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The present study was carried out along the coastal regions of Tuticorin, Tamilnadu,
India, to evaluate the distribution of uranium, thorium and potassium concentrations in surface
soil samples. A total of 5 soil samples were collected from 5 sea shores, lying by the side of
the Sea. The activity concentrations of natural radionuclides 238U, 232Th and 40K were measured
and an average of 2.9957 Bqkg-1, 91.552 Bqkg-1 and 299.708 Bqkg-1. The radium equivalent
activities in the beach sands of Tuticorin district varies from 54.804 Bqkg-1 to 324.991 Bqkg-1,
which is lower than the reference limit of 370 Bqkg-1. Results show that the radiological
parameters obtained for the beach sand from the Tuticorin district of are within the safe limits
and hence these places can be considered as Normal Background Radiation Areas. The areas
with high radiological parameters are within the safe limit with respect to radiological index.
The absorbed dose rate of the district ranged from 25.5 nGyh-1 to 138.0985 nGyh-1 with an
average value of 69.1795 nGyh-1 which is also under safe limits.
1
CHAPTER I
2
INTRODUCTION
1.1.Radioactivity:
Radioactivity is a property exhibited by certain types of matter of emitting energy and
subatomic particles spontaneously. An unstable nucleus will decompose spontaneously, or
decay, into a more stable configuration but will do so only in a few specific ways by emitting
certain particles or certain forms of electromagnetic energy. Radioactive decay is a property of
several naturally occurring elements as well as of artificially produced isotopes of the elements.
The rate at which a radioactive element decays is expressed in terms of its half-life; i.e., the
time required for one-half of any given quantity of the isotope to decay. Half-lives range from
more than 1024 years for some nuclei to less than 10−23 second. The product of a
radioactive decay process called the daughter of the parent isotope may itself be unstable, in
which case it, too, will decay. The process continues until a stable nuclide has been formed.
The emissions of the most common forms of spontaneous radioactive decay are
the alpha (α) particle, the beta (β) particle, the gamma (γ) ray, and the neutrino. The alpha
particle is actually the nucleus of a Helium-4 atom, with two positive charges. Such charged
atoms are called ions. The neutral helium atom has two electrons outside its nucleus balancing
these two charges. Beta particles may be negatively charged or positively charged. The beta
minus [β−] particle is actually an electron created in the nucleus during beta decay without any
relationship to the orbital electron cloud of the atom. The beta plus particle, also called
the positron, is the antiparticle of the electron; when brought together, two such particles will
mutually annihilate each other. Gamma rays are electromagnetic radiations such as radio
waves, light, and X-rays. Beta radioactivity also produces the neutrino and antineutrino,
particles that have no charge and very little mass, symbolized by ν and ῡ, respectively.
In the less common forms of radioactivity, fission fragments, neutrons, or protons may
be emitted. Fission fragments are themselves complex nuclei with usually between one-third
and two-thirds the charge Z and mass A of the parent nucleus. Neutrons and protons are the
basic building blocks of complex nuclei, having approximately unit mass on the atomic scale
and having zero charge or unit positive charge, respectively. The neutron cannot long exist in
the free state. It is rapidly captured by nuclei in matter; otherwise, in free space it will undergo
beta-minus decay to a proton, an electron, and an antineutrino with a half-life of 12.8
minutes.The proton is the nucleus of ordinary hydrogen and is stable. (E. O. Lawrence,1935)
3
1.2.History Of Radioactivity
In the year 1896, Roentgen discovered X-rays. At that time Professor Henri Becquerel
investigated the possibility that this mysterious radiation might be given off spontaneously
from natural substances. He had in mind particularly the class of substances that give off light
of their own accord - phosphorescent substances. Becquerel had been studying the properties
of phosphorescent substances and happened to have in his possession at that time some
phosphorescent salts of uranium, which he had prepared fifteen years before. Almost
immediately he discovered that uranium salts do give off a radiation like X-rays for when the
uranium salts were placed near a photographic plate enclosed in a light-tight box, after a period
of time the photographic plate was activated. Very soon Rutherford, then at McGill, showed
that the radiations continuously emanating from uranium could be divided into two types: one
called the alpha rays, which were very easily absorbed in matter and produced intense
ionization, and a much more penetrating type called the beta rays. When a still more penetrating
type of radiation was discovered, Villard named them the gamma rays. These names for the
three types are still used, although now it is known that the alpha rays are the nuclei or centers
of helium atoms, the beta rays are high-speed electrons, and the gamma rays are indeed very
penetrating X-rays, which are of the same nature as light.
Soon other radioactive substances were discovered and in 1898 Madame Curie isolated
radium. At this stage a number of radioactive substances had been found. Some appeared to
give off radiation continuously and constantly, while the radiation from others decreased with
time. This complicated mass of facts was reduced to order by the transformation theory of
Rutherford and Soddy in 1903.
According to this theory, the atoms of the radio-elements, unlike the atoms of the
ordinary elements, are not stable, but undergo spontaneous disintegration, accompanied by the
expulsion of an alpha or a beta particle. After the disintegration, the resulting atom has physical
and chemical properties entirely different from the parent atom. It may in turn be unstable and
pass through a succession of transformations, each of which is characterized by the emission
of an alpha or beta particle. (E. O. Lawrence,1935)
4
1.3.Ionizing Radiation:
Radiation is a form of energy, such as light or heat. Radiation is characterized according
to the frequencies of these wavelengths. Infrared waves, microwaves, and radio waves occur
at the lowest frequencies. Ionizing radiation occurs at the highest frequencies. The process of
transforming a neutral atom or molecule into an electrically charged component is known as
ionization. Ions are either positively charged or negatively charged, depending upon the
number of protons and electrons present in the atom.
1.4.Radioactive Decay:
5
radionuclide is specific to each radionuclide. The total quantity of ionizing radiation that will
be released is essentially based upon a fixed set of radioactive particles and photons that are
ejected during disintegration. Additional factors such as the energy release per each
disintegration of the radionuclide, as well as the length of time that the radionuclide will exist,
can provide practical adjustments to the sole use of the unit of activity as a quantification
device. (Borrelli,1999)
1.5.Specific Ionization:
The unstable isotope will disintegrate to the stable state through the emission of excess
energy in the form of photons, particles, or a combination of both. Each of these particles and
photons is ejected from the radioactive source at a certain energy level, specific to the source
material. The extent to which ejected particles and photons interact with matter can be
described in terms of specific ionization.
Specific ionization can be defined as the quantity of ion pairs that will be produced,
given a specific amount of ionizing radiation that a radionuclide will release. Approximately
34 eV are required to produce one ion pair. The rate of production of ion pairs is energy specific
and not dependent upon the type of radioactive particle involved in the interaction. Therefore,
a 1 MeV release accompanying the emission of a radioactive particle or a photon will produce
approximately 30000 ion pairs for every release. As a result of the continuous release of energy
from a radioactive source, ion pairs will be generated continually throughout the existence of
the source. A quantity of radioactivity can be measured in terms of the number of ion pairs that
the energy will produce in exposed material. This adjusted measure of radioactivity can be
applied to the vast and highly variable amounts of sources that exist in nature. Such adjustments
can aid in the assessment of the environmental effects of a source defined in terms of the
imparted energy to materials, based upon the number ion pairs that the source will produce.
(Borrelli,1999)
6
1.7.Types of Radiation:
1.7.1.Alpha Particles:
An alpha particle is comprised of two protons and two neutrons. The alpha particle
possesses an electrical charge of +2. Alpha particle decay will occur from a nucleus in which
the number of neutrons is much higher than the number of protons. Nuclei heavier than lead,
such as thorium, plutonium, radon, and uranium decay through alpha emission.
Each radionuclide will emit one or more alpha particles at fixed energy levels. The
resulting release of ionizing radiation will be imparted to a given medium only over a small
distance. Alpha particles collide very easily with matter and lose energy quickly because of
large size and of high electrical charge. Only a few centimeters of air, or the outer layer of skin,
will provide a sufficient barrier to alpha particle penetration. (Borrelli,1999)
1.7.2.Beta Particles:
Beta particles are equivalent to electrons but arise from radioactive decay of unstable
atoms. They are emitted with a continuous range of energies up to a maximum that is
characteristic of each radionuclide. Electrons have a greater range and penetrating power but
much less ionizing potential compared to alpha particles. The range of beta particles in air is
∼4 m per MeV of energy. In water the range in cm is approximately one-half the maximum
beta energy when expressed in MeV. (Borrelli,1999)
Thorium-234 is a nucleus that undergoes beta decay. Here is the nuclear equation for
this beta decay:
90Th
234
→ -1e0 + 91Pa234
1.7.3.Gamma Rays:
Unlike the previous types of decay, gamma rays represent energy that is transmitted in
a wave. Gamma rays are similar to X-rays in that both forms of radiation are photons.
Fundamentally, there is no difference between these types of photons. Gamma rays originate
in the nucleus..These types of radiation occur at the highest frequencies of the energy spectrum.
Gamma rays occur at a higher frequency. Gamma rays have wavelengths shorter than 10 -11
meters and frequencies above 30 x 1018 Hz.
7
Nuclei formed as a result of the previous methods of decay usually are left in an excited
state after particle emission. Excited nuclei then proceed to decay to the ground state through
the emission of gamma rays. A large majority of nuclei in this excited state decay in an
immeasurably short period of time. In some instances, the decay of excited nuclei is delayed.
Excited nuclei appear to exist in a semi-stable, or isomeric, state. The subsequent decay,
an isomeric transition, occurs as the semi-stable nucleus emits a gamma ray in order to exist at
the ground state. Beta particle emission also can take place in the isomeric state.
Because gamma rays are energy waves, they do not possess a mass or an electrical
charge. These photons have the highest ranges of penetration. These forms of radiation can
pass through the human body. Highly dense materials, such as lead or steel, provide effective
barriers to gamma rays. (Borrelli,1999)
1.8.Half Life:
Each radionuclide will decay for a fixed amount of time. This amount of time defines
the existence of each radionuclide. Scientists, engineers, and other professionals in nuclear
related fields use these fixed existences with which to classify radioisotopes. The time that has
elapsed for the activity of a radioisotope to decrease by a factor of two is defined as a half-life.
The probability per unit time that a radioactive nuclide will decay is a constant and independent
of time. (Borrelli,1999)
0.693
t1/2=
𝜆
1.9.Secular Equilibrium :
This is a state in which the rate of decay of a parent radionuclide is equal to that of a
daughter radionuclide. It can occur in a decay series if the half-life of the parent radionuclide
is much longer than that of the daughter radionuclide. The decay rate of a parent radionuclide
and hence the production rate of the daughter radionuclide becomes approximately constant.
The quantity of the daughter radionuclide increases until the rate production of its atoms
becomes equal to its rate of decay. Considering the decay of a parent radionuclide, A, decaying
into daughter radionuclide, B, the idea of radioactive equilibrium can be explained using the
decay law .
𝑑𝑁𝐵
= 𝐴 N𝐴 − 𝐴 𝑁𝐵
𝑑𝑡
8
where NA and NB are number of atoms of A and B at a given time while A and B are the
decay constants of radionuclides A and B, related to their half- lives by;
𝑙𝑛(2)
𝑡1/2
𝐴
N𝐵 = N
𝐵 𝐴
(Kiplangat Elijah,2011).
1.10.Artificial Radioactivity:
1.11.Natural Radioactivity:
People are exposed to natural radiation on a daily basis as our planet earth is radioactive.
More than 60 naturally occurring radioactive materials are found in soil, water and air. These
radioactive elements are classified into the following categories:
1. Primordial - from the creation of earth.
2. Cosmogenic - formed as a result of cosmic ray (from sun
and outer space) interactions with earth's atmosphere.
3. Human produced - enhanced or formed due to human
activities.
In recent years, the source of radioactive elements in soil, water and air is considerably
increased by various human activities such as: disposing the hospital wastes, nuclear wastes
and industrial effluents to the environment, etc. Wastes associated with various industrial
9
activities were enhanced levels of natural radioactivity (Hilal, Attallah, Gehan, & Fayez-
Hassan, 2014). Hence people can be exposed to radiation either externally by a close source of
radiation or exposed internally by radioactive material that has entered the body. Soil not only
acts as a source of continuous radiation exposure to humans but also as a medium of migration
for transfer of radionuclides to biological systems (Mehra, Badhan, Sonkawade, Kansal, &
Singh, 2010). Hence, the basic indicator of radiological contamination in the environment is
the soil.
Radioactivity is an integral part of our environment. All living beings have been
exposed to a constant flux of natural radiation on the surface of our friendly planet. Natural
radioactivity in the environment originates from two sources. First,
primordial radionuclides which were incorporated into the Earth at the time of its formation
are still present in it because of their long half-lives. 238U, 235U, 232Th and their decay
series, 40K, 87Rb and 187Re are examples of this category. Second, cosmic ray-produced
isotopes which are generated continuously in the atmosphere and earth's crust through
interactions of cosmic rays with their constituents.
Natural radioactivity is still the principal source of radiation exposure. Humans are
constantly being bombarded by particles of cosmic radiations every second. Rocks like granite,
which have become symbols of permanence and durability, contain light traces of radioactive
uranium. Sitting on or walking near a block of granite exposes you to previously unencountered
sources of radioactivity. Even the food we eat or the air we breathe contains radioactive
elements. Humans are radioactive too. Eight thousand atoms of potassium 40 or carbon 14
disintegrate in our bodies every second.
The most important natural source of radioactivity is a rare gas known as radon. One
of the products of uranium decay, radon is an ‘inert gas’ that can participate in no chemical
reaction. This would seem to make it completely harmless, were it not for the fact that radon
own radioactive decay produces gases poisonous to humans.
2.4 mSv is a low dose. In certain parts of India, China and Brazil the natural exposure
level rises to 10 or even 20 mSv a year. The fact that humans have survived these comparatively
overexposed conditions indicates that all doses of the order of millisieverts are negligible and
very likely harmless. (Radioactivity.Eu).
1.11.1.Cosmic radiation:
10
Cosmic radiation consists of high-energy particles and radiation that originate from
outside the Earth’s atmosphere, including from the sun and other sources in the universe.
Cosmic radiation is a type of high-energy radiation that originates from outer space, including
the sun and other sources in the universe. Cosmic radiation includes a mix of charged particles,
such as protons, alpha particles, and heavy ions, as well as gamma rays and other forms of
electromagnetic radiation.
Cosmic radiation is present everywhere in space and can penetrate the Earth’s
atmosphere, affecting the planet’s surface and atmosphere. The intensity of cosmic radiation
exposure depends on various factors, including altitude, latitude, and solar activity.
At ground level, the dose of cosmic radiation is generally low and not considered a
significant health risk for most people. However, people who work in high-altitude
environments may be exposed to higher levels of cosmic radiation, which can increase their
risk of radiation-related health effects, including cancer and cataracts.
1.11.2.Terrestrial radiation:
Terrestrial radiation that comes from natural sources on Earth, such as radon gas and cosmic
rays. Terrestrial radiation is a type of radiation that originates from natural sources on Earth. It
includes various forms of ionizing and non-ionizing radiation, such as:
● Cosmic rays: As mentioned earlier, cosmic rays are high-energy particles and radiation
that originate from outside the Earth’s atmosphere, including from the sun and other
sources in the universe.
● Radon gas: Radon is a radioactive gas that is produced by the decay of uranium in soil
and rocks. Radon gas can accumulate in enclosed spaces, such as homes and
workplaces, and can pose a health risk if inhaled in high concentrations.
11
1.11.3.Exposure from Terrestrial Radiation:
The composition of the earth's crust is a major source of natural radiation. The main
contributors are natural deposits of uranium, potassium and thorium which, in the process of
natural decay, release small amounts of ionizing radiation. Uranium and thorium are
“ubiquitous”, meaning they are found essentially everywhere. Traces of these minerals are also
found in building materials, so exposure to natural radiation can occur indoors as well as
outdoors.
1.12.Radioactivity Series:
1.12.1.Uranium Series:
12
The Uranium series, also known as the actinide series, is a radioactive decay chain of
naturally occurring elements that begins with uranium-238 (U-238) and ends with lead-206
(Pb-206). The series includes a total of 14 radioactive elements, with each element in the series
decaying into the next element over time.
The uranium series begins with the decay of U-238, which has a half-life of 4.5 billion
years. U-238 decays into thorium-234 (Th-234), which has a half-life of 24 days. Th-234 then
decays into protactinium-234 (Pa-234m), which has a half-life of just 1.17 minutes. Pa-234m
quickly decays into uranium-234 (U-234), which has a half-life of 245,500 years.
The decay chain continues with U-234 decaying into thorium-230 (Th-230), which has
a half-life of 75,380 years. Th-230 then decays into radium-226 (Ra-226), which has a half-life
of 1,600 years. Ra-226 decays into radon-222 (Rn-222), which has a half-life of just 3.8 days.
Rn-222 then decays into polonium-218 (Po-218), which has a half-life of just 3.1 minutes.
The uranium series continues with Po-218 decaying into lead-214 (Pb-214), which has
a half-life of 26.8 minutes. Pb-214 then decays into bismuth-214 (Bi-214), which has a half-
life of just 19.7 minutes. Bi-214 decays into polonium-214 (Po-214), which has a half-life of
just 164 microseconds.
The uranium series concludes with Po-214 decaying into lead-210 (Pb-210), which has
a half-life of 22.3 years. Pb-210 then decays into bismuth-210 (Bi-210), which has a half-life
of just 5.01 days. Bi-210 decays into polonium-210 (Po-210), which has a half-life of just 138
days. Finally, Po-210 decays into stable lead-206 (Pb-206).
The uranium series has important applications in geology and environmental science,
as the decay of uranium and its daughter elements can be used to date rocks and determine the
age of geological formations. It is also important in nuclear physics and engineering, as
uranium is used as a fuel in nuclear power plants.
13
1.12.2.Thorium Series:
The thorium series, also known as the 4n series, is a radioactive decay chain of naturally
occurring elements that begins with thorium-232 (Th-232) and ends with stable lead-208 (Pb-
208). The series includes a total of 13 radioactive elements, with each element in the series
decaying into the next element over time.
The thorium series begins with the decay of Th-232, which has a half-life of 14.05
billion years. Th-232 decays into protactinium-234 (Pa-234), which has a half-life of 6.7 hours.
Pa-234 then decays into uranium-234 (U-234), which has a half-life of 245,500 years.
The decay chain continues with U-234 decaying into thorium-230 (Th-230), which has
a half-life of 75,380 years. Th-230 then decays into radium-226 (Ra-226), which has a half-life
of 1,600 years. Ra-226 decays into radon-222 (Rn-222), which has a half-life of just 3.8 days.
Rn-222 then decays into polonium-218 (Po-218), which has a half-life of just 3.1 minutes.
The thorium series continues with Po-218 decaying into lead-214 (Pb-214), which has
a half-life of 26.8 minutes. Pb-214 then decays into bismuth-214 (Bi-214), which has a half-
life of just 19.7 minutes. Bi-214 decays into polonium-214 (Po-214), which has a half-life of
just 164 microseconds.
14
The thorium series concludes with Po-214 decaying into lead-210 (Pb-210), which has
a half-life of 22.3 years. Pb-210 then decays into stable lead-206 (Pb-206) through a series of
beta decays and alpha decays.
Like the uranium series, the thorium series also has important applications in geology
and environmental science, as the decay of thorium and its daughter elements can be used to
date rocks and determine the age of geological formations. Thorium is also being explored as
a potential fuel for nuclear reactors, as it is more abundant than uranium and produces less
long-lived nuclear waste.
Both natural and man-made sources of radiation can contribute to the presence of
radioactive elements in soils. Examples of natural sources include the decay of isotopes such
as uranium,thorium, and potassium, while man-made sources include nuclear weapons testing
and the operation of nuclear power plants. The sources of radiation in soils can be divided into
two categories: Natural and Man- Made.
The decay of isotopes of elements such as uranium, thorium, and potassium, which
are naturally occurring in the Earth’s crust.
Cosmic radiation from outer space, which can penetrate the Earth’s atmosphere and
contribute to background radiation levels in soils
Nuclear weapons testing, which has led to the release of radioactive isotopes into the
environment, including soils.
The operation of nuclear power plants, which can release radioactive substances into
the environment through accidents or routine releases.
The use of radioactive materials in industry, medicine, and agriculture, which can
result in the release of radioactive isotopes into the environment and their
accumulation in soils.
The disposal of radioactive waste, which can result in the migration of radioactive
isotopes into soils.
15
It’s important to note that the levels of radiation in soils can vary greatly depending on
the specific location and the presence of both natural and man-made sources. In general, the
levels of background radiation in soils are low, but the presence of man-made sources can
result in elevated levels of radiation that may have impacts on the environment and human
health.
16
Background to the Study
Naturally occurring radionuclide materials have been present in the Earth’s surface
since its formation. These radionuclides include: Uranium-238, Thorium-232 and Potassium-
40. Their concentrations vary from place to place and can be artificially introduced to the soil
by application of inorganic fertilizers and pesticides to enhance soil properties and increase
crop production. Gamma rays, alpha and beta radiations are released when these radionuclides
and their daughters in the series undergo decays. Human beings therefore, cannot avoid
continuous exposure to ionizing radiation both inside and outside their dwellings. Inorganic,
especially phosphate (P) fertilizers contain hazardous elements including heavy metals, for
example Cd, Cr, and Pb, and radioactive elements, for example U, Th and their daughters,
which are considered to be toxic to animal and human health.
Soil is an important resource to human. It can be used for food production and building
shelter. The chemical, mineral and biological components of soil can be inhaled, ingested or
absorbed through the skin, hence can be harmful to human health, for example cancers due to
inhalation of radon gas from the decay of uranium in soil minerals, radiation sickness and
sterility. As soils interact with atmosphere, hydrosphere and biosphere, human health can also
be influenced indirectly, for example the frequent detrimental biological and chemical quality
of recreational and drinking water that are influenced by processes of soil erosion, leaching,
surface runoff and interflow.
The radionuclide concentrations in samples can be determined using several
measurement techniques. Gamma radioactivity can be measured by HPGe and NaI(Tl)
40 238 232
detectors. In this study NaI(Tl) detector is used to measure activity of K, U and Th.
Radium equivalent activity and hazard indices are assessed to evaluate radiological effects of
the surface soils.
17
CHAPTER II
18
LITERATURE REVIEW
Numerous studies have been done to evaluate the risk of radiation exposure due to
naturally occurring radionuclides in the environmental samples. A study on natural
radioactivity level in the soil samples of Eloor Island, India, reported an outdoor annual
effective dose of between 0.1mSvy-1 and 0.7mSvy-1 with a mean value of 0.3 mSvy-1. All the
values were within the recommended dose of less than 1 mSvy-1 (Dhanya et al., 2015).
19
A study carried out at the Minjingu phosphate mines in neighboring Tanzania found
226
concentrations of Ra as high as 5760±107 Bqkg-1 in phosphate rock and 4250 Bqkg-1 in
226
waste rock. These values are more than 100 times the world average value. Elevated Ra
levels were also observed in biological samples such as wild leaf vegetation with a
concentration of 650±11 Bqkg-1 and edible leaf vegetation with concentration of 393±9 Bqkg-
1
. The radiation dose from ambient air over five years at the phosphate mine ranged from 1375
nGyh-1 to 1475 nGyh-1 with 15 an average of 1415 nGyh-1 which is higher than the global
average background radiation from terrestrial sources by a factor of 28. These values suggest
a possible radiation health risk to the area inhabitants resulting from external gamma irradiation
as well as internal exposure from vegetables consumption (Banzi et al., 2000).
Another study involving clay samples from Aswan, South Egypt found average activity
concentrations of natural radionuclides to be within the recommended safe limits (Alharbi and
Taher, 2016).
In another study, soil samples obtained from the region around titanium mines in the
coastal region were also found with low radioactivity levels relative to the world averages
(Osoro, 2007).
Still in the coastal region of the country, soil samples from Mrima hills were found
with 16 elevated absorbed dose rate averaging 440.7 nGyh-1 which is much higher than the
world average of 60 nGyh-1 (Kebwaro, 2009).
20
Further studies on soil and rock samples in soapstone quarries in Kisii annual effective
dose in the ranging from 1.03 mSvy-1 to 1.27 mSvy-1 was observed. (Kinyua et al., 2011)
A study on radionuclide content of sand used for construction in Kakamega County and
226
associated indoor radon diffusion doses found that Ra ranged from 36.79±8.89 Bqkg-1 to
185.21±5.89 Bqkg-1 with a mean of 128.05±8.89 Bqkg-1, 232Th ranged from 51.12±2.56 Bqkg-
1
to 158.92±7.95 Bqkg-1 with a mean of 98.37±6.41 Bqkg-1 and 40K ranged from 322.38±16.12
Bqkg-1 to 17 960.53±48.03 Bqkg-1 with a mean of 756.39±35.99 Bqkg-1. The average values
of radium equivalent activity, absorbed dose rate, annual effective dose rate and external hazard
index were 321.67±12.4 Bqkg-1, 151.76±5.65 nGyh-1, 0.74±0.02 mSvy-1 and 0.88±0.03,
respectively (Shikali, 2013).
A study on the levels of radionuclides in Brazilian state of Rio Grande do Norte found
that the average activity concentrations of Radium-226, Thorium-232 and Potassium-40 in soil
21
samples from the area of study were 29 Bqkg-1, 46.6 Bqkg-1 and 677 Bqkg-1 respectively
(Malanca et al., 1993).
A research on radioactivity in soils of Johor state in Malaysia found out that the
concentration of naturally occuring radionuclide Uranium-238 was in the range of (58.8 Bqkg-
1 - 484.88 Bqkg-1) and that of Thorium-232 ranged from 59.68 Bqkg-1 - 1203 Bqkg-1 .
(Ramli et al., 2005).
In a research on activity concentrations in phosphate and soil samples from El-Sabaea
Aswan in Egypt, it was observed that the activity concentration of 226Ra, 232Th and 40K
ranged from 59.7±6.7 Bqkg-1 to 638±31.0 Bqkg-1, 9.9±1.4 Bqkg-1 to 40.6±6.3 Bqkg-1 and
213.1±9.5 Bqkg-1 to 798.9±30.6 Bqkg-1 respectively (Harb et al., 2008).
Surface soils around Mrima hill were analysed and the activity concentrations of 238U,
232 40
Th and K in the samples were found to be 207.03±11.3 Bq/kg, 500.7±20.3 Bq/kg and
805.4±20.7 Bq/kg respectively. It was found out that the radioactivity concentrations were
higher than the world mean values. The calculated radiation absorbed dose from the different
points where sampling was done ranged from 253.8±2.5 nGyh-1 to 733.1±3.4 nGyh-1 with a
mean of 440.7±16.8 nGyh-1. (Kebwaro et al., 2009)
22
CHAPTER III
23
MATERIAL AND METHODS
3.1.Study Area:
3.1.1.About The Site:
Thoothukudi is known as "Pearl City" due to the pearl fishing carried out in the town.
It is a commercial seaport which serves the inland cities of Southern India and is one of the sea
gateways of Tamil Nadu. The current estimate population of Thoothukkudi city in 2023 is
327,000 , while Thoothukkudi metro population is estimated at 567,000 . The majority of the
people of the city are employed in salt pans, sea-borne trading, fishing, and tourism. The 21
islands between Thoothukudi and Rameswaram shores in the Gulf of Mannar are noted as the
first Marine Biosphere Reserve of India, and have around 36,000 species of flora and fauna.
Thoothukudi is a port town situated in the Gulf of Mannar about 125 km (78 mi) North
of KanyaKumari and its environs form part of the coastal belt which forms a continuous stretch
of the flat country relieved here and there by small rock outcrops. The region, surrounding
Thoothukudi is liberally dotted with rain fed tanks. Red soils found on the southern side of the
Thoothukudi town is composed quartz and variable quantities of fine red dry dust. The port is
an all weather one. The bay formed by the Hare Island, Devils point and the main land gives
ample protection to the lighters from monsoonal weather. The beach of Thoothukudi is featured
with calm breeze and very low waves giving an image of a big river.[16]
24
varies between 1 and 4 m (3.3 and 13.1 ft) below ground level. The city has loose soil with
thorny shrubs in the north and salt pans in the south.
25
3.1.2.Sampling Sites:
The Samples are collected from the various Sea-Shores of the district. The below map
shows the sampling sites of the district.
S1
S2
S3
S4
S5
26
Figure 3: The Sampling Site Pictures
S1 Site S2 Site
S4 Site S5 Site
27
3.2.Sample Preparation:
Five sampling sites have been selected across the coastal region each separated by 10
kilometers. Soil samples were collected according to the standard procedures and they were
labelled as S1,S2,S3,S4,S5 . To find the radioactivity levels, the samples were dried in an oven
till a constant dry weight was obtained. Then these samples were powdered and sieved through
a 150-mm mesh. The processed soil samples were packed in a 250 ml plastic container to its
full volume with uniform mass. These containers were sealed hermetically and sealed
externally to ensure that all the daughter products of uranium and thorium and in particular,
radon isotopes formed do not escape. A time of 30 days was allowed after packing to attain
226
secular equilibrium between Ra and its short-lived daughter products. The net-weight of
each sample was determined before counting. To reduce the contribution from background
radiation while recording the spectrum in the laboratory, the samples were kept in a lead shield,
which has a shielding efficiency of 95%.
28
SPECTRSCOPIC TECHNIQUES
3.3.1.Gamma-ray spectrometry:
Gamma-ray spectrometry is a technique that studies quantitatively the energy spectra
of gamma-ray sources such as those used in the nuclear industry, geochemical investigation
and astrophysics. Most radioactive sources produce gamma rays of various energies and
intensities. When these emissions are detected and analyzed with an energy calibrated gamma
spectroscopy system, a gamma-ray energy spectrum is produced. The detector is usually energy
calibrated using specific energy peaks from standard reference sample so that each channel is
assigned a specific energy value. The spectrum is typically used to identify and quantify the
gamma emitters present in a gamma source given that the gamma spectrum is characteristic of
the gamma emitting nuclides contained in the source.
A NaI(Tl) scintillation counter is a radiation detector which uses the effect known as
scintillation. In this case, scintillation occurs in the NaI(Tl) crystal.
29
A NaI(Tl) scintillation counter is a radiation detector which uses the effect known as
scintillation. Scintillation, which occurs in the NaI(Tl) crystal, is a flash of light produced in a
transparent material by the passage of a particle (an electron, an alpha particle, an ion, or a
high-energy photon). Scintillation occurs in the scintillator, which is a key part of a scintillation
detector. In general, a scintillation detector consists of:
The basic principle of operation involves the radiation reacting with a scintillator, which
produces a series of flashes of varying intensity. The intensity of the flashes is proportional to
the energy of the radiation. This feature is very important. These counters are suited to measure
the energy of gamma radiation (gamma spectroscopy) and, therefore, can be used to identify
gamma emitting isotopes.
The advantages of a scintillation counter are its efficiency and the high precision and
counting rates that are possible. These latter attributes are a consequence of the extremely short
duration of the light flashes, from about 10-9 (organic scintillators) to 10-6 (inorganic
scintillators) seconds. The intensity of the flashes and the amplitude of the output voltage pulse
are proportional to the energy of the radiation. Therefore, scintillation counters can be used to
determine the energy, as well as the number, of the exciting particles (or gamma photons). For
gamma spectrometry, the most common detectors include sodium iodide (NaI) scintillation
counters and high-purity germanium detectors.
30
Thallium-doped Sodium Iodide – NaI(Tl) scintillators:
The most widely used scintillation material is NaI(Tl) (thallium-doped sodium iodide).
NaI(Tl) as the scintillator is used in scintillation detectors, traditionally in nuclear medicine,
geophysics, nuclear physics, and environmental measurements. The iodine provides most of
the stopping power in sodium iodide (since it has a high Z = 53). These crystalline scintillators
are characterized by high density, high atomic number, and pulse decay times of approximately
1 microsecond (~ 10-6 sec). The wavelength of maximum emission is 415 nm. Scintillation in
inorganic crystals is typically slower than in organic ones. They exhibit high efficiency for
detection of gamma rays and are capable of handling high count rates. Inorganic crystals can
be cut to small sizes and arranged in an array configuration so as to provide position sensitivity.
This feature is widely used in medical imaging to detect X-rays or gamma rays. Inorganic
scintillators are better at detecting gamma rays and X-rays. The NaI(Tl) scintillator has a higher
energy resolution than a proportional counter, allowing for more accurate energy
determinations. This is due to their high density and atomic number which gives a high electron
density. A disadvantage of some inorganic crystals, e.g., NaI, is their hygroscopicity, a property
which requires them to be housed in an airtight container to protect them from moisture. The
crystals are usually coupled with a photomultiplier tube, in a hermetically sealed assembly.
Photomultiplier Tube:
Photomultiplier tubes (PMTs) are a photon detection device that uses the photoelectric
effect combined with secondary emission to convert light into an electrical signal. A
photomultiplier absorbs light emitted by the scintillator and re-emit it in the form of electrons
via the photoelectric effect. The PMT has been the main choice for photon detection ever since
due to the fact that they have high quantum efficiency and high amplification.
The device consists of several components and these components are shown in the
figure.
Photocathode:
Right after a thin entry window, is a photocathode, which is made of material in which
the valence electrons are weakly bound and have a high cross section for converting photons
to electrons via the photoelectric effect. For example, Cs3Sb (caesium-antimony) may be used.
31
As a result, the light created in the scintillator strikes the photocathode of a photomultiplier
tube, releasing at most one photoelectron per photon.
Dynodes:
32
Figure 6 : NaI(Tl) Detector
33
EXPERIMENTAL PROCEDURES
3.5.Background Measurement:
The background radioactivity distribution in the environment around the detector was
determined by counting a plastic container filled with distilled water in the same manner and
in the same geometry as the samples. The background measurement was repeated at regular
intervals for quality control. The background radiation was subtracted from each of the
recorded spectrum (Righiet al., 2009)
Yg − Yb = Yn
where Yg is the gross spectra count, Yb is the background radiation and Yn is the net
spectra count of the sample.
Detector efficiency This is the probability that an emitted gamma ray will interact with the
detector and produce a count. It is measured by comparing a spectrum from a source of known
activity to the count rates in each peak to the count rates expected from the known intensities
of each gamma ray. In this research work, standard IAEA certified samples of 238U, 232Th
and 40K were used. The peak corresponding to 1460 keV (40K) for 40K, 1765 keV (Bi-214) for
238
U and 2615 keV (Tl-208) for 232Th were considered in arriving at the activity levels. Certified
activities and number of counts in the peaks were used in the calculation of detector efficiency
using the formula given by ,
𝑁𝑒𝑡 𝐶𝑜𝑢𝑛𝑡𝑠 100
Efficiency = x
𝑇𝑖𝑚𝑒 𝑌𝑖𝑒𝑙𝑑
2.5
2
1.5
1
0.5
0
0 500 1000 1500 2000
Energy (keV)
35
where Ci is the radioactivity concentration of radionuclide i in the sample, M is the
mass of the sample, E is the detector efficiency at a specific gamma-ray energy and 𝑃 is the
emission probability of the specific gamma-ray.
𝐶𝑈 𝐶𝑇ℎ 𝐶𝐾
Hex = + + ≤1
370 Bq/kg 259 Bq/kg 4810 Bq/kg
36
where CU, CTh and CK are the activity concentrations of 238U, and 232Th and 40K, respectively
(Ahmed, 2005).
where CU, CTh and CK are the activity concentrations of 238U, and 232Th and 40K, respectively.
37
CHAPTER IV
38
RESULTS AND DISCUSSION
The aim of this study was to measure natural radioactivity levels in soils obtained from
coasts of Tuticorin district. These activity levels were measured using NaI (Tl) detector. The
soils obtained were prepared and analysed at Scott Christian College Radiation Laboratory.
The analysis of these soil samples included measuring the intensity and calculation of
radioactivity concentration, radium equivalent activity, external and internal hazard indices,
and absorbed dose rate.
Table 3: A summary of the activity concentration of 238U, 232Th and 40K in all the
sampling points.
Sample Location 238U 232Th 40K
39
Table 4: Mean activity concentrations of the soil samples measured in this study
compared to the world average (UNSCEAR, 2016)
232
Th 91.5524 45
40
K 299.708 420
It is also observed that the activity concentration of 40K is highest in all the sampling
sites except sample S5. The high activity concentration of 40K in site S2 may be due to the rich
in presence of potassium. It is also the most abundant radionuclide element under
consideration.
232
The activity concentration of Th in sample S5 is high compared to the other sites.
The high levels of natural radionuclide concentration in some parts of this region might also
have resulted from industrial disposals. The sample site S1 is also having a high thorium level.
238 232 40
The natural radioactivity levels of U, Th and K in these regions have been compared
with published values of worldwide. These variations in the activity concentrations in the soil
of the various locations of the country was due to the geological and geographical conditions
of the area.
238
The activity concentration of U in sample S2 is high among the other sites. Many
Salt pans are situated in that particular area. There are few people living near the area and some
of them are doing fishing.
Fishing harbour and salt pans are more in number near the sampling sites S1 and S2.
The sample site S3 is a public beach which has low activity concentration among the other
sites. Sample S4 is from an island. Hence the Activity Concentrations of the areas are calculated
and observations are made. The Graph is plotted between sampling sites and their Activity
Concentrations.
40
Figure 9 : The Activity concentration of the primordial radionuclides against sampling
900
U-238
800
Th-232
700
Activity Concentration
K-40
600
500
400
300
200
100
0
S1 S2 S3 S4 S5
Sampling Sites
sites
41
Table 5 : Radium equivalent activity
Mean 156.9933
350 324.9914
300
Radium Equivalent Activity
250
197.928
(Bqkg-1)
200
150 131.658
100 75.585
54.804
50
0
S1 S2 S3 S4 S5
Sampling Sites
42
4.3.Hazard Indices:
The external hazard index and the internal hazard index were calculated. The mean
external hazard index was found to be 0.42389 within a minimum of 0.147971 and a maximum
of 0.87748. The average internal hazard index was to be 0.431984 within a minimum of
0.14841 and a maximum of 0.8834. The average values of both external hazard index and
internal hazard index were below 1, which is the world average. The internal hazard index is
higher than the external hazard index. The site S5 has the large index among the other sites.
The Site S5 is near a thermal power plant. A comparison of external hazard index and internal
hazard index obtained in this study.
43
Figure 11 : Values of Hazard indices against sampling sites
1
0.9
0.8
0.7
Hazard Index
0.6
0.5
External H
0.4
Internal H
0.3
0.2
0.1
0
S1 S2 S3 S4 S5
Sampling Sites
The absorbed dose rate was calculated. The absorbed dose rate in air at a height of 1 m
above the ground level was obtained from the different sites ranged from 25.5 nGyh-1 to
138.0985 nGyh-1 with an average value of 69.1795 nGyh-1 . The mean absorbed dose rate is
higher than the world average value of 60 nGyh-1 but lower than maximum allowed health limit
of 1500 nGyh-1 as proposed by UNSCEAR (2016).
44
Table 7 : Absorbed Dose Rate of the sampling sites
Mean 69.1795
160
Absorbed Dose Rate
140 (nGy/h)
120
Dose Rate (nGy/h)
100
80
60
40
20
0
S1 S2 S3 S4 S5
Sampling Sites
45
Absorbed Dose Rate (nGy/h)
25%
40% S1
S2
18% S3
S4
10% 7%
S5
Table 8 : The world average and maximum acceptable safety health limit of radiological
parameters (UNSCEAR, 2016)
46
CONCLUSION
238 232 40
Radioactivity levels of U, Th and K have been measured in the soil samples
collected from sea shore samples of Tuticorin district. The activity concentration of 238U, 232Th
and 40
K in the soils were found to be in the range of (0.16356 – 5.048) BqKg-1, (24.391 –
221.378) BqKg-1 and (80.9278 – 828.685) BqKg-1 respectively. The mean activity of 238
U,
232
Th and 40K in the soil samples were found to be 2.99577 Bqkg-1, 91.5524 Bqkg-1 and 299.708
Bqkg-1 respectively. The concentrations of 232
Th is higher in Sample S5 and S2. The
concentration of 40K was found to be high compared to the World average in sampling site S2.
The average radium equivalent activity (Raeq) in the study area is 156.993 Bqkg-1. This is less
than the recommended safe value of 370 Bqkg-1 so the radiation hazards associated with the
radionuclides present in the soil are within the limits. The hazard indices values are less than
the world average value of unity so there is no radiation harm in the study area. The average
Absorbed dose rate in the study area is 69.1795 nGyh-1 .This is slightly higher than the world
average value of 60 nGyh-1. The absorbed dose rate is high in the sampling site S5. The
232
presence of Th is more in sampling site S5. The sampling site S3 (Pearl City Beach) has
least amount of hazard index (0.148) hence it has absolute no harm in radioactivity. This place
is under safe consideration. The dose absorption rate is high in site S5 (Roche Park) and the
238
soil observed to be black in colour. Hence the levels of radionuclides U , 232Th and 40K are
analysed and using the activity concentration of the radionuclides the Radium equivalent
activity was found. Further the internal and external Hazard indices are calculated which is
used to measure the radioactivity hazard of the study area. Then the Absorbed dose rate for the
study area is calculated by the activity of each sampling sites. From the results it is observed
that the Study area possesses no radiation harm in both air and soil.
47
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