CHAPTER ONE

1.0 INTRODUCTION
1.1 BACKGROUND TO THE STUDY
Measurements of natural radioactivity in soil are very important throughout the world to estimate
the radioactivity level in soils. The exposure to ionizing radiations from natural sources occurs
because of the naturally occurring radioactive elements in the soil and rocks, cosmic rays
entering the earths atmosphere from outer space and the internal exposure from radioactive
elements through food, water and air. The natural radioactivity in soil primarily comes from U
and Th series and natural K. The radiological implication of these radionuclides is due to the
gamma ray exposure of the body and irradiation of lung tissue from inhalation of radon and its
daughters. Therefore, the assessment of gamma radiation dose from natural sources is of
particular importance as natural radiation is the largest contributor to the external dose of the
world population United Nations Scientific Committee on Effect of Atomic Radiation
(UNSCEAR, 1998).
.
3The presence of naturally occurring radioactive materials in soil above threshold levels may
contaminate the environment and caused health problems to humans and plants. The exposure to
radioactive materials has been associated with some health problems like cancer.
Measurement of gamma ray spectrometry involves the collection of a spectrum of the ambient
gamma ray flux at a given site for analysis principally to identify and quantify the radionuclide
present at broad energy windows for the in-situ estimation of K, U and Th radioelement
concentrations. Several thousands of field measurements of full energy spectra can be recorded
in the instrument memory of gamma ray spectrometer (Darnley 1972).

In-situ gamma ray spectrometry has been applied in a wide assortment of environmental
137
radioactivity measurements. These include the measurements of residual Cs levels in soils.
Humans are exposed to different sources of radiation in the environment of which natural
sources deliver the highest radiation dose that people normally receive. The average in-situ
gamma ray spectrometry has been applied in a wide assessment of environmental radioactivity

1
 137
measurements. These include the measurements of residual Cs levels in soils (Miller and
Beck, 1984).

Radiometric technique, with their broad band of applicability to almost all soil matrix types and
their exceptional sensitivity to many elements, make it an indispensable method for
environmental research. Radiation techniques have been use to solve problems in soil fertility,
plant nutrition and environmental preservation over the past decades. Radioisotopes have been
used to study soil nutrients, water to crops from soils and from inorganic fertilizers. The
advantages of radiometric assessment make possible to differentiate the concentration of
radionuclide that is already present and the one that is added to the system. Radioisotopes occur
naturally and changes in their concentration and natural abundance in soils and plants can
provide significant information on the functioning of ecosystems (Beretka and Mattew,1985).

Beside the beneficial influence of the inorganic fertilizers on soil and agricultural plants, it is of
utmost interest to estimate site the decay of naturally occurring radionuclide in the soil to
produce significant human exposure (IAEA, 1990). Natural radioactivity in contaminated
environment is due mainly to the primordial radionuclide, 238U, 232
Th, 40
K and their progenies
which are distributed in varying amounts in the earth. Ground radiometric techniques are very
useful tools in geosciences based on the knowledge of the physical properties of radiation
sources. Gamma rays are the most penetrating radiation from natural and man- made sources,
and gamma ray spectrometry is a powerful tool for the monitoring and assessment of the
radiation environment. Portable gamma ray spectrometry is used for both regional and detailed
mapping surveys for estimating the surface concentrations of the radioelement (UNSCEAR,
2000).

Portable gamma ray spectrometry has been used for uranium exploration, geological mapping
and environmental studies. There are well-established procedures for measurement, instrument
calibration and data processing. The instruments can record the full gamma ray spectrum as well
as sum channels their hazard effect on the environment. The fertilizers are polluting the
environment as they are major source of pollution in soil and water. Fertilizers contain varying

2
amounts of heavy metals as contaminants from their source rock or other ingredients used in the
fertilizer industry.

As some heavy metals are potentially harmful to human health, attention is being given to its
avenues of entry into the human food chain. Uptake of such elements by plants consumed
directly or indirectly by humans is one avenue of entry, so the effects of heavy metal
contaminants of inorganic fertilizers are of concern (Abdel et al., 2001). Vegetables are
extensively cultivated throughout Lagos State, Nigeria either on a subsistent or commercial
scale. Farmlands in Ojo Local Government Area of Lagos State constitute a prime focus for
vegetable production (Alias et al., 2004).

One of the principal advantages of in-situ monitoring is that the detector samples the photon flux
from a large volume of soil which averages out inhomogenities. It is the most suitable method
for rapid assessment of radiation exposure, identification of radionuclide and detection of
changes in environmental radioactivity (Alaamer et al., 2008).
There is a widespread literature from many authors and researchers on the conventional method
of radionuclide determination were samples of soil or vegetation are taken from the field and
analyzed in a standard laboratory spectrometry system in order to reveal the concentrations of the
various components of the mixed radiation field but this method has the disadvantage of being
strongly inhibited by the logistic problem of carrying samples from different locations to the
laboratory. An in-situ gamma spectrometric assembly which is accurately calibrated will yield
the same information as soil samples in a much shorter time and in a much more economical
manner (Miller and Beck, 1984).

At dumpsites there are possibilities for radiation to be emitted due to the presence of radioactive
waste in the landfills as well as naturally occurring radionuclide in the soil. The radioactive
contamination of soil, water and air can be transferred to human through the soil via plants (40K)
or through inhalation (222Rn and 220Rn). This radionuclides even at low concentrations can have
potential impacts on the environmental quality and human health and may pose a long term risk.
Various studies have been carried out in recent years in Nigeria and elsewhere to investigate
radioactivity in dumpsite (Odunaike et al., 2008).

3
In this study, gamma ray spectrometry technique was used to carry out measurement of
radioactivity level in vegetable farm at Ojo Barrack, Lagos State.
`
1.2 STATEMENT OF PROBLEM:
The implication associated with radionuclides contamination in soil is of great concerned,
particularly in agricultural production system. These radionuclides can pose significant health
risk to humans in cumulative concentration above the very low body requirement because they
are non-biodegradable, have long biological half-lives and the potential accumulate in different
body organs leading to unwanted side effect.

1.3 AIM AND OBJECTIVES:

The aim of this project is to use gamma ray spectrometry technique to
investigate and assess the activity concentration of natural and artificial
radionuclides in farm soil in order to ascertain the edibility of the vegetable
plants grown and consumed by the local population residing close to this
farmland.
The objectives of the study are to:

(i) determine the range and mean activity concentrations of radionuclides in the farm soil;
(ii) evaluate the range and mean absorbed and equivalent dose rate and radium equivalent
activity of the radioelement in the study area;
(iii) calculate the annual effective dose equivalent (outdoor and indoor) and assess the level of
radioactive element for health risk assessment;
(iv) compare the internal and external indices, activity concentration index and the lateral
frequency distribution of the radionuclides concentration in the study area.

4
 CHAPTER TWO

2.0 LITERATURE REVIEW

Grasty (1975) illustrated that excessive accumulation of heavy metal in agricultural land
through traffic emission may results in soil contamination and elevated heavy metal uptake by
crops, and thus affects food quality and safety. Gamma ray spectrometry (GRS) provides a
direct measurement of the surface of the earth and with no significant depth of penetration. GRS
measures the spatial distribution of K, Th, and U in the top 30-45 cm of the earths crust.

Gourlay et al. (1996) and Tunstall et.al. (1998) demonstrated the use of radiometric data to
stratify field sampling. They advocate using only radiometrics for stratification so that individual
data layers (such as soils, terrain, vegetation etc.) are independent. Tunstall considers that the
independence of data layers is important when analysing data-sets on multiple attributes. To
apply the technique, individual classes are randomly sampled and statistical analysis was used to
combine the field sampling with the demonstration. Categorical data were converted to
numerical form and simple averaging is used to determine the average value of each soil
property in each class. Predictions of individual soil properties were provided by assuming that
all occurrences of a class have the mean value of the property for that class.

Guiraud et al., (2004) presented that modern agricultural activities adopt high technology,
aiming at increasing productivity. Plants such as soybean, corn and sugar cane use cultivars with
great genetic potential that allied with fertilizers, result in the high productivity. It is impossible
to imagine urban agriculture in the last 20 years without the utilization of large amounts of
fertilizers. This however interferes with the environment causing contamination to soil and
groundwater but the consequences are still poorly known.

Elujoba et al. (2005) explained that during the process of photosynthesis both the stable
inorganic elements and the unstable ones (radioactive element) find their way into living plants.
Natural radionuclides are transferred and cycles through natural processes and between the

5
various environmental compartment by entering into the ecosystem and food chain through
direct or indirect contamination of natural radionuclides. Thorium is almost always associated
228
with its immediate daughter product Ra, which is chemically much more mobile. Radium is
easily leached from the site of deposition and is translocated to different organs. The most
important site of deposition of radium is bone, where it becomes uniformly distributed. Ingestion
by way of food and drinking water is another possible route of entry of thorium and daughter
products into the human system.

Tzortzis (2004) illustrated that human beings are exposed outdoors to the natural terrestrial
radiation that originates predominantly from the surface of the soil. Estimation of the radiation
dose distribution is important in assessing the health risk to a population and serve as reference
in documenting changes to environmental radioactivity in soil due to anthropogenic activities.
The Naturally occurring radioactive material (NORM) represents a potential internal and
external radiation exposure hazard to both workers and members of the public through the
inhalation and ingestion of radionuclides. The specific levels of terrestrial environmental
radiation are related to the geographical composition of each lithologically separated area, and
to the content of the rock from which the soils originated in each area in the radioactive
elements of Thorium (Th), Uranium (U) and Potassium (K).

Jibiri and Farai (2005) carried out a low cost in-situ gamma-ray spectrometric method for rapid
assessment of radiation exposure, identification of radionuclides and detection of changes in
environmental radioactivity in the determination of the natural gamma radiation dose levels in
six major cities of the southeastern region of Nigeria. The soil radioactivity concentrations of the
primordial radionuclides were determined and have been related to the gamma dose rate in the
cities. The mean of the annual outdoor effective dose due to the terrestrial gamma radiation for
the region was calculated as 50 Svy-1 representing 66% of the world average value. In-situ field
gamma ray spectrometry is the collection of a spectrum of the ambient gamma ray flux at a given
site for analysis principally to identify and quantify the radionuclides present at the site. One of
the principles of in-situ measurement is that the detector samples the photon flux from a large
volume of soil which averages out inhomogenities. It is the most suitable method for rapid

6
assessment of radiation exposure, identification of radionuclides and in detection of changes in
environmental radioactivity.

Wang, et al. (2005) highlighted that Vegetables are rich sources of vitamins, minerals, trace
elements, fibers and also have beneficial antioxidant activities. They constitute an important part
of the human diet. Radionuclides contamination of the food items is one of the most important
aspects of food quality assurance. Radioactive elements are known to pose a variety of health
risks such as cancer, mutations, or miscarriages to humans. They are ranked high amongst the
chief contaminants of leafy vegetables. Due to their toxic and mutagenic effects even at very low
concentration, they are given special attention throughout the world.

International Atomic and Environmental Agency (2006) highlighted that it is possible for plants
to absorb radionuclides during nutrient absorption through their roots and transport such
nutrients via their phloem to their active portions. The rate of natural radionuclides uptake is
highly dependent on the activity concentration in the soil. The root uptake depends on soil
properties such as pH, mineralogical composition, organic matter content and nutrient status as
well as metabolic and physiological characteristics of the plant species. Plants uptake of
radionuclides is one of many vectors for the migration of natural radionuclides into humans from
the environment via the food chain. The study of the natural radionuclides levels of medicinal
plants in the environment are of interest within plant evolution and thus provide information in
the monitoring of environmental radioactivity

Farai et al. (2008) explained that many cities in the developing world, lack of access to land
make other lands including hazardous places such as road verges, banks of drainage channels
and dumpsites converted to vegetable gardens. All setbacks along major highways are used by
farmers for vegetable cultivation. Emissions of exhaust fumes from automobiles during heavy
traffic on city roads contain Lead (Pb), Cadmium (Cd), Zinc (Zn), and Nickel (Ni), which are
present in fuel as anti-knock agents. This has also led to contamination of air and soils on which
these vegetables are planted. When cultivation of vegetables is inevitable due to population
pressure, construction of barriers between roadsides and gardens could reduce the amount of
heavy metals accumulated by these crops from the emissions and other aerial sources.

7
Magaji (2012) stressed that due to the fertile nature of the soil at dumpsite, people are cultivating
some vegetables and fruit crops around it. The dumpsite is a source of pollution to soils with
leachates. It is obvious that solid waste problem has become a number one serious
environmental issue facing the country, because of its consequent effects on the pollution
of soil, water and air. Heavy metals toxicity can result in damaged or reduced mental and
central nervous function, lower energy level and damage to blood composition, lungs,
kidney, liver and other neurological organs among others. Intake of heavy metal contaminated
vegetables may pose a risk to the human health. Plants take in minerals from soil media or air
through their roots or foliage. Understanding the distribution of some trace metals in some
common vegetables and tuber crops is important for establishing baseline concentrations
from which anthropogenic effects can be measured.

Pourimani et al. (2015) explained that Plants can transfer radioactivity into human nutrient cycle
and ecosystem directly by vegetable food products and indirectly by animal food products. Also
their role is important in absorption of environmental radioactive pollutants. Plant radioactivity is
different based on soil and rock type including geographical location. Then subtle plant
recognition of each environment can prepare valuable information for researchers. Radioactivity
that is released and dispersed into the atmosphere enters the terrestrial environment due to dry
and wet deposition on soil and vegetation, causing exposure to human beings.

2.1 BASIC PRINCIPLE OF RADIOMETRIC SURVEY

Radiometric surveys involve the detection and mapping of natural radioactive emanations, called
gamma rays, from rocks and soils by using radiation detectors such as gamma ray spectrometer,
scintillation counter, and Geiger Muller counter etc. Scintillation counters are widely used in
gamma ray spectrometry. Thallium-activated sodium iodide Na(Tl) crystals are mainly used as
detectors in field gamma ray surveys.

In-situ field measurements involve the collection of a spectrum of the ambient gamma ray flux at
a given site for analysis principally to identify and quantify the radio nuclides present at the site.

8
This can be carried out in either static or dynamic mode. In static mode, the radioactivity is
measured at discrete points. In dynamic mode, the instrument is transported over fixed distances
during measurement, and the accumulated counts reflect the average radioactivity of the traverse
sector. The observed data, along with identifiers, are stored in internal memory. It is a good
practice to note any geological, topographic, climatic and environmental features that may help
with subsequent interpretation of the data. Field survey can be conducted by car-borne system,
air borne system and using portable hand held devices. All detectable gamma radiation from
earth materials come from the natural decay products of only three elements, i.e. uranium,
thorium, and potassium. The basic purpose of radiometric surveys is to determine either the
absolute or relative amounts of U, Th., and K in the surface rocks and soils ((IAEA, 1989).

In-situ Gamma-Ray Spectrometry (GRS) provides a direct measurement of radionuclides on the

surface of the earth, without considering significant depth of penetration. All rocks and soils are
naturally radioactive; containing various proportions of radioactive elements. The natural decay
of these elements produces a variety of radiation (alpha, beta, and gamma) at specific energy
levels. Only gamma ray radiation has sufficient energy to be useful for geological mapping,
exploration and environmental studies. They may be used to estimate and assess the terrestrial
radiation dose to the human population and to identify areas of potential natural radiation hazard.
They have, for example, been used to delineate areas at risk from atmospheric radon. Regional
surveys provide a base against which man-made contamination can be estimated (IAEA, 1987;
1989).

Gamma ray spectrometer is designed to detect the gamma rays associated with radioactive
elements accurately sort the detected gamma rays by their respective energies. It is this sorting
ability that distinguishes the spectrometer from instruments that measure only total radioactivity.
The soil is a source of food we eat, so whatever is present in the soil, either beneficial or
hazardous must be known. The natural radioactivity of soil is weak and due to the presence of
the elements uranium, thorium and potassium, these elements emit energetic and highly
penetrating radiation (known as gamma radiation) which is capable of destroying or causing
mutations in cells of living beings. If available in high concentrations in environments, these
elements could pose community health problems. Most countries measure their concentrations in

9
the environment (soil, vegetation and air etc.) as these elements could also be altered in course of
time due to human activities (UNSCEAR, 2000).
2.2.1 NATURAL RADIOACTIVE DECAY AND ITS ORIGIN
A brief disintegration or decay of radioactive element can be explained from Figure 1 below:

Figure: 2.1 Principles Guiding the Decay of Radioactive Element (IAEA, 2003)

2.2.2 NATURAL AND FALLOUT RADIONUCLIDES

The activities of many radionuclides belonging to natural decay series can be measured using
40 238 226 210
gamma spectrometry. This includes K and U, Ra and Pb of the uranium decay series
232 228 228
and Th, Ra and Th of the thorium decay series (Avwiri, et al., 1968). The fallout from
atmospheric explosions and accidents causes some background particularly in the northern
137
hemisphere principally from Cs with gamma ray energy of 662keV. Parent isotope and their
corresponding daughter radionuclide in their respective gamma lines are shown in Table 2.1.

10
 Table 2.1: Gamma-Ray Energies for Calibration of Spectrometer (IAEA, 2003).

Parent isotope Daughter Gamma-ray energy Gamma-emission

nuclide (keV) probabilities (%)
226 214
Ra Pb 351.9 37.6
232 228
Th Ac 911.2 26.0
40
K - 1460.7 10.7
137
Cs - 661.7 84.6

The uranium decay series found in soils and rocks is shown in Figure 2.2 (UNSCEAR, 2000)

Figure: 2.2 Uranium Decay series by (United Nations Scientific Committee on Effect of
Atomic Radiation (UNSCEAR, 1988).

238
Natural decay series of U and 232Th are studied for secular equilibrium of chain segments, an
implication in environmental gamma-ray spectrometry measurements. When unstable atom
tries to reach a stable form, energy and matter are released from the nucleus.

11
This spontaneous change in the nucleus is called radioactive decay. Radioactive decay is the
process by which an atomic nucleus of an unstable atom loses energy by emitting ionizing
particles (ionizing radiation) nucleus is called radioactive decay. When there is a change in the
nucleus and one element changes into another, it is called transmutation. Radioactive decay is
random and unpredictable processes (Beretka, 1985).
2.2.3 MAIN RADIOACTIVE DECAYS

The atom is considered the smallest constituents of matter that distinguish their chemical
properties that consist of a nucleus surrounded by electrons. The nucleus consists of positively
charged protons, and uncharged neutrons; both called nucleons. In general, an assembly of
nucleons, with its associated electrons, should be referred to as a nuclide.

The diameter of an atom is of the order 10-10 m, and the diameter of a nucleus is of the order of
10-15 m (Kogan et al., 1971).

The nucleus is commonly identified by the notation above:

2.0

where X is the chemical symbol of the element, Z is the number of protons in a nucleus (called
the atomic number) and defines the element (Z will also be the number of orbital electrons), N
the number of neutrons in a nucleus and A is the mass number given as the total number of
nucleons, A = Z + N. Known the relationship between Z, N and A and because the chemical
symbol uniquely identifies the element (the atomic number as subscript is usually omitted), this
notation is written simply as AX.

Atoms of an element having the same atomic number but different numbers of neutrons (i.e.
Different mass numbers) are called isotopes. Isotopes have identical chemical properties, but
different physical properties. The atomic nuclei of some isotopes have a surplus of energy, are
unstable, and disintegrate to form more stable nuclei of a different isotope. This process is
accompanied by the emission of particles or electromagnetic radiation, termed nuclear radiation.
Nuclides with this feature are called radionuclide, and the process is called nuclear or
radioactive decay.
Alpha Decay
12
An alpha particle, , is a highly energetic helium nucleus that is emitted from unstable heavy
nuclei having high atomic numbers (Z > 83). Since the atomic number and mass numbers are
conserved, an alpha decay can be written schematically to show the relationship between the
parent and daughter nucleus in equations 2.1 and 2.2 below.

4
2 + 42 2.1

where X and Y are the initial and final nucleus species. A typical example is the decay of the
isotope of 226Ra in 222Rn (part of the 238U decay chain):
226 222
88 86 + 42 + 2.2

where Q is the quantity of energy released, equal to the difference in mass between the initial
nuclide and final products shared in a definite ratio because of the conservation of momentum.
For the above example, Q= 4.871 keV, is the energy shared between the Rn and the He, releasing
a mono-energetic alpha particle
Beta Decay
137
An example, of decay is the transformation of Cs to 137Ba shown in the equation below:

137 137
55 56 + + + 2.3
In this case, the decay energy, Q = 1.176 MeV, is shared between the particles in inverse ratio to
137
their masses in order to conserve momentum. The mass of Cs is very large compared to the
mass of the beta particle and neutrino and takes a very small, insignificant portion of the decay
energy. Therefore, the beta particle and the anti-neutrino share almost the whole of the decay
energy in variable proportions ranging from zero to100%.
Gamma Emission
This is not a form of decay like alpha or beta, in that there is no change in the number or type of
nucleons in the nucleus; there is no change in Z, N or A. Gamma-rays are monochromatic
electromagnetic radiations that are emitted from the nuclei of excited atoms following
radioactive transformations: they provide a mechanism of reaching the nuclei energetic stability.
As shown above, gamma emissions usually follow alpha or beta decays since will often lead to
excited states in the daughter nucleus. These transitions are known as isomeric transitions and

13
the long-lived excited states, XA, are called isomeric states or isomers (sometimes metastable
states).

+ 2.4

process that often competes with gamma emission is internal conversion, in which the nucleus
de-excites by transferring its energy directly to an atomic electron, which then appears as free
electrons.
2.2.4 LAW OF RADIOACTIVE DECAY
The Decay Equation
Radionuclides are unstable and decay of one, or more, of the decay modes; alpha, beta minus,
beta plus or electron capture. The amount of a radionuclide in a sample is expressed in Becquerel
numerically equal to the rate of disintegration the number of disintegrations per second. We
refer to this amount as the activity of the sample. The rate of decay is directly proportional to the
number of atoms of the radionuclide present in the source, i.e. the activity, A, is directly
proportional to the number of atoms, N, of nuclide present (Kogan et al., 1971).

The proportionality constant , is called the decay constant (the probability per second that the
emission takes place) and has the units of reciprocal time (s-1). The reciprocal of the decay
constant is the mean lifetime of the radionuclide, the average time which an atom can be
expected to exist before its nucleus decays (IAEA, 2003).

This time represents a decay of the source by a factor of e (i.e. 2.718). It is more convenient and
meaningful to refer to the half-life, t1/2, of the radionuclide the time during which the activity
decreases to half its original value and can be shown in equation 2.5 to 2.7 below:
2 0.693
1/2 = = (, 2003) 2.5

Integrating the Eq. 6 lead to the exponential law of radioactive decay which relates the number
of atoms (Nt ) at a time (t) and half-life (t1/ 2):

() = 0 = 0 2 (, 2003) 2.6
1/2

14
where 0 is the number of atoms at time t = 0. In practice, it is more useful to replace the
number of atoms by activity, bearing in mind that activity is proportional to the number of
atoms:
() = (, 2003) 2.7
10
The historical unit of activity has been the curie (Ci), defined as exactly 3.7 x10
disintegrations/second (s-1 ) which owes its definition to its origin as the best available estimate
of the activity of 1 gram of pure 226Ra. Although still widely used in the literature, the curie is
destined to be gradually replaced by its SI equivalent, the Becquerel (Bq), defined as
disintegration per second, thus:
1 = 2.7031011 (, 2004) 2.8

2.2.5 RADIOACTIVE DECAY SERIES

238 235 232
The natural decay series of U, U and Th are an example of natural radioactive decay
series and therefore are briefly discussed in this section. Radioactive decay series (or chain) often
occurs in a number of daughter products, which are also radioactive, and terminates in a
stable isotope ( ) ( ) (). Assuming that at time t = 0 we have NA0 atoms
of the parent element and no atoms of the decay product are originally present, the number of
the parent nucleus decrease with time according to equation 2.9 to 2.13 below:
= 0 ( . 2003) 2.9
While the number of daughter nuclei increases (grow-up) as a result of the decays of
the parent and decreases as a result of its own decay:

= ( . 2003) 2.10

The solution of the first order differential equation( /) + = is of the form

0
= ( ) 2.11

0
= ( ) 2.12

From Eq. 2.11 and Eq. 2.12 can we calculated the relative activity ratio of the two species:

= (1 ) 2.13

: in the case when the half-life of nuclide is much greater than the half-life of
nuclide, so the parent decays at constant rate we have: = 0 (1 )

15
This equation expresses the secular equilibrium condition, where, as the time t becomes larger
nuclei B decay at the same rate at which they are formed =
This result can also be immediately obtained from (Eq.14), taking dNB/dt = 0. For practical
purposes, equilibrium may be considered to establish after the seven half-lives of daughter
radionuclide.
In the study of uranium decay chain through gamma-ray spectrometry techniques it is important
226
to emphasize that some long lived radionuclides, e.g. Ra, can be the head of decay chain
segments which can be directly measured or through equilibrium grow-up conditions. In
226
gamma-rays spectrometry measurements, Ra can be directly measured through its gamma ray
emitted, 186.2 keV. However, this shows some difficulties since generally it is recorded as a
235 214 214 226
doublet with 185.7 keV from U. Instead Pb and Bi are directly measured and Ra is
estimated under the equilibrium grown up condition, which is generally reached through radon
tight containers within 26.7 days .While, thorium and its daughters are generally found in secular
232 228
equilibrium. However, in Th decay chain the two chain segments headed by Ra (measured
through 228Ac) and 228
Th (measured through 212
Pb, 212
Bi and 208Tl) reach the secular equilibrium
in about one month.

2.2.6 ORIGIN OF NATURAL RADIOACTIVITY

Cosmic Radiation
The primary sources of cosmic radiation are the galaxies in outer space and secondary source is
the Sun in our solar system (significant during maximum sun cycle activity). The galactic cosmic
radiation coming at the upper atmosphere is made up of about 98% baryons and 2 % electrons. It
consists mainly of protons (87 %) and to a lesser extent of helium ions (11 %) and heavier ions
(ranging from carbon to iron; 1 %), with energies ranging from 102 MeV to more than 1014 MeV
(Reitz, 1993). The result of the cosmic radiation is a continuous bombardment of Earth's
magnetosphere by a nearly isotropic flux of charged particles having, different energies.
However, only a part of the cosmic radiation actually reaches the surface of the Earth.
Furthermore, charged particles are deflected from the Earth's magnetic field component that is
perpendicular to the direction of particle motion. This means that the cosmic radiation is
deflected more at the equator than near the poles producing a geomagnetic latitude effect of
cosmic radiation (Bartlett, 2004).

16
Primordial Radionuclides and their Distribution in Rock and Soil
Primordial radionuclide called also terrestrial radionuclides found in nature are related
primarily to the fact that these isotopes themselves have very long half-lives or are created in
decay chains with the head parents having very long half-life. The principal sources of
238
environmental radioactivity monitoring interest are due to the presence of U, 232Th and 40K in
the Earths crust. Generally, other major trace elements like 235U and 87Rb are present. The world
238 232
average abundances of the continental upper crust for U, Th and 40K are respectively 2.7
g/g, 10.5 g/g and 2.3% (Rudnick and Gao, 2003).

2.3 SOILS-TO-PLANT UPTAKE OF RADIONUCLIDES AND PUBLIC EXPOSURE

238 232
Natural radioactivity comes mainly from the primordial radionuclides U, Th, their decay
products, and 40K, which are present in all ground formations. The radionuclides that occur
naturally in soil are metabolically incorporated into plants. Artificial radionuclides introduced
into soil behave in a similar manner. These radionuclides can be incorporated into vegetation
through uptake of radionuclides by the root system or due to activity interception by external
surfaces of plants. To determine the radioactivity levels in vegetables and soil to plant transfer
factors of radionuclides (226Ra, 234
Th and 40
K) Pring onions, Ewedu, Green Soko and Garbage
was selected spanning across the square plot in the cultivated soil.

2.3.1 EXPOSURE TO RADIATION

People are constantly exposed to small amounts of ionizing radiation from the environment as
they carry out their normal daily activities; this is known as natural background radiation.
Radiation has always been present and is all around us. Life has evolved in a world containing
significant levels of ionizing radiation. Our bodies are adapted to it. The following are the four
major sources of public exposure to natural radiation:

cosmic radiation

terrestrial radiation

inhalation

17
 ingestion

2.3.2 EXPOSURE FROM COSMIC RADIATION

The earth's outer atmosphere is continually bombarded by cosmic radiation. Usually, cosmic
radiation consists of fast moving particles that exist in space and originate from a variety of
sources, including the sun and other celestial events in the universe. Cosmic rays are mostly
protons but can be other particles or wave energy. Some ionizing radiation will penetrate the
earth's atmosphere and become absorbed by humans, which results in natural radiation exposure.
The doses due to natural sources of radiation vary depending on location and habits. Regions at
higher altitudes receive more cosmic radiation.

2.3.3 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,
will 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 from indoors as well as outdoors.

2.3.4 EXPOSURE THROUGH INHALATION

Most of the variation in exposure to natural radiation results from inhalation of radioactive gases
that are produced by radioactive minerals found in soil and bedrock. Radon is an odorless and
colorless radioactive gas that is produced by the decay of uranium. Thoron is a radioactive gas

produced by the thorium. Radon and Thoron levels vary considerably by location depending on
the composition of soil and bedrock. Once released into the air, these gases will normally dilute
to harmless levels in the atmosphere but sometimes they become trapped and accumulate inside
buildings and are inhaled by occupants. Radon gas poses a health risk not only to uranium
miners, but also to homeowners if it is left to collect in the home. On average, it is the largest
source of natural radiation exposure.

2.3.5 EXPOSURE THROUGH INDIGESTION

18
During the process of photosynthesis both the stable inorganic elements and the unstable ones
(radioactive element) find their way into these plants. Plants absorb radionuclides during nutrient
absorption through their roots and transport such nutrients via their phloem to their active
portions. Plants uptake of radionuclides is one of many vectors responsible for the migration of
natural radionuclides into humans from the environment via the food chain. The health effects of
radiation exposures to NORMs (Natural Occuring Radioactive Materials) from intake of
vegetable plants as food are the cause of most forms of leukemia and cancer of many organs
210
such as the bone, lung, breast and thyroid in the long term since approximately 10e15% of Pb
and 214Pb ions, 99% of 226 Ra and 228Ra, 214Bi (bone seeker) and 210Po (soluble) reaches the blood
and the lung fluid stream and are distributed to the whole body (UNSCEAR, 2000). Generally,
lead contaminations occur in vegetables grown on contaminated soil. Lead poisoning is a global
reality, and fortunately is not a very common clinical diagnosis yet in Nigeria except for few
occupational exposures (Adewuyi et al., 2006).

2.4 GROUND RADIOMETRIC METHOD

Ground radiometric plays an important role in examining the physico-chemical properties of
radioactive elements. Uranium and it's daughter elements are undergoing constant disintegration
and releasing alpha and beta particles and gamma radiation characteristic of daughter elements
214 226 238
Bi, Ra of the U series indicates the presence of U. Radiometric surveys measure the
distribution of three radioactive elements (uranium, thorium and potassium) in the Earth's crust,
by recording the gamma-radiation emitted during the decay of these elements.

Devices that measure gamma radiation sample a larger volume of rock or soil than either alpha
or beta detectors. Alpha particles have a mass of four atomic mass units and are stopped by
collisions with other atoms. Few alpha particles escape from the soil or rock and are stopped
within a few micrometers of their origin by rock and within a few centimeters by air. Beta
particles are electrons which have a much lower mass but are still stopped easily by collisions
with solid matter.

Gamma photons have no mass and in general more energy than either alpha or beta particles
emitted by the nuclides in the uranium decay series thus they can penetrate tens of centimeters of

19
rock before being attenuated. Alpha, beta, and gamma radiation have greatly different abilities to
escape the soil or rock where they originate. Alpha measurements are from the surface only.
Beta measurements test only the first centimeter of the surface. Gamma measurements range
from ten cm to a meter in depth. Some gamma rays lose energy by scattering in escaping from
the source and also during passage through the air to the crystal. This therefore guides us in
knowing that the closer the device is placed to the sample the more accurate the reading (Santos
et al., 2006).

2.4.1 MODE OF DEPLOYMENT OF GROUND RADIOMETRIC SURVEY

The equipment for in-situ measurement of radioactive element on the field involves: Portable
gamma ray spectrometer using NaI(Tl) crystals as detectors, GPS, Meter rule, pencil and pen and
field note book. In this work the static mode was adopted since the equipment is a portable
handheld device, the radio elements are measured at discrete points along each traverse. A square
grid of 100m x100m was measured in the Vegetable farm and 10 traverses of 100m in length
was realized spaced at 5m apart. The total discrete point of 200 was mapped spread across the
square grid.

The portable GRS device was used for taking readings, and was calibrated for Background
radiation. The spectrometer readings were taken with the same sample spacing of 5m across the
whole square grid, and a total count reading within 60 seconds was observed for each mapping.
All data obtained will be recorded, stored and compiled both manually, and written in the field
note books and electronically in the memory storage of the device.

2.4.2 GAMMA RAY SPECTROMETER

Portable hand-held gamma ray spectrometers are widely used in field studies. Portable threshold
spectrometers have up to 100 cm3 of NaI(Tl) crystals as detectors, and several switch-operated
energy thresholds. The threshold can be set to a low energy for total count measurement and to
energies slightly below 1.46 MeV, 1.76 MeV and 2.62 MeV for K, U, and Th measurement,
respectively. A reference gamma ray emitting source is used for instrument gain adjustment.

Threshold spectrometers with small crystal volumes are suitable for crude spot measurements of
total count anomalies. Portable hand-held gamma ray spectrometers are widely used in field
20
studies and it is a logical extension of the scintillometer where it separates characteristic gamma
rays of 40K, U and Th for identification of the source.
Most modern portable gamma ray spectrometers are differential spectrometers. These typically
have at least 350 cm3 of NaI(Tl) detectors and record either 256 or 512 channel of data in the
energy range 0-3 MeV (IAEA, 2003).The instruments can record the full gamma ray spectrum as
well as sum channels over broad energy windows for the in-situ - estimation of K, U and Th
radioelement concentrations.

2.4.3 RS-230 BGO SUPER SPEC GROUND RADIATON DETECTOR

Systematic detailed ground RS-230 BGO SUPER SPEC gamma ray spectrometric is a portable
state of the art remote sensing unit use for measuring the vertical and lateral spatial distribution
of the radioelement concentration. Instant air dose rate indices in D(nGyh-1) or D(nSvh-1) are
displayed on the screen of the detector, provided by Radiation Solutions Canada. It offers an
integrated design with a large detector, direct assay data, data storage, ease of use and highest
sensitivity. The spectrometer uses 6.3cu in3 bismuth germinate oxide detector which provides
typically three times equivalent performance over comparably sized Sodium-Iodide detectors
(IAEA, 2003).

The detector is previously calibrated and self-stabilized to gives a direct measurement of total
radiation of uranium and thorium concentrations in ppm, potassium concentration in percentage
and the dose rate. Both the spectrometer function and variations in background radioactivity have
been checked daily at an established reference station in the survey area. The assay time was set
to one minute to achieve the best accuracy. The assay data were stored on the internal memory of
the spectrometer which is then dumped into the PC using the GeoView software delivered with
the spectrometer. In this study, the software was not available and Microsoft excel was use to
process and analyzed the result both qualitatively and quantatively. The locations of the
measuring points were identified using a Garmin GPS model 71, and the measurement was
recorded on a field note book (IAEA, 2003).

2.4.4 FACTORS INFLUENCING GAMMA RAY SPECTROMETRY

21
The gamma ray method is unusual in that it requires the consideration of many factors. The
source intensity and the source-detector geometry affect observed gamma ray fluence rates.
Environmental and other effects such as soil moisture, rainfall, vegetation, non-radioactive
overburden, and the distribution of airborne sources of radiation all affect the measured fluence
rates (International Atomic and Environmental Agency, 2003).
The number of gamma rays counted at a given measurement point depends on several factors
listed below:
Sensor Field of View: only photons traveling along a path contained within the sensor field of
view will have a chance to interact with the detector.
Soil Density: soil density affects photon attenuation and thus the number of counts recorded
per disintegration.
Gamma-ray Energy: photon energy affects photon attenuation and thus the number of counts
recorded per disintegration.
Detector Efficiency: some, but not all photon-detector interactions produce a valid count
depending on the detector efficiency.
Amount and Distribution of Radionuclide in the Soil: the source geometry (concentration and
distribution) is the parameter solved for in the conversion process - normally, exponential
distribution must be assumed in order to determine concentration.

2.4.5 APPLICATION OF RADIOMETRIC METHOD

The method can be applied to a large variety of environmental and biological materials such as
air, water, soil, sediments, vegetation (grass, hay, etc.) and, particularly, individual foods of
vegetable and animal origin as well as total diet mixtures. Portable gamma ray spectrometry has
been used since the 1960s for uranium exploration, geological mapping and environmental
studies (International Atomic and Environmental Agency, 2003).

22
2.4.6 ADVANTAGES AND LIMITATIONS OF IN-SITU MEASUREMENT OF GAMMA
RADIONUCLIDE ACTIVITY IN SOIL

2.4.6.1 ADVANTAGES OF IN-SITU MEASUREMENT SPECTROMETER

(i) They have the ability to measure gamma emitters directly in the original sample
without the need for chemical separations.
(ii) They allows both qualitative identification and quantitative determination of the
radionuclides in a sample.
(iii) In-situ measurement relates to the detector field of view which enables appropriate
detector design and placement, permitting count of photons emitted over an extended
area to be mapped.
(iv) Provide a means for the complete characterization of the gamma radiation field at a
given location
(v) Direct and quick assay for the individual contributions of K, U and Th, the three
radioactive elements and measurement of the dose rate.
2.4.6.2 LIMITATIONS OF IN-SITU MEASUREMENT SPECTROMETER

(i) The scintillometer only records total count reading and has to wait on lab results and
further analysis before knowing whether an anomalous zone is mainly uranium.
(ii) The determination of depth distribution of a radionuclide requires measurements of
several samples taking at different depth.
(iii) Poor determination of radionuclides in a disturbed terrain by erosion and human
activities.

23
2.5. GENERAL GEOLOGY OF SOUTH WESTERN NIGERIA
Nigeria lies approximately between latitudes 4oN and 15oN and Longitudes 3oE and 14oE, within
the Pan African mobile belt in between the West African and Congo cratons. The Geology of
Nigeria is dominated by crystalline and sedimentary rocks both occurring approximately in equal
proportions. The geology map of Nigeria is shown in Figure 2.4 below.

The crystalline rocks are made up of Precambrian basement complex and the Phanerozoic rocks
which occur in the eastern region of the country and in the north central part of Nigeria (Jones
and Hockey, 1964). The Precambrian basement rocks in Nigeria consist of the migmatite
gneissicquartzite complex dated Archean to Early Proterozoic (2700-2000 Ma).

Other units include the NE-SW trending schist belts mostly developed in the western half of the
country and the granitoid plutons of the older granite suite dated Late Proterozoic to Early
Phanerozoic (750-450Ma) (Jones and Hockey, 1964).

Figure: 2.3 Geological map of Nigeria (After Jones and Hockey, 1964).

24
2.5.1 DAHOMEY BASIN
The Dahomey basin is a combination of inland/coastal basin that stretches from south eastern
Ghana through Togo and the republic of Benin to south-western Nigeria. It is separated from
the Niger Delta by a subsurface basement high referred to as the Okitipupa ridge. Its offshore
extent is poorly defined. Sediment deposition follows an east- west trend. In the Republic of
Benin, the geology is fairly well known (Billman, 1976; De Klasz, 1977). In the onshore,
cretaceous strata are about 200m thick (Okosun, 1990).

A non-fossilliferous basal sequence rests on the Pre-Cambrian basement. This is succeeded by

coal cycles, clays and marls which contain fossilliferous horizons. Offshore, a 1000m thick
sequence consisting of sandstones followed by black fossilliferous shale towards the top has
been reported. This was dated by Billman (1976) as being Pre- Albian to Mastrichtian; the
cretaceous is divisible into two geographic zones, North and South. The sequence in the
Northern Zone consists of basal sand that progressively grades into clay beds of the Mastrichtian
are almost entirely argillaceous. The Southern zone has a more complicated stratigraphy with
limestones and marl beds constituting the major beds.

2.5.2 STRATIGRAPHY OF THE DAHOMEY BASIN

The most recent and detailed stratigraphy is that of Omatsola and Adegoke (1981). They
proposed three new easily recognized litho-stratigraphic units of formational rank which are; Ise
Formation, Afowo Formation and the Araromi Formation, these units make up the Abeokuta
group. Others include the Ewekoro Formation, Oshosun Formation, Akinbo Formation and Ilaro
Formation as shown in Figure 2.4.

25
Figure 2.4: Stratigraphic column of the Eastern Dahomey Basin (Omatsola and Adegoke,
1981).

2.5.3 ISE FORMATION

This is referred to as the oldest sedimentary unit found in the south-west of Nigeria (Omatsola
and Adegoke, 1981). It is a pre-continental drift sequence of continental sand, grits and
sandstone overlying the basement complex (Omatsola and Adegoke, 1981).

2.5.4 AFOWO FORMATION

This unit unconformably overlies the Ise formation. The beds are mostly composed of coarse to
medium grained sandstone with variable, but thick shale, and clay (Omatsola and Adegoke,
1981).

2.5.5 ARAROMI FORMATION

This formation overlies the Afowo unit and it is the youngest stratigraphic unit within the
Abeokuta group (Omatsola and Adegoke, 1981). The formation was formerly referred to as the
Araromi shales by Reyment (1965), but formation by later authors. The unit is composed of
fine-medium grained sand at the base, which is overlain by shale and silt with thin inter bedded
limestone and marl, especially at its upper boundary with the carbonaceous Ewekoro Formation.

26
The shales are light gray to black in colour, highly fissile and well laminated and are rich in
organic Carbon.

2.5.6 EWEKORO FORMATION

This formation was discovered by Jones and Hockey (1964) and was found to be unit overlying
the Araromi Formation uncomformably. The type section is the limestone unit exposed in the
Ewekoro quarry.

2.5.7 AKINBO FORMATION

This unit is the lateral equivalent of the Imo Formation in the south-eastern Nigeria (Adegoke,
1969), and it is overlain by the Oshosun Formation (Omatsola and Adegoke, 1981). Also, Ogbe
(1972) demonstrated that the shales on either side of the Okitipupa Ridge differ markedly from
each other in physical featured. He then proposed the name Akinbo Formation for the unit in the
western side of the ridge, and selected the section exposed in the Ewekoro and Shagamu quarries
as the type locality. It is composed of shale, glauconitic rock band, and gritty sand to pure gray
and little clay.

The shales are greenish to greenish gray with thin band and lenses of limestone from the
Ewekoro Formation grading laterally into the Akinbo shale near the base (Ogbe, 1972).

2.5.8 OSHOSUN FORMATION

The name Oshosun was first used in geological literature in connection with description of
phosphoric deposits which are best developed near the Oshosun village by Russ (1924). The
Oshosun Formation is composed of pale greenish laminated and glauconitic shale (Russ, 1924).

2.5.9 ILARO FORMATION

This formation was named by Jones and Hockey (1964) for a sequence of predominantly coarse
sandy estuarine, deltaic and continental beds which display rapid lateral facie changes. The
contact between the Ilaro Formation and the Oshosun is marked at the base of the first major
sandy bed above the Oshosun Formation (Kogbe, 1976) with the formation consisting of gritty
clay, gritty sand, yellowish brown shale, fine to coarse grained sand, bluish gray mudstones
grading into glauconitic shales of the underlying Oshosun Formation.

27
2.6 GEOLOGY OF LAGOS STATE

The geology of Lagos is mainly sedimentary of tertiary and quaternary sediment. There is no
basement outcrop within the state, because its basement is several kilometers beneath the earth
surface, hence, it is not reachable with the type of survey in this research. Lagos state lies on the
longitude 30E and latitude 60N with alternate wet and dry seasons. Tertiary sediments are
unconsolidated sandstones, grits with mudstone band and sand with layers of clay. Quaternary
sediments are recent deltaic sands, mangrove swamps and alluvium near the coast.

Lagos is located within the Western Nigeria coastal zone, a zone of coastal creeks and lagoons
developed by barrier beaches and sand deposition, underlain by recent deposits which vary from
the littoral and lagoon sediments to the coastal belt and alluvial deposits of the major rivers. The
surface geology is made up of the Benin formation (Miocene to Recent) and the recent littoral
alluvial deposits. The Benin formation consists of thick bodies of yellowish (ferruginous) and
white sands (Jones and Hockey, 1964).

2.6.1 GEOLOGY OF THE STUDYAREA

The present study was undertaken in a former dumpsite that was later converted to vegetable
garden at Ojo Barrack, southwest city, Lagos state of Lat.60 27' 43.59"N and Long.30 12'
27.79"E.The area has a bimodal rainfall pattern with peaks in June and September and is the
commercial capital of Nigeria, characterized by the heaviest traffic on major highways along
where the commercial vegetable cropping takes place. The soils in this area are from
sedimentary rock formation. A total area under cultivation is about two heater and irrigated by
stagnate water. The main vegetables cultivated in the study area are spring onions, Amaranthus
hybriddus (green), Celosia argentea (soko), scent leave, okra, eggplant and garbage, Cochorus
olitorus (Jute, ewedu) ( Adu et al., 2014).

On the vegetable farm inorganic fertilizers are added into the soil year after year to enhance the
yield of these edible vegetables. There is constant dumping of waste very near the study area and
it is very close to the market. The farmers are illiterate dominated by peasant dwellers.
The study area renders foul smell as a result of lack of toilet and the dwellers defecate very close
to the vegetable farm.

28
Market waste and residential waste such as sugarcane molasses, scraps of metals (from used
items like vehicles, household electronics (television sets etc.) ashes, cattle dung and other
animal wastes (bones) from a small abattoir in the area.

Figure: 2.5 Site Map of the Study Area

Figure. 2.6: Vegetable Farm in the Study Area

29
 CHAPTER THREE

3.0 METHODOLOGY
3.1 DATA ACQUISITION
The data was acquired using RS-230 BGO Super SPEC hand held gamma ray spectrometer, a
self-stabilizing unit, measuring tape for measuring the distances , Global Positioning System
(GPS) for locating the position and elevation of the survey point, and a field note for recording
the field data. A square grid of 100m by 100m layout measured in the vegetable farm and 10
traverses were set out at 5m spacing. The in-situ radiometric survey was carried out in static and
assay mode of operation within the study area. In static mode, the radionuclides were assessed at
discrete point along the traverses. A total of two hundred sampling point were measured at
predetermined distance.

The measurements were made by holding the portable detector 1m above the ground surface at
each sampling point in the study area. The assay mode displayed the concentrations of the K %,
U (ppm) and Th (ppm) at a count rate of 60 seconds on the Liquid Crystal Display (LCD) screen.
Site coordinates were also recorded for the purpose of tracing the sampling point using a Global
Positioning System (GPS). The field work took a couple of three days; stagnant irrigated water
was avoided at the ground surface prior during measurement. Precautionary measures were taken
to ensure the reliability of the measurements. To minimize the interference due to
geomorphology, relatively flat laying area were chosen. The field equipment RS-230 BGO Super
SPEC for data acquisition is shown in plates 1 and 2.

30
 Plate1: RS-230 BGO Super SPEC Hand held Gamma-Ray Spectrometer

3.2 SETTING OF DEAD TIME ON THE DETECTOR

Instruments used for in-situ gamma ray spectrometry are usually specified by the energy
137
resolution of the Cs photopeak at 662 keV. Dead time of 60 seconds was set during the
measurement which refers to the finite time required for the detector to process an individual
particle of radiation. During this time all incoming pulses are ignored during the survey.

Plate.2: Field operation using RS- 230 BGO Gamma Ray Spectrometer recording of
Assay result at Ojo Barrack

31
 3.3 DATA PROCESSING AND INTERPRETATION

3.3.1 STATISTICAL ANALYSIS OF THE RADIOMETRIC DATA

Radioactive decay is a statistical phenomenon. The range, mean and standard deviation of
activity concentration of K, U, and Th in the study area were determined from statistical analysis
using Microsoft excel for extracting subtle information, due to the fact that geologic structures
are not uniform in radioactivity. The analysis was to look at deviations from the unit means.
Large deviation from the mean could be due to errors in the mapping of the unit boundaries.
Since atomic disintegration during radioactive decay occurs completely independently of every
other decay event, and time interval between disintegrations is not constant. For a large number
of randomly disintegrating atoms of a particular radionuclide, the frequency of radioactive decay
is given by Poissons distribution ( . , 1997).

For Poissons distribution to hold, the variance 2 of a distribution is equal to the mean value and
is the standard deviation as shown in Equation 3.1 to Equation 3.4 (Kogan et al., 1997).

() = exp( ) 3.1
!

Where is the decay rate, is the probability, that the number of atomic nuclei will decay
within a time unit.

The emission of particles and gamma rays in radioactive decay is proportional to the number of
disintegrating atoms, and the standard deviation may be used to estimate the range of deviations
and errors of the radiometric measurements.

If counts are recorded in time t, then the standard deviation of the recorded counts is:

() = 3.2

Where is the mathematical expectation of the number of counts (the mean count of repeated
measurements). The fractional standard deviation of a count (error of measurement of ) is:

() 1
=

For a count rate = ( ), the standard deviation is given by () = / = 3.3

32
And the fractional standard deviation of the count rate n (error of measurement of n) is:

() 1
= 3.4

The probable deviation (P= 0.5) is 0.674 , a multiple of standard deviation. Equations

(3.1) and (3.4) indicate that the precision of radiometric measurements can be increased by

increasing the counts, N, increasing the count rate, n, and by increasing the counting time, t.

3.3.2 DETERMINATION OF RADIOLOGICAL HAZARD INDICES

The radiological hazards in the study area under investigation can be known by calculating the
238
activity concentration of U, 232Th and 40K measured. The hazard associated with radioactivity
is assessed through hazard indices. The various types of radiological hazard indices are the
radium equivalent activity, external and internal hazard indices, radioactivity level index, dose
rate, annual effective dose and total absorbed dose rate

3.3.3 RADIUM EQUIVALENT ACTIVITY (Raeq)

226
For the purpose of comparing the radiological effect or activity of materials that contain Ra,
232 40
Th and K by a single quantity, which takes into account the radiation hazards associated
with them, a common index termed the radium equivalent activity (Raeq) is used. This
activity index provides a useful guideline in regulating the safety standards on radiation
protection to the general public residing in the area under investigation.

The Raeq index represents a weighted sum of activities of the above mentioned natural
radionuclides and is based on the estimation that 1Bqkg -1 of 226
Ra, 0.7 Bqkg 1of 232
Th,
and 13Bqkg 1 of 40K produce the same gamma radiation dose rates (Beretka and Mathew,
1985).
The permissible limit of Raeq is 370Bq.kg-1 in soil that contain 238
U, 232Th and 40K measured in
Bq.kg-1 (UNSCEAR 2000).
The index is given as:
Raeq = CRa + 1.43CTh + 0.077Ck (UNSCEAR 2000) 3.5
Where CRa, CTh and Ck are the average activity concentration in Bqkg1 of 226Ra, 232Th, and 40K,
respectively.
33
3.3.4 DETERMINATION OF EXTERNAL (Hex) AND INTERNAL HAZARD INDEX (Hin)
The decay of naturally occurring radionuclide in soils produces a radiation field that transcends
the soil-air interface to produce a significant human exposure (UNSCEAR, 2000).
The quantification of this exposure factor was determined by external hazard index, which is
given by the following expression (equation 3.6).

= + 259 + 4810 1 (UNSCEAR, 2000) 3.6
370

Internal exposure to radon and its daughter products are very hazardous and can lead to
respiratory diseases like asthma and cancer, and can be calculated by the expression (equation
3.7).

= + + 1 (UNSCEAR, 2000) 3.7
185 259 4810

The values of the indices (Hex, Hin) must be less than unity for the radiation hazard to
negligible.
3.3.5 CALCULATION OF ANNUAL EFFECTIVE DOSE RATE (AEDR)
The annual effective dose rates, the conversion coefficient from absorbed dose in air to effective
dose (0.7Sv.Gy-1) and outdoor occupancy factor (0.2) (i.e. people on the average spent 20% of
their time outdoor) were calculated according to (UNSCEAR 2000). An increase in the
representative gamma index greater than the universal standard of unity may result in radiation
risk leading to the deformation of human cells thereby causing cancer.
The annual effective dose rate (mSv.yr-1) was calculated using the following formula shown in
equation 3.8(UNSCEAR 2000).
( ) = ( ) 8760 0.7 (103 /109 ) 0.2
= 1.21 103 ( ) , 2000 3.8
OR
()(Sv/y) = (1 ) 8760 0.7/ 0.2 103
To estimate the annual effective dose, the conversion coefficient from absorbed dose in air to
effective dose (0.7Sv.Gy-1) and indoor occupancy factor (0.8), (i.e. people on the average spent
80% of the time indoor) proposed by UNSCEAR 2000 are used. Hence, the annual effective
dose (mSv.yr-1) was calculated using the following formula shown in equation 3.9 (UNSCEAR,
2000).
() = ( ) 8760 0.7 (103 109 ) 0.8

34
 = 4.91 103 ( ) (, 2000) 3.9
()(Sv/y) = (/) 8760 0.7/ 0.8 103

3.3.6 ABSORBED DOSE RATE

The absorbed dose rates due to gamma radiation of naturally occurring radionuclide (238U, 232Th
40
and K) was calculated on guidelines provided by (UNSCEAR, 2003).The absorbed dose rate
(D) due to radiation in air at 1m above the soil surface for uniform distribution of activity
concentration of natural radionuclide was calculated directly using in-situ gamma ray
spectrometer from the following expression as shown in equation 3.10 (Veiga et al., 2006).
( ) = 0.491 + 0.621 + 0.0417 3.10
The maximum permissible dose rate is 51nGy/h (UNSCEAR 2000).
D = Absorbed dose rate in air measured in (nGyh-1)
A (K) = Activity Concentration of Potassium in Bqkg-1
A(U) = Activity Concentration of Uranium in Bqkg-1
A (Th) = Activity Concentration of Thorium Bqkg-1

3.4 CONVERSION OF RADIONUCLIDES FROM PERCENTAGE (K) AND PART PER

MILLION TO SPECIFIC ACTIVITY
In geology, soil science and nuclear geophysics, radioelement concentrations in soils and rocks,
air and water are expressed in the following units: mass concentration of K: %K (percent
potassium), mass concentration of U: ppm U (parts per million of uranium) etc.
The conversion of radioelement concentration to specific activity is shown in Table 3.1 (IAEA,
2003).
Table 3.1: Constant for Converting Radionuclide Concentration to Specific Activity
Radionuclide Concentration Activity Concentration (Bq/kg)
1%K 313Bq/kg 40K
1 ppm U 12.35 Bq/kg 238U
1ppm Th 4.06 Bq/kg 232Th

35
The theoretical gamma ray exposure rates and gamma dose rates 1 m above a plane and infinite
homogeneous soil medium per unit radioelement concentration assuming radioactive equilibrium in the
uranium and thorium decay series is shown in Table 3.2
Table 3.2 Exposure Rate and Dose Rate of Radioelement Concentration (IAEA, 1989)
Radioelement Concentration Exposure Rate Dose Rate
1%K 1.505 13.078
1 ppm U 0.653 5.675

1ppm Th 0.287 2.494

The bench marks for assessing radiological hazard indices recommended by (UNSCEAR, 2000).
is shown in Table 3.3 below:
Table 3.3: Bench Marks for Radiological Indices to Assess Radiation Hazard
S/N Radiological Indices Bench Marks References
1 Activity Conc. (Bq/kg)
40
K 140 - 850.0 UNSCEAR, 2000
226
Ra 17.0 60.0 UNSCEAR, 2000
232
Th 11.0 64.0 UNSCEAR, 2000
2 Dose Rate (nGy/h) 56 UNSCEAR,1993
3 Annual Effective Dose Equivalent 70 UNSCEAR,1993
(outdoor and indoor) (Sv/y)
4 Raeq (Bq/kg) 370 (max) Beretka & Mathew, 1995
5 Hex(Bq/kg) <1 UNSCEAR, 2000
6 Hin (Bq/kg) <1 UNSCEAR,2000
7 Equivalent Dose Rates (mSv/yr) 1.0 UNSCEAR,2000

Safety limit for assessing radiological hazard indices to the environment, human, plants and
microorganisms recommended by (UNSCEAR, 2000) are shown on the Table 3.4
Table 3.4: Recommended Safety Limit for Radiological Hazard Indices (UNSCEAR, 2000).

Radiological Hazard Indices Value

Annual Effective Dose Rate 0.07(Svy-1 )
Radium Equivalent Activity 370 (Bq/kg)
Absorbed Dose Rate 51- 55 (nGyh-1)
Equivalent Dose Rate 0.5 1.0 (mSv/y)

36
 CHAPTER FOUR

4.0 RESULT AND DISCURSION

4.1 RESULTS
The activity concentrations of the radionuclides in the study area is shown in Table 4.1, while
the plot for the frequency distribution of the mean activity concentration in (Bq/kg) against the
sampling point is presented in Figure 4.1.

The mean dose rates in air at 1m above the soil surface for uniform distribution of the
radionuclides including the absorbed and effective dose rate is presented in Table 4.2.
The plot to indicate their frequency distributions is shown in Figure 4.2 and Figure 4.3.

The annual effective dose equivalent received outdoor and indoor and radium equivalent activity
(Raeq) in (Bq/kg) are presented in Table 4.3 while their frequency distribution is shown in
Figure 4.

The internal and external hazard indices and the activity concentration index are displayed in
Table 4.4 while their distribution in air above the surface soil is shown in Figure 4.5.

4.2 DISCUSSION
4.2.1 Activity concentrations of Radionuclides in the Vegetable Farm
Table 4.1 shows the specific activity concentration of the radionuclides in the vegetable farm.
40
The activity concentration of K ranges from 73.56Bq/Kg to 126.76 Bq/kg and the mean
238
activity is 108.51Bq/kg. The activity concentration of U ranges from 5.18 Bq/kg to 15.52
232
Bq/kg with mean value of 11.10 Bq/kg, while the Th ranges from 9.14 Bq/kg to 9.87 Bq/kg
with mean value of 9.496 Bq/kg. The calculated values from the activity concentration of the
radionuclides fall between the standard values (140- 850) Bq/kg as shown in Table 3.3.

37
Table 4.1: Specific Activity concentration of Radionuclides in the study Area

TRAVERSE K %(Bq/kg) U (Bq/kg) Th (Bq/kg)

T1 73.56 12.66 9.14
T2 125.2 15.52 9.87
T3 126.76 5.13 9.38
T4 137.72 16.73 9.72
T5 89.21 15.19 10.63
T6 93.9 26.98 8.87
T7 121.76 13.26 9.32
T8 117.06 15.28 5.02
T9 120.19 14.82 10.15
T10 72.62 4.1 1.34
MEAN 108.50667 11.103333 9.433333
MAX 126.76 15.52 9.87
MIN 73.56 5.13 9.14
STDV 24.71923 4.382194 0.303791

This shows that the radionuclides in the vegetable farm soil in the study area is still within the
acceptable limit recommended by the regulatory body. Figure 4.1 shows the frequency
distribution of the radionuclides. The concentration of 40K is higher than that of 238
U and 232
Th
in the study area; this could be due to constant application of phosphate fertilizer on the surface
soil to improve the yield of vegetable crops in the farm.

160
Concentration (Bq/kg)

140
120
100
80 K %(Bq/kg)
60 U(Bq/kg)
40
Th (Bq/kg)
20
0
T1 T2 T3 T4 T5 T6 T7 T8 T9 T10

Sampling Point

Figure 4.1: Specific Activity Concentration of Radionuclide in the Study Area

38
 4.2.2 Absorbed and Equivalent Dose Rates of the Radionuclides
Table 4.2 shows the absorbed and equivalent dose rates received by the population around the area of
study. The absorbed dose ranges from 10.44(nGyh-1) to 12.24(nGyh-1) with an average value of
11.36(nGyh-1). The absorbed dose rate due to the soil concentrations is two times lower than the
worldwide average value of 56nGy/h (UNSCEAR, 2000). The value of equivalent dose, expresses the
biological effect of radiation to organ or tissue of the people living within or close to the study area
and those consuming the vegetables. It ranges from 0.09mSv to 0.11mSv with a mean value of
0.10mSv. It can be observed that the equivalent dose does not exceed the recommended value of
1mSv shown in Table 3.3. Therefore, the farm soil satisfies the safety criterion for general public and
the vegetables does not pose hazard to the consumers. Figure 4.2 shows the frequency distribution of
the effect of the equivalent dose in the study area. The contribution to the radiation exposure of the
population in the study area can be considered to be insignificant. Figure 4.3 depicts the lateral
frequency distribution of the equivalent dose rate, which shows that traverse 9 has the highest dose of
radionuclide concentration and there is a positive correlation for all the traverses in the study area.

Table 4.2 Absorbed Doses and Equivalent Dose Rate

TRAVERSE D (nGyh-1) E(mSv/yr)

T1 10.425 0.091
T2 11.43 0.1
T3 12.235 0.11
T4 12.463 0.11
T5 13.035 0.11
T6 11.455 0.1
T7 13.474 0.11
T8 13.121 0.11
T9 13.674 0.12
T10 13.267 0.12
MEAN 11.363333 0.1003333
MAX 12.235 0.11
MIN 10.425 0.091
STDV 0.740432 0.00776

39
 16
14
Concentration 12
10
8
6 D(nGyh-1)
4
2
0
T1 T2 T3 T4 T5 T6 T7 T8 T9 T10
Sampling point

Figure 4.2: Absorbed Dose Rate in the Study Area

0.14
0.12
Concentration

0.1
0.08
0.06
E(mSv/yr)
0.04
0.02
0
T1 T2 T3 T4 T5 T6 T7 T8 T9 T10
Sampling Point

Figure 4.3: Equivalent Dose Rate in the Study Area

The frequency distribution of the absorbed dose and equivalent dose illustrated in Figure 4.2 and
Figure 4.3 correspond with the concentration of 40K. The exposure to radiation from concentration
40
of K in vegetable plants has been found to be fairly constant. The results show that all
vegetables predominantly absorb 40 K more than 226 Ra and 228Th radionuclide. This is due to the
fact that potassium is an essential element and plants do not have the capability of
elemental isotopic differentiation thus 40 K is preferred to the other two radionuclides.

40
4.2.3 Annual Effective Dose Equivalent (Outdoor and Indoor) and Radium Activity.
Table 4.3 illustrates the values of the annual effective dose equivalent (outdoor and indoor) which
enable the level of radioactive element for health risk assessment in the study area. The estimate of
annual effective dose equivalent outdoor from natural radiation shows that radon the ground-daughter
of uranium (mainly in indoor air) ranges from 51.14 (Sv/yr) to 60.04 (Sv/yr) with a mean value of
51.14 (Sv/yr) which is lower than the world average. The annual effective dose equivalent outdoor
ranges from 12.79(Sv/yr) to 15.01 (Sv/yr) having an average of 12.79(Sv/yr). Measured mean
value of the annual effective dose of radionuclide concentrations was found to be less than the world
average values shown in Table 3.3. Radium equivalent activity is calculated based on the fact that the
226 232 40
distribution of Ra Th and K in soil is not uniform. Uniformity with respect to exposure to
radiation has been defined in terms of radium equivalent activity (Raeq) in Bq kg-1 to compare the
226 232 40
specific activity of materials containing different amounts of Ra, Th and K. The radium
equivalent activity in Table 4.3 ranges from 10.43Bq/Kg to 12.24Bq/Kg with mean value of
11.37Bq/Kg, which is less than the safety limit (370Bq/Kg).
Table 4.3 Annual Effective Dose Equivalents (Outdoor and Indoor) and Radium Activity.

TRAVERSE AEO(Sv/yr) AEI(Sv/yr) Raeq

T1 12.79 51.14 10.43
T2 14.02 56.07 11.43
T3 15.01 60.04 12.24
T4 15.32 61.14 12.49
T5 15.99 63.94 13.04
T6 14.04 56.19 11.45
T7 16.52 66.09 13.48
T8 16.77 64.37 13.06
T9 18.15 67.08 14.8
T10 16.27 65.08 13.18
MEAN 13.94 55.75 11.366667
MAX 15.01 60.04 12.24
MIN 12.79 51.14 10.43
STDV 0.908075 3.640449 0.740285

Figure 4.4 below depicts the plot of the frequency distribution of annual effective dose for
outdoor and indoor and radium equivalent activity.

41
 These show that the values for radium content in the farm soils of study area are generally low
as compared to the compared to the world standard

80
70
60
concentration

50
40 AEO(Sv/yr)
30 AEI(Sv/yr)
20
Raeq(Bq/kg)
10
0
T1 T2 T3 T4 T5 T6 T7 T8 T9 T10
Sampling Point

Figure 4.4: Annual Effective Dose Equivalent (Indoor and Outdoor) and Radium Equivalent

4.2.4 Internal and External Hazard Indices and Activity Concentration Index (ACI)
The internal and external hazard indices explain the presence of naturally occurring radioactive
material in the soil above threshold levels that may contaminate the environment and cause
health problems to humans and plants. Table 4.4 below shows the values of the radiological
hazard indices and the activity concentration index. The external and internal hazard index
ranges from 0.08 to 0.19 respectively. Since these values are lower than unity, therefore the soil
from these regions is safe and can be used for the cultivation of agricultural product without
posing any significant radiological threat to the consumers of these farm products.

42
Table 4.4: Hazard Index (Hex, Hin and Activity Concentration Indices in the Study Area
Traverse Hin Hex ACI
T1 0.12 0.09 0.22
T2 0.15 0.10 0.28
T3 0.09 0.08 0.21
T4 0.15 0.11 0.09
T5 0.07 0.07 0.11
T6 0.13 0.09 0.33
T7 0.13 0.09 0.26
T8 0.14 0.09 0.23
T9 0.09 0.09 0.28
T10 0.09 0.09 0.09
MEAN 0.12 0.089 0.2366667
MAX 0.15 0.1 0.28
MIN 0.19 0.08 0.21
STDV 0.008155 0.008165 0.030912

Figures 4.5 shows the frequency didtribution of internal and external hazard including the activity
concentration index which shows a significant trend of about 0.35 as a result of the emanation of gamma
ray in the study area. From radiological point of view, there is no significant radiological risk
because the radiological indices is lower compared to the one recommended by (UNSCEAR,
2003).

0.35
Mean concentration (Bq/kg)

0.3

0.25

0.2 Hex

0.15 Hin
ACI
0.1

0.05

0
T1 T2 T3 T4 Sampling
T5 T6
point T7 T8 T9 T10

Figure 4.5: Hazard Index (Hex, Hin) and Activity Concentration Indices in the Study Area

43
 CHAPTER FIVE
5.0 CONCLUSION AND RECOMMENDATION

5.1 CONCLUSION
The concentration of naturally occurring radionuclides (40K, 238
U, 232
Th) was measured in-situ
using portable handheld RS- 230 BGO Super Spec spectrometer, an auto stabilizing unit that
does not required any test sources. The field survey was conducted in static mode and
measurement was adopted in the study area under investigation. The assay modes of the
equipment display the %K, ppm of U and Th and absorbed dose rate in (nGyh-1).

The specific activity concentration (Bq.kg-1) in the study area ranges from 73.56 Bq/kg to
40
126.76Bq/kg with mean value of 108.51 Bq/kg for K, 5.18 Bq/kg to 15.52 Bq/kg with mean
238
value 11.10 Bq/kg for U and 9.14 Bq/kg to 9.87 Bq/kg with mean value of 9.496 Bq/kg for
232
Th. For the radiation hazard indices, the radium equivalent activity (Raeq) in the farm ranges
from10.43Bq/kg to 12.24Bq/kg and the mean value is 11.37Bq/Kg, which is less than the safe
limit 370Bq/Kg recommended by (UNSCEAR 2000).The calculated absorbed dose rate in the
vegetable farm ranges from 10.43 (nGyh-1) to 12.24(nGyh-1) with a mean value of 11.36 (nGyh-1).

The study shows that internal and external hazard index correspond to internal exposure to radon
gas in the environment ranges from (0.08- 0.1) Bq/Kg in internal and (0.09 0.15) external with
a mean value of 0.09Bq/kg and 0.12Bq/kg for internal and external respectively. From this value
it is shown that the radiation hazard is negligible which less than unity. The annual equivalent
dose rate in the study area ranges from 0.11mSv to 0.09mSv with a mean value of 0.1mSv which
is far less than the standard (1mSv/yr) indicated by radiological protection. The annual effective
dose rate indoor and outdoor ranges from (51.14 Svy-1 to 60.04Svy-1) for indoor with a mean
value of 55.75Svy-1 while the effective dose rate outdoor ranges from (12.79 Svy-1 to
15.01Svy-1) with a mean value of 13.94Svy-1. This value is lower than the world average
(0.07Svy-1), and could be due to constant disturbance of the surface soil by the farmers during
weeding and irrigation activities.

44
Also, this study reveals importance of using gamma ray spectrometry in an area where
calibration facilities are lacking and where cosmic background cannot be measured accurately,
empployed in-situ ground gamma ray spectrometry technique to determine the concentrations of
K, Th, and U of the area under investigation. The results so far indicate predominant contribution
of U and daughter nuclides in the gamma activity. The results would be useful for establishing a
database in the area under consideration and represent the basis to assess any future changes in
the radioactivity background levels due to various geological processes or any artificial
influences around the study area. The results further show that consumption of the studied plants
would impose no health consequences to the consumers.

5.2 RECOMMENDATION
It is recommended that regular monitoring should be conducted to take care of unforeseen
eventualities. The data and information generated from this study may be useful for establishing
a comprehensive framework to investigate other areas and develop guidelines for monitoring and
controlling NORMs (Natural Occurring Radioactive Material) in the environment as a whole in
Nigeria.

45
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50
 APPENDIX A
GROUND RADIOMETRIC DATA

51
TABLE A1: GPS LOCATIONS

Spacing(m) Latitude Longitude

0 60 27' 42.23"N 30 12' 27.50"E

5 60 27' 41.23"N 30 12' 27.50"E

10 60 27' 41.53"N 30 12' 27.60"E

15 60 27' 41.77"N 30 12' 27.60"E

20 60 27' 41.97"N 30 12' 27.51"E

25 60 27' 41.88"N 30 12' 27.68"E

30 60 27' 42.14"N 30 12' 27.64"E

35 60 27' 42.35"N 30 12' 27.68"E

40 60 27' 42.42"N 30 12' 27.62"E

50 60 27' 42.65"N 30 12' 27.62"E

55 60 27' 42.84"N 30 12' 27.62"E

60 60 27' 43.07"N 30 12' 27.72"E

65 60 27' 43.19"N 30 12' 27.72"E

70 60 27' 43.24"N 30 12' 27.75"E

75 60 27' 43.24"N 30 12' 27.79"E

80 60 27' 43.46"N 30 12' 27.91"E

85 60 27' 43.57"N 30 12' 27.95"E

90 60 27' 43.94"N 30 12' 27.99"E

95 60 27' 43.90"N 30 12' 28.01"E

100 60 27' 42.02"N 30 12' 28.16"E

52
Table A2: Activity Concentration of Radionuclides in Traverse One and Two

Table A3: Activity Concentration of Radionuclides in Traverse Three and Four

53
Table A4: Activity Concentration of Radionuclides in Traverse Five and Six

54
Table A5: Activity Concentration of Radionuclides in Traverse Seven and Eight
55
Table A6: Activity Concentration of Radionuclides in Traverse Nine and Ten

56
TABLE A7: Conversion of Specific Activity From (% and ppm) to (Bq/kg) (UNSCEAR 2000)

57
58
59