editor: Mohamed Eddouks

Medicinal plants: Investigation

9 of the soil-to-plant transfer


factor of radon using SSNTD
technique
El Amraoui, M.2, M. Eddouks2 and L. Oufni1
1
University of Cadi Ayyad, Polydisciplinary Faculty of Beni Mellal, BP 592
23000, Beni Mellal, Morocco; 2UFR Physiology of the Nutrition and Endocrine
Pharmacology, BP 509, Boutalamine, 52000, Errachidia, Morocco

Abstract
The degree of radon (222Rn) root uptake from
soil into three medicinal plants (Retama raetam,
Peganum harmala and Zizyphus lotus) used in the
Errachidia area (South-eastern Morocco) has
been quantified using soil-to-plant transfer factors
(TF). The radon TF was studied using CR-39
and LR-115 type II SSNTDs technique. TF for
roots were higher than those for stems and leaves.
Correspondence/Reprint request: Dr. L. Oufni, University of Cadi Ayyad, Polydisciplinary Faculty of Beni
Mellal, BP 592, 23000, Beni Mellal, Morocco. E-mail: Oufni@lycos.com
140 El Amraoui, M. et al.

The radon activity in the soils has been found to be varying from 27.35 ±
2.14 Bq m-3 to 43.03 ± 3.35 Bq m-3; these values are lower in the leaves and
stems than those determined in the roots of the studied plants. The aim of this
study was to analyze the radon transfer from soil to different compartments
of these medicinal plants and then to evaluate radiotoxicity caused by radon
in order to contribute to the health risk assessment.

Introduction
It’s well known that the radiations emitted from the primordial radionuclide
originating from the Earth’s crust are the major contributors to the total
background exposures to the human populations. They include external gamma
exposures and inhalation exposures, approximately in equal measure, the latter
being due to radon (222Rn), thoron and their progenies in the indoor environment.
222
Rn, a progeny of uranium-238 (238U), is a colorless, odorless, noble and
radioactive gas. Its half-life is 3.82 days, its decay with the emission of 5.48 MeV
α-particles. Radon and its short-lived decay products (Fig.1) in dwellings present
the main source of public exposure from the natural contributing to nearly 50% of
the global effective dose to population [1]. Lung cancer pathologies caused by
inhalation exposure to radon is due to alpha-dose deposited by short-lived radon
decay products. It’s well known that exposure of population to high
concentrations of radon and its daughters for a long period leads to some
pathological effects like the respiratory functional changes and the high
occurrence of lung cancer [2]. Radon appears mainly by diffusion processes from
the point origin following α-decay of 226Ra in underground soil. Radon diffusion
and transport through different media is a complex process and is affected by
several factors [3,4]. It is well known that for material medium, the porosity,
permeability and the diffusion coefficient are the parameters which can affect
directly the capacity to hinder the flow of radon soil gas.
To estimate a realistic radiation exposure of the population, the behavior
of the deposited radionuclides in the food chain has to be known. After the
Chernobyl accident, research activities have been focused on the soil-plant
transfer of Caesium isotopes and the long lived-fission products. Much less is
known about the transfer of the nuclides of the primordial decay chains, most
investigations refer to 226Ra. [5]. People from all cultures have traditionally
relied on natural resources, mainly of plant origin, as folk medicines to treat
diseases and disorders. Herbs have also been the source of many “modern”
single-component drugs. Today, medicinal plants are being accepted and
used increasingly by general populations in both Eastern and Western
countries as medicines or dietary supplements, either alone or in combination
with more modern chemotherapeutic agents [6]. In the present study, we used a
Radiotoxicity and medicinal plants 141

Rn
222
Rn

Short-lived decay products 3.8d


At

210 214 218


Po Po Po
Po
5d
20min
-4
140d 10 s 3.1min
Bi

22y 27min

Pb

206 210 214 218 222

Mass no.

Figure 1. Decay scheme for 222Rn showing the short-lived decay products to 210
Pb
and subsequent transformations to 206Pb.

method based on calculating the detection efficiencies on the LR-115 type II and
CR-39 SSNTDs for alpha-particles emitted by the uranium (Radon) and thorium
(Thoron) series and exploiting the corresponding track densities for evaluating
the resulting alpha-activity in the soils and three medicinal plants: Peganum
harmala (PH), Zizyphus lotus (ZL) and Retama raetam (RR) which are used
traditionally as antidiabetic plants in the North of Africa [7,8]. We also determine
the annual effective dose rate due to radon in the studied medicinal plant samples.
These measurements of radon activities were used to determine their soil-to-plant
transfer factors (TF). The SSNTD technique has also been used for determining
alpha and beta dose-rates, the radon diffusion coefficient and radon exhalation
rate in various quaternary samples [3,9,10,]. This technique has been previously
used to study the indoor radon level in different dwellings [11-16].

Material and methods


Geological setting and samples
Soil and medicinal plant samples were collected from three fields
throughout Errachidia area (South-eastern Morocco, Fig.2) during the spring
period of 2002. The Errachidia area has a Saharan Mediterranean climate and
situated between 31°55’27.00” North latitude and 4°21’38.00” Western
longitude with elevation of 1045 m (3428 feet). The soil samples collected
from each place were dried at 30°C during one week, passed through 2mm sieve
and then were thoroughly mixed and pulverized with an agate ball mill.
The mean annual temperature was 18°C, with a minimum of 4°C (January) and
maximum of 30°C (July). The soil of the experimental areas had a clay loamy
142 El Amraoui, M. et al.

Mediterranean
Tanger
Rif las
At
e
dl

an
Rabat
id

ce
Beni-Mellal M

O
ic
tlas
High A
nt
Marrakech
la
At
Errachidia

Agadir

Smara

Dakhla

Figure 2. Map showing the localization of the studied samples in the Errachidia
district (Morocco).

texture with 29.6% clay, 34% loam, 36.4% sand, a bulk density of 1.35kg/l, a
porosity of 49.3%. The soil contained 0.07% total N, 0.88 organic mater and
a pH of 8.5 (H2O) in the 0-20 cm horizon. Aboveground plant material
was weighed, dried at 100 °C until constant weight and milled before
radioactivity quantification.

Method of study
The LR-115 type II (film track detector) is a cellulose nitrate (C6H2O9N2)
film of 12 µm thickness manufacture by Kodak Path, France. The CR-39
SSNTD (500 µm thick) is the diglycol carbonate (C12H18O7) supplied by
Pershore Mouldings Ltd, United Kingdom. Disk-shaped Pershore Mouldings
CR-39 and Kodak LR-115 type II Solid State Nuclear Track Detectors
(SSNTDs) films of about 1.5×1.5 cm2 have been separately placed in close
contact with homogeneous natural studied samples (soils and corresponding
medicinal plants) in a hermetically sealed cylindrical plastic container for one
month (Fig.3).
During this time, α-particles emitted by radon, thoron and their
corresponding daughters bombarded the SSNTD films. After the irradiation,
the detectors were etched separately with a NaOH solution (2.5 N at 60°C for
120min for LR-115 type II films and 6.25 N at 70°C for 7 h for the CR-39
sheets). The temperature was kept constant with accuracy of ± 1°C during
etching time; the detectors were taken out from the etching and immediately
Radiotoxicity and medicinal plants 143

LR-115 SSNTD

Plastic container
Pulverized sample

CR-39 SSNTD

Figure 3. Arrangement of the studied natural material sample on a solid state nuclear
track detector (SSNTD) in a well-closed plastic container.

rinsed by distillated water. After this chemical treatment, the track densities
registered on the LR-115 type II and CR-39 were determined by means of an
optical microscope. For our experimental etching conditions, the residual
thickness of the LR-115 type II SSNTD is of 5µm which corresponds to the
lower (Emin = 1.6 MeV) and upper (Emax = 4.7 MeV) energy limits for registration
of tracks of alpha particles in LR-115 type II films [17].All alpha-particles
emitted by the 238U and 232Th series that reach the LR-115 type II SSNTD with a
residual energy situated between 1.6 and 4.7 MeV are registered as bright track-
holes. The CR-39 SSNTD is sensitive to all α-particles reaching its surface.
Different soils and corresponding plants (widely used in Morocco as
medicinal plants) have been pounded and homogenized. Disc-shaped Pershore
Moudlings CR-39 and Kodak LR-115 type II SSNTD films of 4 cm diameter
were separately placed on each studied material sample in a hermetically sealed
cylindrical plastic container for 1 month (Fig. 3), measuring track density rates
(tracks cm-2 s-1) registered on the CR-39 (DG(CR)) and LR-115 type II
(DG(LR)). One can evaluate radon (Ac (222Rn)) and thoron (Ac (220Rn)) alpha-
activities (in Bq cm-3) inside the sample by using the following equations:

A c ( 222 Rn ) ⎡ 8 A c ( 220 Rn ) 7 ⎤
D G (LR ) = ⎢∑ i i i
k R ε + ∑ i i i⎥
k R ε (1)
2 ⎣ i =1 A c ( 222 Rn ) i =1 ⎦

and

A c ( 222 Rn ) ⎡ 8 A c ( 220 Rn ) 7 ⎤
D G (CR ) = ⎢∑ k i R i ε i + ∑ k i R i ε i' ⎥
' (2)
222
2 ⎣ i =1 A c ( Rn ) i =1 ⎦

where Ac(222Rn) and Ac(220Rn) are the radon (222Rn) and thoron (220Rn)
α-activities (Bq cm-3) inside the studied material sample, ki is the branching
144 El Amraoui, M. et al.

ratio corresponding to the disintegration of the nuclei of uranium and thorium


groups, Ri is the range of α-particle of energy Eαi in the material sample and
it is calculated by means of the TRIM programme,18 εi and ε i are
'

respectively the detection efficiencies of the LR-115 type II and CR-39


detectors for the emitted α-particles.
Combining Eqs. (1) and (2), we obtain the following relationship
between thoron-to-radon ratios and track densities:

D G (LR ) 8 8

A c ( 220 Rn ) D G (CR ) i =1
∑ i ii ∑
k R ε '

i =1
k i R iεi
222
= 7 (3)
D G (LR ) 7
∑ ∑
A c ( Rn )
k R ε
i i i − k i R i ε i'
i =1 D G (CR ) i =1

From where one obtains the Radon activity given by:

2D G (LR )
A c ( 222 Rn ) = (4)
D G ( LR ) 8 8

8 ∑ i ii ∑
D G (CR ) i =1
k R ε '
− k i R iεi 7

∑ k i R iεi + 7
D G ( LR ) 7
i =1
∑k R ε i i i
i =1
∑i =1
k iR iεi − ∑
D G (CR ) i =1
k i R i ε i' i =1

Calculation of the transfer factor


The entry of trace contaminants, which are present in the terrestrial
environment, into human food chains is controlled in the long term by their
uptake by plant roots. For radionuclides, it is generally assumed that the
concentration of a nuclide in a plant or plant part, Cp (Bq kg-1, dry weight), is
linearly related to its concentration in soil within the rooting zone, Cs (Bq kg-
1
, dry weight), i.e.

Cp = β Cs (5)

The proportionality constant β will be noted TF which is called the soil-


to-plant transfer factor, it is given by:

Activity concentration of plant (Bq/kg dry weight)


TF =
Activity concentration of soil (Bq/kg dry weight)

In our case,
Radiotoxicity and medicinal plants 145

A c ( 222 Rn ) of plant
TF = (6)
A c ( 222 Rn ) of soil

Results and discussion


Alpha-activities per unit volume due to radon have been determined
inside various natural material samples (soils and the corresponding
medicinal plants). Data obtained are shown in Tables 1-3. From the statistical
error on track counting one can determine the error on track density rate and
then evaluate the relative uncertainty of the radon determination which is
of 8%.

Table 1. Data obtained for radon activities inside soil and Retama raetam (RR) samples.

Retama raetam Preparation Ac(222Rn) (Bq m-3)


Soil-1 34.18 ± 2.50
Root-1 15.82 ± 1.12
RR-1
Stem-1 8.02 ± 0.64
Leaf-1 13.86 ± 1.11
Soil-2 27.35 ± 2.14
Root-2 12.55 ± 1.02
RR-2
Stem-2 8.64 ± 0.67
Leaf-2 10.90 ± 0.83
Soil-3 30.41 ± 2.38
Root-3 14.35 ± 1.14
RR-3
Stem-3 12.02 ± 0.92
Leaf-3 13.86 ± 1.08

Table 2. Data obtained for radon alpha activities inside soil and Peganum harmala
(PH) samples.

Peganum harmala Preparation Ac(222Rn) (Bq m-3)


Soil-1 43.03 ± 3.35
Root-1 18.31 ± 1.44
PH-1
Stem-1 11.50 ± 0.85
Leaf-1 12.77 ± 0.94
Soil-2 42.21 ± 3.36
Root-2 18.02 ± 1.35
PH-2
Stem-2 15.72 ± 1.24
Leaf-2 17.25 ± 1.35
Soil-3 39.41 ± 3.10
Root-3 18.33 ± 1.38
PH-3
Stem-3 12.92 ± 1.03
Leaf-3 14.06 ± 1.06
146 El Amraoui, M. et al.

Table 3. Data obtained for radon alpha activities inside soil and Zizyphus lotus (ZL)
samples.

Zizyphus lotus Preparation Ac(222Rn) (Bq m-3)


Soil-1 35.58 ± 2.70
Root-1 14.70 ± 1.16
ZL-1
Stem-1 10.62 ±0.83
Leaf-1 9.90 ± 0.78
Soil-2 37.00 ± 2.84
Root-2 15.30 ± 1.15
ZL-2
Stem-2 14.92 ± 1.17
Leaf-2 13.33 ± 1.02
Soil-3 38.95 ± 3.10
Root-3 14.52 ± 1.14
ZL-3
Stem-3 14.00 ± 1.08
Leaf-3 12.82 ± 0.95

We notice that alpha-activities due to radon are clearly different in the three
soil samples collected from various places. This difference can be explained
by the transport conditions and of the uranium dissolution at the time of the
sedimentation of these soils because 222Rn is member of the 238U decay series.
Radon is soluble in water, its solubility decreasing rapidly with an increase in
temperature (510, 230 and 169 cm3/kg at 0°C, 20°C and 30°C, respectively)
[18,19]. From the Tables 1-3 we find that the radon activity in soil varies
from a minimum of 27.35 ± 2.14 Bq m-3 to a maximum of 43 ± 3.25 Bq m-3.
222
Rn activities have been determined inside various medicinal plants
(Retama raetam, Peganum harmala and Zizyphus lotus, see Tables 1-3,
respectively) widely utilized in Moroccan traditional medicine. These
activities are different from one plant to another. It is to be noticed that roots
of each studied plant show higher radon activity than the other parts (stems
and leaves) of the plant materials.
For the species of Retama raetam and Peganum harmala, one notices that
the radon activity increases in the leaves that in the stems: In the case of these
two plants, one can write: [A c ( 222 Rn )root ] 〉 [A c ( 222 Rn)leaf] 〉 [A c ( 222 Rn)stem] .
On the other hand we noticed that the radon activity was increased in the stems of
Zizhyphus lotus that in these leaves. These results show that radon and its
daughters can be transferred from soil into plants via the root absorption. From
the Tables 1-3 we find that the radon activity in three studied medicinal plants
varies from a minimum of 8.02 ± 0.64 Bq m-3 to a maximum of 18.33 ± 1.38 Bq
m-3.
Thus, it is known that radionuclides occur naturally in soil incorporated
metabolically into plants. In addition to root uptake, direct deposition may
Radiotoxicity and medicinal plants 147

occur on foliar surfaces, and when this happens the radionuclides may be
absorbed metabolically by the plants. Uptake of the radon by plants depends
to a considerable degree on whether it remains within reach of the roots of
plants and the extent to which it is chemically available. The rates at which
the various radionuclides will migrate through different soils under varying
conditions of pH and moisture are not well known.
The radon activities in the studied soils and medicinal plants can be used
for the determination of soil-to-plant transfer factor (transfer coefficients
between soil and plants). In the literature this transfer factor (TF) is also known
as the relative concentration factor [20] or plant-soil concentration ratio [21].
Table 4 shows the data of the transfer factor of 222Rn, whereas the TF of 222Rn
decreases from the roots over stems to the leaves of Zizyphus lotus (ZL) plant.
In contrast, the TF of 222Rn increased in the leaves of Retama raetam (RR) and
Peganum harmala (PH) plants. Transfer factor values for different plants range
between 0.23 to 0.47. The reason for the high variability of soil-to-plant
transfer factors is obvious. This macroscopic parameter integrates a number of
soil chemical, soil biological, hydrological, physical and plant physiological
processes. The comparison with investigations reviewed given by IAEA
demonstrated the wide variation of obtained transfer factors, depending on
environmental conditions and selected plant species [22].
Radon-222 is an important radionuclide for the assessment of radiation
exposure to the public because of its wide distribution in the environment.
Consequently, the annual radon effective dose rates (ED) have been determined
in the studied medicinal plant samples. Data obtained is shown in Table 5.
We notice that these dose rates of 222Rn are lower in the leaves and stems
than those determined in the roots of the studied plants. It is also noticed that the
leaves have a higher dose rate than the stems in PH and RR plants. Annual radon
Table 4. 222Rn soil-to-plant transfer factors (TF).
222
Medicinal Plants Rn soil-to-plant transfer factors (dimensionless)
Root Stem Leaf
RR-1 0.46 0.23 0.40
RR-2 0.46 0.32 0.40
RR-3 0.47 0.40 0.45
PH-1 0.42 0.26 0.30
PH-2 0.43 0.37 0.40
PH-3 0.46 0.32 0.35
ZL-1 0.41 0.30 0.27
ZL-2 0.41 0.40 0.36
ZL-3 0.37 0.36 0.33
148 El Amraoui, M. et al.

Table 5. Data dose rates of 222Rn (inside) in the studied medicinal plants.

Medicinal Plants Dose rates of 222Rn (mSv.y-1)


Root Stem Leaf
RR-1 0.40 ± 0.03 0.20 ± 0.01 0.35 ± 0.02
RR-2 0.32 ± 0.02 0.22 ± 0.01 0.27 ± 0.02
RR-3 0.36 ± 0.02 0.30 ± 0.02 0.35 ± 0.02
PH-1 0.46 ± 0.03 0.29 ± 0.02 0.32 ± 0.02
PH-2 0.45 ± 0.03 0.39 ± 0.03 0.43 ± 0.03
PH-3 0.46 ± 0.03 0.32 ± 0.02 0.35 ± 0.02
ZL-1 0.37 ± 0.02 0.27 ± 0.02 0.25 ± 0.01
ZL-2 0.39 ± 0.03 0.37 ± 0.02 0.33 ± 0.02
ZL-3 0.36 ± 0.02 0.35 ± 0.02 0.32 ± 0.02

effective dose rates (ED) values are found to vary from 0.20 ± 0.01 mSv y-1 (stem
of RR-1) 0.46 ± 0.03 mSv y-1 (root of PH). Anomalous values of radon
activity and annual radon effective dose rates are not found in these three
medicinal plant samples of this area.
The objective of this study was to contribute to understanding of the
radon transfer from soil to different compartments (roots, stems and leaves)
of these three medicinal plants. The choice of this strategy is double; first, to
analyse physical characteristics of radon transfer from soil-to-plant system;
secondly, a concept of radiotoxicity evaluated by radon content of these
medicinal plants will be analyzed in this case.

Conclusion
The soil-to-plant transfer factor is an important parameter to estimate the
concentrations of radionuclides and elements in plants using a transfer model.
The transfer factor generally shows a very wide range of variation in the
elements (roots, stems and leaves) of the studied medicinal plants. Therefore,
it seems reasonable that the parameter used for the estimation of the transfer
of the nuclides should be evaluated under site-specific conditions.
The soil-to-plant transfer factor (TF) is regarded as one of the most
important parameters in environmental safety assessment needed for nuclear
facilities [22]. This parameter is necessary for environmental transfer models,
which are useful in the prediction of the radionuclide concentrations in
agricultural crops for estimating dose impacts to human. In general, transfer
factors show a large degree of variation dependent upon several factors such
as soil type, species of plants, and other environmental conditions. These
preliminary results have been used to design subsequent experiments in order
to improve our knowledge of the radon in terrestrial and aquatic ecosystems.
Radiotoxicity and medicinal plants 149

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