Distribution and environmental impact of radionuclides in marine sediments along the Venezuelan...
Transcript of Distribution and environmental impact of radionuclides in marine sediments along the Venezuelan...
Distribution and environmental impact of radionuclides in marinesediments along the Venezuelan coast
Juan A. Alfonso • Karla Perez • Daniel Palacios •
Helga Handt • John J. LaBrecque • Abrahan Mora •
Yaneth Vasquez
Received: 2 July 2013
� Akademiai Kiado, Budapest, Hungary 2014
Abstract The activity concentrations of 137Cs, 40K, 226Ra
and 232Th in Bq/kg from 42 marine sediment samples col-
lected at nine sampling sites were determined in order to
establish a radiological baseline along the Venezuelan coast.
The radioactivity levels were determined by means of a
gamma-ray spectroscopy system using a hyper-pure ger-
manium detector in a low-background configuration. Parti-
cle size distribution and total organic matter content were
also determined. Activity concentrations of 137Cs were lower
than the detection limit of the analytical technique (0.9 Bq/kg)
in all studied sites. The results suggest that the variation of
grain-size distribution is one of the most important factors
influencing the spatial variations of 40K, 226Ra and 232Th in
sediments along the Venezuelan coasts. In all sampling sites,
average concentrations of 40K, 226Ra and 232Th were lower
than the world average values. Activity concentrations of226Ra, 232Th and 40K in coastal marine sediments along the
Venezuelan coast could be considered to be low when
compared with global average values, indicating that they
are not apparently above of the range that might be consid-
ered normal or background. These results suggest that the
studied sites do not pose any significant radiological threat to
the population. The results attained in this study should be of
considerable value as baseline data and background refer-
ence levels for Venezuelan coastlines.
Keywords Natural radioactivity � Venezuelan coast �Marine sediments � Radionuclides
Introduction
Everyone on the planet is exposed to some background
level of radiation. Natural environmental radioactivity and
the associated external exposure due to gamma radiation
depend primarily on the geological and geographical con-
ditions, and appear at different levels in the soils of each
region in the world. Human exposure to ionizing radiation
is one of the scientific subjects that attract public attention,
since radiation of natural origin is responsible for most of
the total radiation exposure of the human population [1].
The natural radioactivity in beach sands come from natural
K, U and Th series. Also, artificial radionuclides such as137Cs can be present. The determination of baseline levels
of pollutants and/or contaminants in the environment is
very important because it serves as the control point for
evaluating future environmental alterations. Therefore, it is
important to determine the baseline levels of radionuclides
in the different environmental compartments before pol-
lution or contamination events happen. The measurement
of the natural radioactivity is necessary not only due to its
radiological impacts, but also because it acts as excellent
biochemical and geochemical tracer in the environment.
J. A. Alfonso (&) � H. Handt � A. Mora � Y. Vasquez
Centro de Oceanologıa y Estudios Antarticos, Instituto
Venezolano de Investigaciones Cientıficas (IVIC),
Apartado 20632, Caracas 1020A, Venezuela
e-mail: [email protected]
K. Perez
Fondo Nacional de Ciencia, Tecnologıa e Innovacion
(FONACIT), Torre Ministerial, esquina El Chorro,
Av. Universidad, Caracas, Venezuela
D. Palacios
Universidad Simon Bolıvar (USB), Apartado 89000,
Caracas, Venezuela
J. J. LaBrecque
Centro de Quımica, Instituto Venezolano de Investigaciones
Cientıficas (IVIC), Apartado 20632, Caracas 1020A, Venezuela
123
J Radioanal Nucl Chem
DOI 10.1007/s10967-014-2999-z
Radioactivity monitoring in the marine environment is
normally based on the analyses of specific nuclides in
seawater, suspended particulate matter and/or sediments. In
a marine environment, radioactive materials can be attached
to particulate matter in water. Some isotopes remain dis-
solved and are termed conservative within water. Others are
scavenged out of solution onto particulate material by
biological or chemical processes, e.g., adsorption and co-
precipitation. They may be deposited in sediments on the
bottom of the sea. Uranium and thorium radionuclides have
different behaviour in the marine environment. While ura-
nium remains dissolved in water, thorium is a particularly
insoluble element in natural waters and it is usually found
associated with solid matter [2]. The sediments play a
predominant role in aquatic radioecology. Sediments are
formed when rocks and/or organic materials are broken into
small pieces by moving water. Sediment layer settles out of
the moving water. The radioactivity contents inside the
material are normally unaffected because the breaking of a
rock into pieces does not change its chemical composition.
Sediments also play a key role in the transport and accu-
mulation of contaminants within a geographic area, thus
they can be considered as the environmental host of the
waste discharged by natural or artificial processes [3]. Only
few studies have been reported on radionuclides in sedi-
ments of Venezuela, however, such studies have only
considered a limited number of radionuclides, and have
mainly been undertaken in restricted areas. This work aims
at establishing a radiological baseline along Venezuelan
coasts, via measurement of the activity concentrations of137Cs, 226Ra, 232Th and 40K in marine sediments.
Experimental
A total of 42 coastal marine sediment samples (upper
3 cm) were collected from nine sampling sites (Fig. 1),
Paraguaipoa in the state of Zulia (site 1), Casigua, Los
Pozones and Boca de Aroa in the state of Falcon (sites
2, 3 and 4), Buche and Playa Chocolate in the state of
Miranda (sites 5 and 6), Boca de Uchire in Anzoategui
(site 7), and Mata Cuare and Isla Larga in the state of
Sucre (sites 8 and 9). After collection, each sample was
dried up at room temperature and sieved through a 2 mm
mesh-sized sieve to remove stones, pebbles and other
macro-impurities. All samples were then oven dried at a
temperature of 105 �C for 24 h to remove moisture. The
homogenized samples were then packed and sealed in an
impermeable air tight 1-L PVC container to prevent the
escape of radiogenic gases radon (222Rn) and thoron
(220Rn). About 650–700 g of sample was used for
measurements. Before measurements, the containers were
kept sealed hermetically for about 4 weeks to allow
226Ra and its short-lived decay products to reach the
secular equilibrium.
The gamma spectrometric measurements were performed
with a hyper-pure germanium (HPGe) detector with an
energy resolution of less than 1.8 keV for the 1.33 MeV
gamma-ray of 60Co and with relative detection efficiency
greater than 25 %. To reduce gamma-ray background, a
cylindrical lead shielded (100 mm thick) with a fixed bottom
and movable cover shielded the detector. The lead shield
contained an inner concentric cylinder of aluminum (0.4 cm
thick) and an outer concentric cylinder of copper (0.7 cm
thick) to absorb leads X-rays. Standard gamma-ray sources241Am, 133Ba, 137Cs and 60Co (Isotope Products Laborato-
ries, Inc.) were used to calibrate the detector energy scale. All
the samples were counted for a period of 24 h.
The activity concentrations of 137Cs, 40K, 226Ra and232Th in Bq kg-1 of dried material were determined using
the comparative method with constant geometry. Most
prominent gamma energy peaks of 295.2 and 351.9 keV
(for 214Pb); 609.31 keV (for 214Bi); 238.6 keV (for 212Pb);
911.07 keV (for 228Ac); 1,462 keV (for 40K) and
661.6 keV (for 137Cs) were considered for activity con-
centration calculations. 226Ra concentration was deter-
mined from the average concentrations of 214Bi and 214Pb,
while 232Th concentration from the average concentrations
of 212Pb and 228Ac. Full energy peak efficiencies for
coastal marine sediment matrices were determined by
RGU-1, RGTh-1, RGK-1, SOIL-6 and SL-2 reference
materials (International Atomic Energy Agency IAEA,
Vienna, Austria). The reference materials and silica blank
were prepared and measured the same as the samples. The
detection limits of 137Cs, 40K, 226Ra and 232Th for this
method were determined to be 0.9, 2, 1.8 and 1.4 Bq kg-1,
respectively. The detection limits were calculated as 4.66
times the square root of the background counts for the
respective gamma-ray.
Granulometric analysis provides basic information for
the geochemical investigations of marine sediments and
was carried out by laser granulometry (Mastersizer 2000
particle size analyzer, Malvern Instruments Ltd.) to
measure particles in the 4–2,000 lm size range [4]. Total
organic matter content was determined by ignition at
550 �C [5]. Particle size distributions and total organic
matter content were determined on one representative
sample of each sampling site. Radiological indices such
as radium equivalent activity (Raeq) and absorbed dose
rate (D) were also calculated.
Results and discussion
The average activity (Bq kg-1) values of 137Cs, 40K, 226Ra
and 232Th in coastal marine sediment from the nine
J Radioanal Nucl Chem
123
sampling sites are presented in Table 1. The calculated
values for granulometric analysis and total organic matter
content are presented in Table 2.
It can be seen in Table 1, that the nine sampling sites
had coastal marine sediments with 137Cs activities lower
than the detection limit of 0.9 Bq kg-1. Our results
suggest that little if any 137Cs fallout from the atmo-
spheric nuclear weapon test was found in these marine
sediments. It should be noted that anomalous levels, as
high as 140 Bq kg-1 of 137Cs fallout were reported to
have been measured in surface soils of the tropical cloud
forests in the island of Margarita (Venezuela) [6]. But, it
does not seem that any significant amount of this 137Cs
has been transported by man or nature to estuaries or
coastal waters. The baseline levels of 137Cs reported
herein for coastal marine sediments are very similar to
the reported in coastal marine sediments of Margarita
Island [7] and Los Roques archipelago [8] with values
B1.0 Bq kg-1.
The range of measured natural radionuclide concentra-
tions differed widely as their presence in marine environ-
ment depends on their physical, chemical and geochemical
Fig. 1 A map of the
Venezuelan coast showing the
sampling sites
Table 1 Average concentration
and standard deviation values of137Cs, 40K, 226Ra and 232Th in
the studied sites
Sampling
site
Number
of samples
137Cs
(Bq/kg)
40K
(Bq/kg)
226Ra
(Bq/kg)
232Th
(Bq/kg)
1 4 \0.9 168.3 ± 30.7 5.8 ± 3.1 9.0 ± 4.3
2 4 \0.9 51.2 ± 19.1 7.2 ± 4.3 8.5 ± 5.7
3 4 \0.9 45.2 ± 12.7 4.8 ± 2.0 6.7 ± 3.1
4 5 \0.9 150.7 ± 27.6 8.6 ± 4.8 12.9 ± 7.7
5 5 \0.9 318.4 ± 42.0 23.7 ± 8.5 31.7 ± 9.6
6 5 \0.9 257.3 ± 28.9 18.4 ± 5.5 20.3 ± 4.0
7 4 \0.9 27.8 ± 11.1 3.7 ± 0.8 5.6 ± 1.0
8 5 \0.9 75.5 ± 22.0 11.0 ± 7.0 14.7 ± 7.6
9 6 \0.9 286.5 ± 38.3 19.4 ± 8.1 22.3 ± 4.4
Table 2 Sediment texture (coarse sand, fine sand, silt and clay
content) and total organic matter content in representative sediment
samples of each studied site
Site Clay
(%)
Silt
(%)
Fine sand
(%)
Coarse sand
(%)
Total organic
matter (%)
1 0 0 99.0 1.0 5.3
2 0 0 10.6 89.4 3.5
3 0 1.4 38.5 60.1 7.4
4 0 0 80.5 19.5 5.8
5 2.4 9.6 26.4 61.5 26.6
6 0 2.6 91.1 6.3 8.6
7 0 0 4.6 95.4 3.9
8 0.2 2.7 18.3 78.7 7.8
9 1.0 3.4 47.4 48.2 11.1
J Radioanal Nucl Chem
123
properties and the pertinent environment [9]. In all sam-
pling sites, mean activity concentration is of the order40K [ 232Th [ 226Ra. 232Th concentration is found to be
higher than 226Ra concentration in all the sampling sites
along the Venezuelan coast. This may be due to the low
geochemical mobility and insoluble nature in water of
thorium. The 40K activity concentration dominates over226Ra and 232Th elemental activities like what normally
happens in soil [1].
From Table 1 one can see that the highest mean
activities of 40K, 226Ra and 232Th are found in Buche
(site 5), whereas the lowest mean activities are found in
Boca de Uchire (site 7). The obtained results (Tables 1, 2)
showed that, the lowest mean values were found in
sandy sediments, while the highest mean values were
found in sandy loam sediments. This can be attributed to
the difference in grain size texture. The radionuclide
activity concentrations increase as the particle size
decrease, because of the increase in surface area per unit
of mass [10, 11]. The increase and decrease of radio-
nuclides in soil and sediment samples are also affected
by the amount and composition of the organic matter
content, adsorption kinetics and the pH of the medium
[11]. The results show that the mean activity concen-
trations of 40K, 226Ra and 232Th are higher in the site 5,
where the total organic matter content is highest. Buche
(site 5), is an estuary located to the west of the mouth of
the Tuy River, which has a plume known to move in a
northwesterly direction and receives waste water efflu-
ents from the metropolitan area of Caracas, via the
Guaire River [12]. Desorption of radium from estuarine
sediments is enhanced by the combined effects of low
pH and high salinity [11]. Characteristics of environ-
mental radioactive particles, i.e. activity and atom/activ-
ity ratios, are related to the origin, whereas properties
such as size distribution, share, crystalline structures, and
oxidation states of matrix elements depend on the spe-
cific conditions of the release mechanisms [14].
While a plot of one radionuclide activity concentration
against another (or a calculation of a correlation coefficient)
can be used to deduce some conclusions about the coexis-
tence of the radionuclides, these correlations should not be
mistaken for actual chemical interactions among the ra-
dionuclides [15]. In the present data set, 226Ra shows a very
good linear correlation with 232Th (Fig. 2). This fact sug-
gests that both thorium and uranium series nuclides are
probably associated with the same mineral fraction [15, 16]
along the Venezuelan coast. The natural radionuclides
concentrations found in this study are within the range or
are very slightly higher than those previously reported for
coastal marine sediments and soils in Venezuela [7, 8]. In
all sampling sites, average concentrations of 40K, 226Ra and
232Th in the sediments, are lower than worldwide mean
values (worldwide mean of 226Ra, 232Th and 40K is 35, 30
and 400 Bq/kg, respectively [1, 18]). Only one sample of
the site 5 has a value slightly higher than world average of232Th. A comparison of radionuclide activities in the sedi-
ment of the studied sites and in other coastal and aquatic
environments is given in Table 3. Concentrations in coastal
marine sediments along the Venezuelan coast can be
interpreted to be low on a global scale for 226Ra, 232Th and40K, indicating that they are not apparently above of the
range that might be considered normal or background.
The absorbed dose rate is the first major step for eval-
uating the health risk. With regard to biological effects, the
radiological and clinical effects are directly related to the
absorbed dose rate. The measured activity concentrations
of 226Ra, 232Th and 40K are converted into doses by
applying the conversion factors 0.462 nGy/h for 226Ra,
0.604 nGy/h for 232Th and 0.0417 nGy/h for 40K [1]. These
factors are used to calculate the absorbed dose rate D (nGy/h)
due to radiations in air at 1 m above the ground surface,
using the following equation:
D ¼ 0:462CRa þ 0:604CTh þ 0:0417CK ð1Þ
where CRa, CTh and CK are the activity concentrations (Bq/kg)
of 226Ra, 232Th and 40K in sediment samples, respectively.
Radium equivalent Raeq (Bq/kg) is a convenient index to
describe the gamma output from different mixtures of
radium, thorium and potassium in the sediments sampled
from different locations. It is a widely used hazard index
and it is defined based on the assumption that 10 Bq/kg of226Ra, 7 Bq/kg of 232Th and 130 Bq/kg of 40K produce the
same gamma dose. It is calculated using the Eq. (2) [2, 11]:
Raeq ¼ CRa þ 1:43CTh þ 0:077CK ð2Þ
where CRa, CTh and CK are the activity concentrations (Bq/kg)
of 226Ra, 232Th and 40K in sediment samples, respectively.
The D and Raeq calculated values for our sampling sites are
0
5
10
15
20
25
30
35
0 5 10 15 20 25
232 T
h (B
q/K
g)
226Ra (Bq/Kg)
r = 0.98
Fig. 2 Scatter plot of 226Ra versus 232Th in the studied sites with
linear regression line showing positive correlation
J Radioanal Nucl Chem
123
presented in Table 4. Average absorbed dose rate (D) for
all samples is lower than the world average value (57 nGy/h)
[1]. The estimated average values of Raeq are lower than
the recommended maximum value of 370 Bq/kg for the
safe use of materials in the construction of buildings [1].
Therefore, the sites studied do not pose any significant
radiological threat to the population. The results attained in
this study should be of considerable value as base line data
and background reference level for Venezuelan coastlines.
Conclusions
All of our values for 137Cs in the studied coastal sediments
were lower than our detection limit of 0.9 Bq kg-1 dry
weight. The highest mean activities of 40K, 226Ra and 232Th
are found in Buche, whereas the lowest mean activities are
found in Boca de Uchire. Our results suggest that the
variation of grain-size distribution is one of the most
important factors influencing the spatial variations of 40K,226Ra and 232Th in sediments along the Venezuelan coasts.
The high correlation found between 226Ra and 232Th sug-
gest that both thorium and uranium series nuclides are
probably associated with the same mineral fraction in the
studied sites. The natural radionuclides activity concen-
trations found in this study are within the range or are very
slightly higher than those previously reported for coastal
marine sediments and soils in Venezuela. In all sampling
sites, average concentrations of 40K, 226Ra and 232Th are
lower than world average values. Concentrations in coastal
marine sediments along the Venezuelan coast can be
interpreted to be low on a global scale for 226Ra, 232Th and40K, indicating that they are not apparently above of the
range that might be considered normal or background. Our
results suggest that the studied sites do not pose any sig-
nificant radiological threat to the population. The results
attained in this study should be of considerable value as
base line data and background reference level for Vene-
zuelan coastlines.
Acknowledgments This work was supported by the FONACIT-
Venezuela. We thank Carlos Bastidas and Juan M. Carrera for their
assistance.
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