transfer of 137cs and 60co from irrigation water to a soil–tomato plant system
TRANSCRIPT
Transfer of 137
Cs and 60
Co from irrigation water to a soil-tomato plant system
C. Sabbarese1,*
, L. Stellato1, M.F. Cotrufo
1, A. D'Onofrio
1,
A. Ermice1, F. Terrasi
1, S. Alfieri
2
(1)
Dipartimento di Scienze Ambientali, Seconda Università di Napoli, via Vivaldi, 81100
Caserta, Italy (2)
Centrale Nucleare Garigliano, Sogin, Sessa Aurunca (Caserta), Italy * Corresponding author. E-mail: [email protected]
Abstract
An experiment has been performed at the Nuclear Power Plant of Garigliano (Caserta, Italy),
aiming to the measurement of transfer factors of 137
Cs and 60
Co radionuclides from the irrigation
water to a soil-plant system, with particular attention to the influence on such transfers of the
irrigation technique (ground or aerial). Tomato plants were irrigated weekly with water
contaminated with 137
Cs and 60
Co (about 375 Bq/m2 week), using both irrigation techniques. After
13 weeks fruits, leaves, stems, roots and soil were sampled, and radionuclide concentrations were
measured by high-resolution spectroscopy. It was found that the activity allocated to the plant
organs is significantly dependent upon the irrigation technique, amounting to 2.1% and 1.6% for
aerial treatment and 0.4% and 0.3% for the ground treatment, for 137
Cs and 60
Co respectively. The
activity absorbed by plants is allocated mainly in leaves (>55%), while less then 10% is stored in
the fruits, for both irrigation techniques. Transfer factors (soil-plant and irrigation water-plant) of
tomato plants and of weeds have been determined for 137
Cs and 60
Co, as well as for natural 40
K in
the soil.
Keywords: Radionuclide transfer factor; Foliar and ground sorption; tomato
1. Introduction
Assessment of internal doses to humans from ingestion of radionuclides present in
agricultural products requires detailed information on the main processes determining the route of
radionuclides in the environment (Russel, 1966; Peterson, 1983; IAEA, 1995). A large amount of
data is available but, generally, they do not reflect natural conditions, and the mechanisms of
translocation and mobility of radionuclides within the soil-plant system are still not understood
(Fresquez et al., 1998; Krouglov et al., 1997; Howard et al., 1995; Strand et al., 1994; Konshin,
1992; Frissel, 1992; Alexakhin & Korneev, 1992; Desmet et al., 1990).
The knowledge of the contributions of direct contamination of plant fruits and of the process
of root to fruit transfer can improve the understanding of exposure through ingestion and of the
mechanisms determining sorption and translocation. Agricultural soil can be contaminated because
of radioactive fallout in atmosphere or because of irrigation which uses contaminated water. Plants
growing on that soil absorb radionuclides by roots and/or by leaves. Radionuclides absorbed are
transferred to the plant organs and their quantities are determined on the basis of the kind of
contamination source and of biological and environmental processes. Plant physiology, soil
characteristics, nuclide and plant kind are important parameters which influence sorption (Howard
et al.,1995; Strand et al.,1994; Konshin,1992).
Few studies have been designed considering real agricultural conditions and very few
simulate a contaminated rain which daily falls on the plants or on soil surface only. In the present
research, both kinds of contaminations have been studied in experimental conditions very close to
the real-life situation. Transfer factors have been calculated considering the weekly increase of
contamination in soil and the increase of plant mass.
2. Materials and methods
An experimental field, 25x30 m long, was arranged in the soil area of the Nuclear Power
Plant of Garigliano (Caserta, Italy) to perform the experiment. The field was on anthropogenic soil
characterized by morphological heterogeneity and spatial discontinuity, suggesting variability in its
properties. After adequate soil preparation and fertilization, the field was divided in 30 plots as
displayed in Fig. 1. Tomato plants were cultivated in the same conditions in 24 plots, 2x2 m2: 12
(named P) were contaminated using a low radioactivity water solution containing 137
Cs and 60
Co,
while the other 12 plots (named B) were not contaminated and used as blank reference. The
remaining 6 plots were also contaminated but not cultivated (named S) to obtain a control of
uncultivated soil. The 12 P-plots were divided in two groups of 6 plots named P1 and P2, and, at the
same way, B1 and B2 for B plots. The indices 1 and 2 indicate irrigation at rain and at foot
respectively. Hence, five different groups of plots with different cultivation kinds were performed:
B1: irrigation at rain using uncontaminated water;
B2: irrigation at foot using uncontaminated water;
P1: irrigation at rain using contaminated water,
P2: irrigation at foot using contaminated water,
S: irrigation of nude soil using contaminated water.
Each plot was irrigated weekly using 80 l of water with or without contamination as before
explained. Water due to natural rain, eventually present during the week, was measured and
subtracted from 80 l; hence, in each week supplemented water quantity was variable but the
contamination quantity was the same.
The contamination solution was obtained from two radioactive sources produced by
Amersham International containing 2 MBq of 137
Cs and 60
Co respectively. Contaminant solution
used for irrigation was homemade in acid environment and on April 7h, 1998 contained (0.31
0.02) kBq/ml of 137
Cs and (0.30 0.02) kBq/ml of 60
Co. Weekly, 5 ml of such solution were used
for irrigation of each plot. At the end of cultivation, 13 weeks long, each plot received (19.9 1.7)
kBq of 137
Cs and (19.5 1.7) kBq of 60
Co, and the entire experimental field received about 700
kBq (19 Ci). It is worth to emphasise that such activity represents 0.00019% of dumping liquids of
the Nuclear Power Plant of Garigliano; hence, the environmental impact was practically zero.
After 13 weeks of cultivation, tomatoes, leaves, stems, roots and soil of the entire
experimental field were collected, separated per plot, disposed in containers and exposed to the sun
for two days. Tomatoes were separated in ripe and unripe and were analysed separately; as no
significant difference was found between the two categories, we have analysed the data without
distinction between ripe and unripe. Each part of the plants was placed in oven at 60°C for 36 h and,
then, at 105 °C for 12 h to obtain a satisfactory sample dehydration. Samples removed from oven
were pulverized to obtain a homogeneous matrix, which was weighted and placed in a 350 cc
Marinelli beaker. Root samples were placed in 80 cc volume cylindrical containers because of the
small amounts available. Also weed growled in the plots was collected and analysed using the same
procedure of tomato plants.
Soil samples were collected in 30x30 cm2 cores, 20 cm deep from six contaminated plots
(S1, S2, P11, P15, P23, P24). Four samples of 5 cm long sections of soil cores of each plot were
considered. They were placed in oven at 60°C for 36 h and 12 h at 105 °C, were sieved at 2 mm and
placed in 2.8 l Marinelli beaker. Moreover, in the P15 plot six soil cores were collected at different
positions to study the variability of radionuclide concentration.
Soil density was also determined in six plots, which were representative of the entire
experimental field. Samples were extracted by using 270 cc volume metallic cylinders, which are
opened at two bases. Soil captured by cylinders was oven-heated and its mass was determined to
calculate dry bulk density.
High-resolution -spectrometry was used to measure radionuclide activities of the vegetable
and soil samples. Two germanium hyperpure detectors (1.9 keV resolution and 30% efficiency)
properly shielded were used with standard electronics: spectra were analysed, displayed and stored
using a computer.
Total efficiencies for each detection geometry were experimentally determined by using the
same matrix contaminated in a uniform way by a polinuclides source produced by Amersham
International. Radionuclide specific activities were obtained from a quantitative analysis of -ray
spectra using the lines at 661.6 keV (137
Cs), 1173.2 keV and 1332.5 keV (60
Co). Analysis results
yield specific activity of each detected radionuclide referred to dry mass.
As potassium and caesium elements have similar chemical characteristics, and potassium
radionuclide (40
K ) is naturally present in the soil, we analysed also the 40
K peak (1460.5 keV)
present in -ray spectra and we calculated its specific activity too.
3. Results and discussion
Data analysis was performed by dividing data per plant organs: tomatoes, leaves, stems, and
roots. Then, we compared results obtained on the same organ of the six plots of the same treatment.
Table I shows 137
Cs, 60
Co and 40
K specific activities of the plant organs of all plots. The variations
of these values measured on the same organ and for the same treatment show variations in the six
repetitions larger than the respective experimental errors. For this reason, sample standard
deviations in each group were taken as representative of the variability of experimental conditions.
In Fig. 2 mean values and standard errors of measured specific activities are reported for the plant
organs of two treatments.
Specific activities of uncontaminated plant organs are negligible with respect the
corresponding contaminated ones, while differences of 137
Cs and 60
Co results between two
irrigation techniques are statistically significant at 95% confidence level, as indicated by the student
t-test. It is evident from the results that the procedure of irrigation influences strongly the sorption
of radionuclides: the aerial irrigation (P1-plots) furnishes a quantity of radionuclides higher than the
ground irrigation (P2-plots). The 40
K values are not different between the two irrigation techniques
as expected. In the Table II the ratios between P1 and P2 specific activities for each plant organ and
each radionuclide are reported.
The relative distribution of mean specific activities among plant organs has been displayed
in Fig. 3. No significant difference appears between two irrigation techniques; in effect, percentage
values are about the same for P1 and P2. This fact indicates that plants not distinguish between the
two ways of sorption and they distribute the absorbed quantity of radioactivity in the same way. 40
K
distributions in the plant organs are similar in the P1, P2, B1 and B2 plots, but they are very
different from the distributions of artificial radionuclides. Tomatoes contain about 60% of 40
K of
plant, stems and roots contain a percentage about equal for 137
Cs and 60
Co ones. In conclusion, 40
K
is especially allocated in fruits and 137
Cs and 60
Co are allocated especially in leaves, independently
of treatment, as shown by Smolders & Merckx (1993) for hydroponic cultivation.
To obtain data of direct human interest, we have calculated also specific activities referred to
fresh mass of tomato. Such mean specific activities of fresh mass are (3.0 0.5)Bq/kg and
(0.4 0.1) Bq/kg for 137
Cs, (1.1 0.2) Bq/kg and (0.2 0.1) Bq/kg for 60
Co for P1 and P2
treatments, respectively and (75 6) Bq/kg for 40
K.
Weed growled during the cultivation in the plots was also collected and analysed. Mean
specific activities of 137
Cs and 60
Co measured in weed samples show no differences within the
measurement errors for the two treatments, as expected, due to the small weed height above ground
(Table I).
To calculate transfer factors from soil to plants, specific activities of 137
Cs, 60
Co and 40
K in
the upper 20 cm of soil have been measured. Mean specific activities are (22 2) Bq/kg, (21 2)
Bq/kg and (1080 96) Bq/kg for 137
Cs, 60
Co and 40
K, respectively. About 80% of the activity
present in the soil is detained in the upper 5 cm. The aerial variability of radionuclide distributions
is characterised by a standard deviation of about 20%.
Using the mean density of analysed soils of six plots (1.15 0.08) g/cm3, total activities
detained in the upper 20 cm of each plot of (5.1 0.9) kBq/m2, (4.8 0.8) kBq/m
2 and (250 66)
kBq/m2 for
137Cs,
60Co and
40K are in agreement with total activity given to the plot through water
(5.0 0.9 kBq/m2 of
137Cs, 4.9 0.9 kBq/m
2 of
60Co). The resulting transfer factors, calculated as
ratios of the plant specific activity to the soil aerial activity at the end of the experiment (i.e. 13
weeks) are reported in Table III for P2 treatment. In order to compare the two kinds of treatment,
the transfer factors from irrigation water to plant was also calculated for P1 and P2 plots and are
reported in Table II, where are also reported transfer factors from irrigation water to weed.
Coming back to soil-plant transfer, one may note from Table III that 137
Cs has a transfer
factor large by a factor about 2 with respect to 40
K. The average 137
Cs to 40
K specific activity ratio
in the soil is 0.029. On the other hand, if one considers the individual transfers to different plant
organs, one can see from the data in Table IV that the 137
Cs to 40
K discrimination is strongly
dependent on the compartment considered.
4. Correction of the transfer factor.
The transfer factors obtained above have been calculated assuming that the total amount of
radionuclides was present in soil from the beginning of cultivation without considering its weekly
increase due to the contaminated irrigation water. Hence, the transfer factors reported in the Table
III are not comparable with those measured in conventional experiments performed in soils fully
contaminated before plantation. In order to correlate the two approaches we consider the differential
equation which describes the increase of the activity in the tomato plants as a function of the
activity in the soil (Somlders & Merckx, 1993). If we neglect the decrease of activity due to the
radioactive decay and we assume an exponential behavior of plant growth (constant value of
relative growth rate, RGR), the variation of the specific activity in the plant, C, is
)1()()( tCRGRtUdt
dC
where U (t), expressed in Bq/kg/d, is the increase of radionuclide activity at constant mass per mass
unit and RGR is the relative growth rate of plant per mass unit expressed in d-1
. If U(t) and RGR
are considered constants, the solution of the equation (1) is
where U/RGR is the asymptotic value of the specific activity absorbed from the plant and it is equal
to F*Cs, where F is the soil-plant transfer factor and Cs is the specific activity of radionuclide in the
soil. Hence,
In our experiment Cs(t) is linearly increasing with time and it can be expressed as
tktCs
)( , with **)( ttCk s and t* the time at the end of the experiment.
The solution of eqn. (1), in this case, is
where
The transfer factor F (eq. (4)) has to be compared with the transfer factor Fc calculated
neglecting the time dependence of soil contamination, i.e. normalizing the specific activity at time
t*, C(t
*), to the total activity supplied to the soil during time t
*, Cs (t
*):
)()()(
)(*
*
**
**
tf
tRGRF
tftC
tRGRtCF c
s
In our cultivation, we calculated C(t*) from the average specific activities of the six plots of
the same treatment at the end of cultivation (t = 92 d, RGR = 0,051 d-1
and k = 54 Bq/g/m2 for
)2(1)( RGRteRGR
UtC
)3(sCRGRFU
)4()()(
)(*
*
tftRGR
tCFtC s
tRGRetf tRGR 1)(
137Cs and k = 53 Bq/g m
2 for
60Co). To correct the transfer factors calculated above, the following
expression
)( ** tftRGRFF c
can be used.
The soil-tomato plant and soil-weed transfer factors calculated with this formula are 0.014
Bq/g m2 and 0.011 for
137Cs and
60Co, respectively. This correction increases values of about 27%;
accounting for the fact that the entire quantity of radionuclides was not available to plants from the
beginning of the cultivation. If one takes into account that uptake efficiency is in fact decreasing
with plant growth (Sabbarese et al., 2000), the correction factor can be expected to be larger.
5. Conclusions
The experiment presented, regarding tomato plant cultivation in an agricultural soil with
irrigation water containing 137
Cs and 60
Co, allowed to conclude that tomato plants absorb less than 2
% of the activity available in the soil. This quantity is about 6 times higher if contaminated
irrigation was aerial with consequent foliar absorption. In effect, the ground irrigation reduces by
about 80% the absorption of radionuclides from plant. Relative distributions of radionuclide in the
organs of tomato plants are not different for the two treatments. In both treatments, more than 90%
of the entire activity of plant was absorbed by steams and leaves, and the remaining activity is
distributed between fruit and root. Otherwise, the 40
K activity distribution is very different from the
artificial radionuclides. Transfer factors are also calculated for tomato plants and for weed with
respect to irrigation water and to soil contamination for 137
Cs, 60
Co and 40
K.
Acknowledgements
The authors are grateful to technical operators of the Nuclear Power Plant of Garigliano
which participated to the experiment, and they thank, in particular, Mr. G. Fiore for its continuous
attention for cultivation.
References
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Konshin, O.V. (1992). Transfer of 137
Cs from soil to grass: Analysis of possible sources of
uncertainity. Health Physics., 63, 307-315.
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transfer of 137
Cs and 90
Sr from Chernobyl-contaminated soils to grain crops. Journal of
Environmental Radioactivity, 34, 3, 267-286.
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(ed.), Radiological Assessment: A Textbook on Environmental Dose Analysis. U.S. Nuclear
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Russel R.S. (1966). Radioactivity and Human Diet. Pergamon Press, Oxford.
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Smolders E., R. Merckx, (1993). Some principles behind the selection of crops to minimize
radionuclide uptake from soil. The Science of the Total Environment, 137: 135-146.
Strand, P., P.J. Howard, L. Skuterud, V. Averin (1994). Fluxes of radionuclides in rural
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Figure and Table Captions
Figure 1. Experimental field scheme, with indications of the five treatments.
Figure 2. Mean specific activities divided for radionuclide and for plant organ are reported for each
treatment.
Figure 3. Percentage distribution of mean specific activities among plant organ for each analysed
radionuclide.
Table I. Specific activities of 137
Cs, 60
Co and 40
K, expressed in Bq/Kg, measured in all vegetable
samples of the present experiment.
Table II. Ratios between the specific activities of three radionuclides studied in two cultivation
treatments (P1 and P2).
Table III. Transfer factors calculated in the described experiment.
Table IV. Ratios of 137
Cs to 40
K specific activities in plant organs are reported with respect the
correspondent average ratio in the soil.
P1 P2 B1 B2
137Cs 60Co 40K 137Cs 60Co 40K 137Cs 60Co 40K 137Cs 60Co 40K
T
O
M
A
T
O
82 2 36 1 1524 41 5.6 0.2 4.7 0.3 1466 41 1.6 0.2 < 0.1 1857 47 0.7 0.2 < 0.1 1310 34
63 1 27 1 1314 40 8.2 0.2 4.6 0.4 1560 49 0.9 0.2 < 0.1 1404 37 0.5 0.2 < 0.1 1219 32
65 1 19 1 1411 49 6.6 0.2 1.4 0.2 1518 42 0.9 0.2 < 0.1 1555 41 0.3 0.1 < 0.1 1114 29
47 1 16 1 1272 39 9.8 0.2 4.5 0.4 1513 43 0.5 0.2 < 0.1 1104 29 0.6 0.2 < 0.1 1288 34
57 1 17 1 1646 45 5.4 0.2 2.6 0.2 1497 42 0.7 0.2 0.8 0.2 1428 37 0.2 0.1 < 0.1 1397 36
46 1 14 1 1450 42 9.4 0.3 2.2 0.2 1460 42 0.9 0.2 0.8 0.1 1303 35 < 0.1 < 0.1 1303 34
S
T
E
M
343 9 266 7 1034 38 48 12 31 8 1215 39 2.1 0.3 < 0.1 1381 39 0.5 0.3 < 0.1 1140 31
438 11 283 7 1147 31 38 2 24 1 1137 40 1.7 0.3 < 0.1 957 29 0.5 0.3 < 0.1 1108 30
224 6 161 5 951 35 62 1 38 1 1435 44 1.3 0.3 < 0.1 938 27 < 0.1 < 0.1 1062 29
350 9 201 5 934 28 55 1 38 1 799 23 < 0.01 < 0.1 989 29 < 0.1 < 0.1 927 38
246 7 164 5 746 30 33 1 25 1 969 33 1.3 0.3 < 0.1 1027 29 < 0.1 < 0.1 786 22
373 10 228 6 1057 31 93 3 52 2 742 26 < 0.01 < 0.1 807 25 < 0.1 < 0.1 776 22
L
E
A
V
E
1269 31 1136 27 695 26 121 3 101 3 726 25 2.4 0.2 < 0.1 747 20 4.3 0.3 4.9 0.3 697 21
1040 25 851 20 710 25 227 6 167 5 847 28 1.7 0.2 0.8 0.1 675 19 2.6 0.3 < 0.1 713 22
750 18 670 17 688 24 174 5 138 4 1006 33 2.1 0.3 < 0.1 647 19 2.5 0.3 < 0.1 730 22
840 20 624 15 596 22 131 4 104 3 486 22 1.1 0.3 1.0 .2 653 19 1.9 0.3 < 0.1 645 19
841 20 661 16 620 23 149 4 114 3 498 22 2.1 0.2 < 0.1 658 19 1.8 0.3 < 0.1 532 17
759 18 585 14 653 23 339 9 240 7 456 20 1.4 0.3 < 0.1 464 16 1.7 0.3 < 0.1 535 17
R
O
O
T
95 8 139 10 1296 99 46 4 76 6 886 77 < 0.2 < 0.2 < 0.2 < 0.2 < 0.2 751 69
56 5 101 8 1294 100 21 2 40 3 1525 116 < 0.2 < 0.2 1298 121 < 0.2 < 0.2 1321 101
90 7 150 11 1434 110 23 3 43 4 1335 103 < 0.2 < 0.2 1351 104 < 0.2 < 0.2 1492 113
76 6 115 9 1255 96 13 3 36 3 1177 91 < 0.2 < 0.2 469 61 < 0.2 < 0.2 1266 97
27 3 50 4 302 54 31 3 67 5 1466 112 < 0.2 < 0.2 787 73 < 0.2 < 0.2 1336 102
63 6 117 9 785 73 34 4 75 6 1001 79 < 0.2 < 0.2 1304 100 < 0.2 < 0.2 1354 104
W
E
E
D
552 481 86324 432 422 90135 0.30.2 < 0.2 340 11 < 0.2 < 0.2 751 69
742 692 121232 432 341 87429 0.60.5 0.30.2 918 27 < 0.2 < 0.2 1321 101
312 291 85994 312 251 49323 1.70.3 < 0.2 1003 28 < 0.2 < 0.2 1492 113
344 331 101135 422 492 97032 < 0.2 < 0.2 705 21 < 0.2 < 0.2 1266 97
381 391 90425 181 191 97533 < 0.2 < 0.2 821 24 < 0.2 < 0.2 1232 94
171 161 84731 492 612 86030 < 0.2 < 0.2 536 21 < 0.2 < 0.2 1354 104
Table I
PLANT ORGANS 137
Cs 60
Co 40
K
TOMATOES 8.0 1.1 6.5 1.5 0.96 0.04
STEMS 6.0 1.1 6.2 1.0 0.93 0.11
LEAVES 4.8 0.9 5.3 1.0 0.99 0.14
ROOTS 2.4 0.6 2.0 0.4 0.86 0.16
Table II
TRANSFER FACTOR CULTIVATION
TREATMENT
137Cs
60Co
40K
Soil – Tomato Plant
(Bq/kg/Bq/m2)
P2 0.011 0.002 0.009 0.002 0.005 0.001
Soil –Weed (Bq/kg/Bq/m2) P1, P2, S 0.007 0.001 0.007 0.001 0.004 0.001
Irrigation Water – Tomato
Plant (Bq/kg/Bq/l)
P1 15 2 11 2 -
P2 3.0 0.7 2.2 0.6 -
Irrigation Water –Weed
(Bq/kg/Bq/l) P1, P2, S 1.9 0.2 1.7 0.2 -
Table III
P2 PLANT ORGANS (137
Cs/40
K)plant/(137
Cs/40
K)soil
TOMATOES 0.17
STEMS 1.81
LEAVES 9.83
ROOTS 0.79
WEED 1.54
Table IV
1 2 3 4 5 6
B1: irrigation at rain usinguncontaminated water
B2: irrigation at foot usinguncontaminated water
P1: irrigation at rain usingcontaminated water
P2: irrigation at foot usingcontaminated water
S: irrigation of nude soil atrain using contaminatedwater
P1 TREATMENT
1
10
100
1000
10000
TOMATOES STEMS LEAVES ROOTS
SP
EC
IFIC
AC
TIV
ITY
(B
q/k
g) Cs-137 Co-60 K-40
P2 TREATMENT
1
10
100
1000
10000
TOMATOES STEMS LEAVES ROOTS
SP
EC
IFIC
AC
TIV
ITY
(B
q/k
g) Cs-137 Co-60 K-40
B1 TREATMENT
0,1
1
10
100
1000
10000
TOMATOES STEMS LEAVES ROOTS
SP
EC
IFIC
A
CT
IVIT
Y (B
q/k
g) Cs-137 Co-60 K-40
B2 TREATMENT
0,1
1
10
100
1000
10000
TOMATOES STEMS LEAVES ROOTS
SP
EC
IFIC
A
CT
IVIT
Y (B
q/k
g) Cs-137 Co-60 K-40