Evaluation of Natural Radioactivity and Hazard Indices in The Soil Collected From The Residential College Areas of University Malaya, Malaysia
Evaluation of Natural Radioactivity and Hazard Indices in The Soil Collected From The Residential College Areas of University Malaya, Malaysia
Evaluation of Natural Radioactivity and Hazard Indices in The Soil Collected From The Residential College Areas of University Malaya, Malaysia
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OKEREAFOR CASMIR NNEJI
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FACULTY OF SCIENCE
UNIVERSITY OF MALAYA
KUALA LUMPUR
2017
EVALUATION OF NATURAL RADIOACTIVITY AND
HAZARD INDICES IN THE SOIL COLLECTED FROM
THE RESIDENTIAL COLLEGE AREAS OF UNIVERSITY
MALAYA, MALAYSIA
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OKEREAFOR CASMIR NNEJI
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(MATERIALS SCIENCE)
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DEPARTMENT OF PHYSICS
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FACULTY OF SCIENCE
UNIVERSITY OF MALAYA
KUALA LUMPUR
2017
UNIVERSITY OF MALAYA
ORIGINAL LITERARY WORK DECLARATION
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Field of Study: Experimental Physics (Radiation)
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I do solemnly and sincerely declare that:
(1) I am the sole author/writer of this Work;
(2) This Work is original; M
(3) Any use of any work in which copyright exists was done by way of fair dealing and
for permitted purposes and any excerpt or extract from, or reference to or
reproduction of any copyright work has been disclosed expressly and sufficiently
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and the title of the Work and its authorship have been acknowledged in this Work;
(4) I do not have any actual knowledge nor do I ought reasonably to know that the
making of this work constitutes an infringement of any copyright work;
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(5) I hereby assign all and every rights in the copyright to this Work to the University of
Malaya (“UM”), who henceforth shall be owner of the copyright in this Work and
that any reproduction or use in any form or by any means whatsoever is prohibited
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without the written consent of UM having been first had and obtained;
(6) I am fully aware that if in the course of making this Work I have infringed any
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ABSTRACT
exposure. In connection with this, soil samples collected from all residential colleges of
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42.16 to 61.27 Bq/kg, 232-Th ranged from 52.89 to 81.80 Bq/kg and 40-K ranged from
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73.07 to 306.43 Bq/kg. Radium-226, Thorium-232 and Potassium-40 have average
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respectively. The results show that the average concentrations of the primordial
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radionuclides were lower than Malaysia average values. But 232-Th and 226-Ra are
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higher than the world average while 40-K is lower compared with values giving in
UNSCEAR 2000. The dose rate and radiological indices were obtained and compared
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ABSTRAK
(NORM) pada semua media bawakan bumi, adalah penting penilaian ketumpatan bahan
kesihatan penghuni. Berkaitan ini, sampel tanah dipungut dari semua kawasan asrama
sinar gamma HPGe. Ketumpatan aktiviti dari 42.16 ke 61.27 Bq/kg bagi 226-Ra, 52.89
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ke 81.80 Bq/kg bagi 232-Th dan 73.07 ke 306.43 Bq/kg bagi 40-K
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didapati. Ketumpatan aktiviti 52.31±2.40 Bq/kg, 68.42±1.92Bq/kg and
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pengukuran mendapati nilai ketumpatan purata radionuih rendahlid kuno adalah lebih
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rendah dari nilai purata. Negara Malaysia. Walaubagaimana pun nilai bagi 232-Th dan
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226-Ra adalah lebih tinggi dari purata dunia, manakala nilai bagi 40-K adalah lebih
rendah, berpandukan UNSCEAR 2000. Kadar dos dan indeks radiologi didapati dari
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ACKNOWLEDGEMENTS
My special thanks and appreciation goes to Prof. Dr. Mayeen Uddin Khandaker, my
ideal supervisor. His sage advice, insightful criticisms, and patient encouragement aided
me so much. I would also like to thank Prof Yusoff Bin Mohd Amin whose support of
this project was greatly needed and deeply appreciated.
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I would like to thank my mom and my brothers and sister for supporting me
spiritually throughout this study and my life in general
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I must acknowledge as well the many friends, colleagues, fellow students and
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teachers, especially Dr. Matthew Tikpangi Kolo, who assisted, advised, and supported
my research and writing efforts.
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TABLE OF CONTENTS
Abstract ............................................................................................................................iii
Abstrak ............................................................................................................................. iv
Acknowledgements ........................................................................................................... v
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CHAPTER 1: INTRODUCTION .................................................................................. 1
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1.1 Soil and Radionuclides ............................................................................................ 1
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1.3 NORM and TENORM ............................................................................................. 2
1.3.1
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Cosmogenic radionuclides and radiation.................................................... 3
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1.3.2 Primordial (Terrestrial) Radionuclides ....................................................... 5
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2.2 Radioactive half life ............................................................................................... 22
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2.5.4 Differences between Alpha, beta and gamma .......................................... 27
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2.5.5 Characteristics of alpha beta and gamma rays ......................................... 28
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2.7 Intensity ................................................................................................................. 29
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Interaction of gamma rays with matter .................................................................. 29
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3.4.1 Energy calibration .................................................................................... 41
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CHAPTER 4: MEASUREMENTS AND RESULTS ................................................. 50
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4.2 Activity concentration ........................................................................................... 51
4.3 M
Hazard indices ....................................................................................................... 52
4.3.6 External and Internal hazard indices (Hex and Hin) .................................. 57
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5.5 Annual gonadal dose equivalent ............................................................................ 75
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6.1 Limitation and suggestion for further studies ........................................................ 78
References ....................................................................................................................... 79
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LIST OF FIGURES
Figure 1.5 Routes of human exposure to sources of natural and man made ................... 15
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Figure 3.2 Detection efficiency curve of the detector ..................................................... 43
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Lumpur, Malaysia ........................................................................................................... 47
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Figure 3.4 Collection of samples at the sample sites ...................................................... 48
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Figure 3.5 Photos of samples preparation (oven drying, weighing and storage) ............ 49
Figure 4.1 Photo of P-type Coaxial ORTEC, GEM-25 high purity germanium
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Gamma ray detector with the MCA and gamma vision PC ............................................ 51
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LIST OF TABLES
Table 1.1 Average radiation dose from natural sources (UNSCEAR 2000) .................... 5
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Table 1.1 Neptunium decay series with half-life……………………………………….12
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Table 3.1 Energy calibration ........................................................................................... 42
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Table 3.2 Radionuclide, Energy and Detection efficiency ............................................. 43
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Table 3.3 Sampling sites coordinates. ............................................................................. 45
Table 4.1 Mean of activity concentration for 226Ra, 232Th and 40K in the soil
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Table 4.2 Mean of radium equivalent activity for 226Ra, 232Th and 40K in the
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Table 4.3 Mean of absorbed dose rate values in the soil samples from
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Table 4.4 Mean of annual effective dose equivalent (AEDE) values in the soil
Table 4.5 Mean of annual gonadal dose equivalent (AGDE) values in the soil
Table 4.6 Mean of activity utilization index (AUI) in the soil samples from
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Table 4.7 Mean of external and internal hazard indices values in the soil samples
Table 4.8 Mean of representative gamma index indices values in the soil samples
Table 4.9 Mean of excess lifetime cancer risk (ELCR) values in the soil samples
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the soil samples from residential college areas of University of Malaya ....................... 61
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CHAPTER 1: INTRODUCTION
Soil is typically a mixture of many substances like water, air, organic remains, clay,
particles of rock and inorganic materials. Organic remains are found as soil
components in a decay of living matters while the inorganic constituents exist in form
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materials either by natural means or human activities. Oxygen, silicon, aluminum,
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calcium and iron are the major uncontaminated components of soil (Manzoor et al.,
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2013) Soil serves as medium of transport for radionuclides through food chain which
depends on their chemical properties and the uptake process by the plants and animals.
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The radioactive elements in the soil provide large percentage of ionizing radiation from
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natural sources. And natural radiation is the largest contributor of external dose (80%)
to the world population which depends on the local geological characteristics and
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conditions of soils (UNSCEAR, 1993). The radioactivity in the soil is mainly from the
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238 235
naturally occurring radionuclides U (99.2745% of uranium), U (0.72% of
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232
uranium), Th (100% of thorium) and their decay products, and the primordial
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radionuclide 40K (0.0117 % of potassium) found in the earth crust (Rabesiranana et al.,
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2008). In the world average soil, potassium, uranium and thorium has mass fraction of
U
14%, ~2µg g-1 and 9µg g-1 (Bowen, 1993). According to Rohit et al., (2009) natural
radioactive materials can reach unsafe radiological level under certain levels.
1.2 Radioactivity
particularly uranium, emit radiations that are similar to x-ray in 1896 initiated scientific
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discovered that other elements such as thorium (Th), polonium (Po) and radium (Ra) are
also radioactive (Gasparini, 1984). Of all these elements, the primordial radionuclides
of Uranium (U), Thorium (Th) and isotope of potassium (K) are of significant
radiation emitted from these primordial radionuclides and their decay progeny is one the
radiation have been an indispensable component of the globe since its creation. And all
living things existing in the world are exposed to radiation. The nucleus found at the
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centre of an atom consists of protons and neutrons. These protons and neutrons are held
together by strong nuclear force but some nuclei still appear to be unstable. The
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unstable atomic nuclei undergo radioactive decay (spontaneous nuclear transformation)
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to form more stable nuclei thereby emitting energy in the form of particles and
Radionuclides are classified based on their origin. The radioisotopes that contribute to
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natural radiation are called Naturally Occurring Radioactive Materials (NORMs) while
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occurring radioactive material. NORMs are part of nature and it is found everywhere in
humans are continually exposed to it through food, soil, solar and water. Therefore,
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everything in nature has some amount of natural radioactivity. Natural radiation are
formed as a result of technology and human activities based on quest for economic
growth and development. Such activities includes oil and gas exploration, uranium and
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phosphate mining and milling, coal fired power plants, tobacco, air travel, metal ore
processing, manufacture of building materials and others, that could enhance and
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modify the concentration of NORMs, their environmental distribution and radiation
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exposure dose to human beings. Generally, some of the non-nuclear industrial processes
includes waste water treatment sludge, phosphate fertilizer and potash, phosphate
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industry waste, oil and gas production scale and sludge, paper and pulp industry, scrap
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metal release and recycling, coal ash, uranium overburden and mines spoils, geothermal
nuclear reaction when high energy cosmic radiation passes through the earth’s
atmosphere. The highly energetic cosmic ray particles collide with stable elements in
the atmosphere and in the ground. According to Alatise et al 2008, the entire geosphere,
the atmosphere and all parts of the earth that directly exchange materials with
atmosphere contains cosmogenic radionuclides with the major production being from
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the interaction of cosmic rays with atmospheric gases. These radionuclides are produced
through bombardment of the upper atmosphere by high energy heavy particles. The
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cosmogenic radionuclides comprise C, Na, 7Be and tritium. Only 14
C and tritium
internal exposure through inhalation. The exposure from these sources is relatively low
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and uniform over the surface of the planet (Benneth, 1997). C is present in carbon di-
oxide in the air, in the terrestrial biosphere, and in bicarbonates in the ocean. This
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particles/energy with N. The neutron spectrum covers a wide energy range in the
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Cosmic radiation
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Cosmic radiation refers to both the primary energetic particles of extra-terrestrial
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origin and to secondary particles generated by the interaction of primary particles with
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the atmosphere. Cosmic rays radiation consists of 85% protons, 14% alpha particles and
about 1% nuclei of atomic number between 4 and 26 (James, 1996). These particles are
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highly penetrating and have high energies. The annual external dose rates from cosmic
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rays depend slightly on latitude and strongly on altitude. Biehl et al., (1949) studied the
effects of geomagnetic latitudes on the total cosmic rays and found that the ratio of
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65:100. Annual effective dose from cosmic ray radiation around the world is estimated
between the ranges of 0.26 to 2.00 mSv/year. The table 1.1 below shows natural sources
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Table 1.1 Average radiation dose from natural sources (UNSCEAR 2000)
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1.3.2 Primordial (Terrestrial) Radionuclides
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Primordial radionuclides are the radionuclides found in the earth’s crust. They
4.5×109 years ago. Radiation from primordial sources constitutes about 85% of the
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(IAEA, 1996, Obed et al., 2005). About 70 out of 340 naturally occurring nuclides on
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the earth are radioactive therefore humans are continually exposed to radiation due to
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natural radioactivity in the terrestrial environment (Olomo, 2006). The specific activity
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lithological area and to the content of the rock from which the soils originated (Akhtar,
2004 and Tahir, 2005). These radionuclides when ingested or inhaled enter the human
body and are distributed among body organs according to the metabolism of the
element involved. The organs normally exhibit varying sensitivities to the radiation and
thus, varying doses and risks result from their consumption or inhalation.
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1.3.2.1 Radioactivity decay series
These are radionuclides that are headed by parent radionuclides that decay in
sequence to other radionuclides with different half live and decay modes, and finally
end to stable isotopes (NCRP,1992). There are four naturally occurring radioactive
decay series (Table 1.2). These include Thorium (232Th), Uranium (238U), Neptunium
(237Np) and Actinium (235U). These radionuclides do not decay to stable isotope in one
step, but give rise to decay series. And not all nuclides of the series emit gamma
radiations (Firestone, 1998). The members of natural radioactive series are genetically
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related by alpha decay (Ghoshal, 2005).
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Table 1.2 Natural radioactive decay series (Tait,1980)
207 235
Actinium 4n+3 Pb U 7.1x108
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Thorium-232 occurs naturally with atomic number 90 and has half life of 1.4×1010
years significantly longer than the age of the earth. It has a long decay series that
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beta emitter is a direct descendant of thorium-232, with half life of 5.75 years enters the
body mainly through food. The isotope of Radon-220 that appears in the decay series of
thorium has a half life time of 55.6 seconds which is too short for significant escape.
Thorium-232 undergoes ten steps, six alpha and four beta decay steps with possible 346
gamma ray emissions before becoming a stable isotope, 208Pb as shown in figure 1.1and
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radionuclide in biological material is almost negligible. This radionuclide also is not
mobile in the environment. The highest concentrations of thorium in the body have
found predominantly in the pulmonary lymph nodes and lungs. The presence of high
concentrations in this area of the body indicates that infiltration occurs mainly as a
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Figure 1.1 Thorium 232 decay series. (Nancy Walton (Modified 2016).
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228
Ra β 5.8 years
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Ac β 6.1 hours
U
228
Th α 1.9 years
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Ra α 3.7 days
220
Rn α 55.6 seconds
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Po α 0.15 seconds
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Pb β 10.6 hours
212
Bi 36% α and 64% β 60.5 minutes
212
Po α 3.0x10-7 seconds
208
TI β 3.1 minutes
208
Pb stable stable
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(b) Uranium (U) (4n+2) series
Uranium has atomic number of 92 and three naturally occurring isotopes namely;
234 235 238
U, U and U as show in table 1.4 in page 8 which already undergo radioactive
uranium isotopes are all radioactive and their decays produce a number of secondary
radioactive elements that continue to decay until they reach stable nuclei. Of the three
235 238
isotopes of uranium, U and U are the most important radionuclides of primary
origin in the earth’s crust. Uranium-238 has a half life of 4.47×109. 238
U (Uranium-
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radium) series takes about 14-16 steps to reach Pb, with possible 458 gamma rays as
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shown in figure 1.2 and table 1.5 in page 9. The decay products of U include
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important radionuclides such as radium-226, and radon-222. The release of radiation
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during the decay process raises health concerns. Humans could be exposed to uranium
Isotopes U U U
Natural Abundance (%) 99.27 0.72 0.0055
4.47×109 7×108 2.46×105
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Half-life (years)
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U
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Table 1.5 Uranium -238 decay series with half-life
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Polonium 214 Po 84 214 α 1.6x10-4 secs
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Lead 210 Pb 82 210 β 19 years
Bismuth 210 Bi 83 210 β 5 days
Polonium 210 Po 84 210 α 138 days
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Lead 206 Pb 82 206 - Stable
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(c) Actinium (4n+3) series
235
Actinium series is a daughter of Uranium-235. The decay of U (Uranium to
207
Actinium) series goes through 11- 14 radionuclides to Pb as shown in figure 1.3 and
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Thorium Th 90 231 β 25.5 hrs
Protactinium Pa 91 231 α 32,760 yrs
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Actinium Ac 89 227 α, β 21.7 yrs
Francium Fr 87 223 α,β 21.8 mins
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Thorium Th 90 227 α 18.7 days
Radium Ra 88 223 α 11.4 days
Radon Rn 86 219 α 4 secs
Astatine
Bismuth
At
Bi
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85
83
219
215
α, β
β
56 secs
7.7 mins
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Polonium Po 84 215 β 1.8 mins
Astatine At 85 215 α 0.1 min
Lead Pb 82 211 β 36.1 mins
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Neptunium has atomic number of 93. It is a radioactive series that was brought to
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light after the synthesis of trans uranium element. It takes 12 steps from Np to
U
bismuth 209 which is a stable nuclei as shown in figure 1.4 and table 1.7 in page 12.
The series contains some important radionuclides like uranium, thorium, actinium,
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Table 1.7 Neptunium decay series with half-life
Nucleon Mode of
Isotope Symbol Proton number Half life
number decay
Neptunium Np 237 93 α 2.14x10 years
Protactinium Pa 233 92 β 27 days
Uranium U 233 91 α 159200 years
Thorium Th 225 90 α 7304 years
Radium Ra 225 88 β 15 days
Actinium Ac 225 89 α 10 days
Francium Fr 221 87 α 5 minutes
Astatine At 217 85 α 32 seconds
Bismuth Bi 213 83 α, β 46 minutes
Polonium Po 213 84 α 4.2x10-6 minutes
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Thallium Ti 81 209 β 2.2 minutes
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Lead Pb 82 209 β 3.25 minutes
Bismuth Bi 83 209 stable 1.9x109 years
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1.3.2.2 Potassium-40 (40K)
most abundant element in the crust of the earth and the sixth most abundant element in
solutions in the oceans (Argonne National Laboratory, EVS 2005). It has a half-life of
1.3x109 years. It is a both beta and gamma emitter. The main decay modes of 40K are β-
40 40
decay to stable Ca and electron capture to an excited state of Ar, emitting 89% of
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40
1.314 MeV of β- particles most of the time (Kathren, 1998). Ar decays to its ground
sate by the emission of a gamma ray of 1.461 MeV which happens in 10.67% of all
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decays. This photon value makes it easy to identify and quantify potassium-40 by
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gamma ray spectroscopy. It is an excellent calibration point because of the presence of
which varies with time and location. The technological advancement and research in
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environment produces more radiation sources other than natural sources. The sources of
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man-made radiation includes; nuclear power plants (for energy production and nuclear
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weapons for warfare) and reprocessing facilities, radiation generating devices such as x-
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rays machine for medical diagnosis and therapy, nuclear accelerators for the study of
nuclear transmutations and sources used for industrial and agricultural applications
example is the major nuclear accident at Chernobyl-4 nuclear power installation in 1986
when huge amounts of various radionuclides escaped into the atmosphere (Olomo,
2006). Radiation used in medicine for both diagnostic and therapeutic purposes
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especially the management of cancer in humans make a significant contribution to
Man- made sources of radiation can only affect a small size of the population at any
time under controlled management. Some common consumer products enhanced man’s
exposure, like the luminous watches and clock which contains 3H, 147
Pm or 226
Ra as
activating agent (UNEP, 1991; NCRP, 1977). Television sets produce x-rays, but
modern television sets have designed to produce negligible amounts when used
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correctly and serviced appropriately (Larmash, 1983). Also, smoke detectors contain
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alpha emitting sources such as Americium-241. Some porcelain dentures and eyes
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glasses which contain uranium and thorium (NCRP, 1977), also enhanced exposure.
Starters for fluorescent tube lights and electrical appliances contain sealed radionuclides
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although they do not cause any hazard unless they are broken (NCRP, 1977), X-rays
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machines used for screening travellers (Mettler and Sinclair, 1990), cigarette smoke and
tobacco which contain Pb-210 and Po-210 (Larmash, 1983; NCRP, 1977, Paschal,
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2006) and combustible fuels as well as building materials which could be mixed with
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uranium, thorium and potassium containing waste etc (NCRP, 1977). All these radiation
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sources could contaminate the human body through irradiation, inhalation and ingestion
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The level of radiation dose to man can be increased due to the radionuclides in the
exposure is a direct exposure of man from the environment while internal exposure is an
dust, ingestion of dirt and dust, inhalation of radon diffusing from material and skin
contamination (see figure 1.5). Radioactive materials can be released into air or directly
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into water or soil. When they are released in air, they can travel some distance,
depending on some factors like wind speed and direction and altitude of the release. The
products of airborne releases can be transported to humans by several ways. Man can
directly inhale them or the materials will finally deposit themselves on the ground,
where they will find their ways into plant and animal life, as a result of that into the
food chain. Deposition of airborne contaminants into water can reach humans either by
direct ingestion or through the food chain. Likewise, depositions on the soil and water
find their way into the food chain through plant and animal life. Rain water runoff can
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carry soil into oceans, rivers, lakes and streams, thereby transporting any soil (sediment)
contamination to the water. Additionally, radioactive materials can leach into porous
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soils and into ground water (Doendara, 2007). Apart from all these ways, radionuclides
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in the aquatic environment could cause external exposure via the use of riverbed sand
Xiaolan, 2006).
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Figure 1.5 Routes of human exposure to sources of natural and man made
(www.google.com/search?q=Routes+of+human+exposure+to+sources+of+natural+and
+man+made).
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1.6 Biological effect of ionizing radiation
Ionizing radiation is a form of energy which transfers enough energy above the
threshold energy to cause ionization. The subsequent health effects when radiation
interacts with any biological entity are due to physical and chemical changes that came
as a result of ionization. The basic building blocks of human body are the cells that
form tissues and organs. Living tissues are very sensitive to change and the ionization
can alter to damage them. A unit cell in human body consists of nucleus, which is
surrounded by about 70% colourless fluid called cytoplasm that contains variety of
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compounds such as salts, fats, carbohydrates, amino acids and proteins. A cell is injured
when exposed to radiation which eventually interacts with other non-irradiated cells and
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thereby causing damage to the entire biological entity. The injury incurred as a result of
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exposure to ionizing radiation may lead to molecular changes and formation of
chemical species or radicals (H+ and OH_) which have deleterious effects on the
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chromosomes materials of the cells. The H+ and OH- attack Deoxyribonucleic acids
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(DNA) causing the breakage of the molecules and the rupturing of the molecular bonds.
The breakage of the DNA molecules ends up to the sudden random change in genetic
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code, and as a consequence causes genetic mutation. Such mutated cells may be
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repaired in a process called DNA degeneracy. Mutated cells that are not properly
repaired may die through apoptosis or survive as viable but transferred from a parent to
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organism) cells are complicated. The water content in the cell experiences ionization
and excitation within 10-16 seconds when radiation transfers energy to a biological
medium. The resulting ions interact with other water molecules and cause a number of
new products like H+ and OH- and strong oxidizing agent H2O2 ( hydrogen peroxide).
The nature and extent of damage caused by ionizing radiation depends on the amount of
exposure, the frequency of exposure, types of radiation, radio-sensitivity of the cell and
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the penetrating power of radiation to which an individual is exposed. Low doses of
radiation over a long time can cause various types of cancer, such as thyroid, breast,
lung cancer and leukemia. Shahid in 2012 reported the biological effect of ionizing
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Figure 1.6 Biological effects of ionizing radiation
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classified recently into two categories (stochastic and deterministic effects) based on
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presence and absence of a threshold radiation dose to produce the effect. When
effects, while the radiation effects occur without a threshold level is known as
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stochastic.
Stochastic effects include malignant and hereditary diseases for which the
proportional to the effective dose level. In stochastic effects, any radiation dose no
matter how small is capable of initiating an effect. Genetic mutations are examples that
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can result from stochastic effects. A gene mutation occurs when Deoxyribonucleic Acid
radiation and reported that radiation can cause alteration to the genetic information
contain in a germ cell. Genetic mutation caused by radiation exposure can be transferred
from a parent to an offspring. If the mutant gamete is successfully fertilized and the
zygote (fertilized ovum) developed into a life offspring, then the mutation is carried into
the progeny. Radiogenic cancer is a stochastic effect of ionizing radiation and the risk
of incurring cancer from radiation exposure depends on factors like; the dose
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administered over time, the age, sex and genetic background of the exposed person. In
recent times, cancer has assumed greater importance in the health agenda throughout
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the world and it has been observed that exposure to ionizing radiation increases the risk
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of incurring cancers (Farai et al., 2000, Brenner et al., 2003).
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1.7.2 Deterministic effects
consequences of exceeding a given threshold radiation dose. In other words, the severity
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effects are non-malignant skin damage (erythema), and hematological effects (changes
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in the composition of the blood). Somatic effect is deterministic and may be observed
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when an individual is irradiated. The damage due to somatic effect is only limited to the
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exposed individual, and in essence the individual suffers and die with the damage.
Somatic effects may take a longer time to develop and become evident after ionizing
radiation had been administered either acutely or over an extended period. This is
referred to as delayed somatic effect. Another delayed somatic effect is cataract which
affects the opacity of the lens of the eye. A radiogenic cataract is a deterministic effect
because there is practical threshold of ionizing radiation dose below which cataract is
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not produced or manifested; and its severity, when it occurs, is related to the magnitude
of the radiation dose and the time over which it is administered (Nobuyuki et al 2014).
All the habitat of the globe has presence of radioactive materials (radionuclides).
Therefore, the earth is a source of natural radiation. Natural radiation is mostly due to
232 and their daughters, in addition potassium-40 that is naturally present in the earth
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crust. Man has always been exposed to natural radiation emerging from within and
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outside the earth surface. It is a common knowledge that the irradiation due to ionizing
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radiations from natural sources happens because of the primordial radioactive elements
in the soil and rocks, cosmic rays gaining access into the earth’s atmosphere from outer
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space and the internal exposure from radioactive elements through food, water and air.
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Natural radioactivity is widespread in the earth’s environment and it exists in various
geological formations in soil, plants, rocks, water and air (Surinder et al., (2005).
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hostels environment to control the occupants’ health from radiation exposure. And have
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a baseline for future changes in the environmental radioactivity due to human activity.
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1.9 Aims and objectives
The aim of this research is to evaluate natural radioactivity and hazard indices in the
soil collected from the residential college areas of University of Malaya, Malaysia. The
232 228 40
1. To evaluate the activity concentrations of natural radionuclides U, Ra and K
in the surface soil samples collected from different areas of UM using High-purity
a
2. To calculate radiation levels and associated gamma-absorbed dose rates by members
ay
of the public
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3. To determine the areas in terms of radiological implication associated with studied
radionuclides.
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4. To evaluate the radiological threats on members of the public utilizing the
of
environment.
20
CHAPTER 2: LITERATURE REVIEW
All matter is made up of atoms and their effective diameters are about 3x10-10m
(Abraham 1986). Nearly all the mass of the atom is concentrated in the nucleus which is
centrally placed within the atom. The nucleus of an atom contains protons which carry a
positive electric charge and neutrons which carry no charge at all. They are held
a
together by a strong nuclear force. Each atom contains equal number of protons and
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electrons and is therefore electrically neutral. The number of electrons in the atom and
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hence the number of protons in the nucleus called the atomic number, Z gives an
M
element its unique properties. Since the protons and neutrons have almost the same
mass and are much heavier than electrons, most of all atom’s mass is concentrated in
of
the nucleus, thus the total number of protons added to neutrons is referred to as the mass
number, A of the particular atom. Thus, the mass number minus the proton number
ty
gives the neutron number, N; that is N = A-Z. Although many nuclides are stable, most
si
are not, the stability of nuclei is determined mainly by the neutron to proton ratio ( ) of
r
ve
a nuclide. For light nuclei, neutron to proton ratio, = 1 while for heavy nuclei, neutron
ni
to proton ratio, = 1.5. This is the ideal situation for stability of a nucleus.
U
Radioactivity is a natural and spontaneous process that occurs when unstable nuclei of
an element emit or radiate excess energy in the form of particles or waves. The particles
are called ionizing radiation because they have the ability to ionize or change the
physical and chemical structure of an atom they pass through. In some cases, one or
radiation in the form of alpha or beta particles and gamma rays. They undergo
21
spontaneous nuclear transformation which results in the formation of new elements.
cause ionization of molecules is the basis for health hazards and provides the means by
which radiation can be detected and evaluated. A radionuclide can be identified by the
characteristics of the radiation it emits. These characteristics include the rate of decay or
a
2.2 Radioactive half life
ay
The rate at which particles are disintegrated is expressed by the half-life of the
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radionuclide. The half-life, T1/2 is the period of time it takes for an unstable atom to
decay to half its initial value. The half-life is related to the decay constant by T1/2 =
M
. As a radionuclide decays, it becomes an isotope of an element, which can be
of
deduced as follows:
ty
∝N ( 2.1)
ni
for every radionuclide and minus sign because of the fact that number of radioactive
=- N (2.2)
(2.3)
22
Integrating both sides of the above equation,
(2.4)
Which gives;
) = - λ(t-to) (2.5)
where No is the number of radionuclides in a sample at some arbitrary initial time to.
a
Since to = 0, the equation above become
ay
(2.6)
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The above equation can be written as exponential form as:
t
N = Noe- (2.7)
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N is the quantity of radionuclides that remain after and has not yet decay after a time t.
ty
si
Since At = Nt (2.8)
t
A = Aoe- (2.9)
ni
U
where the activity A, of a radionuclide is the total number of decay per second; Ao is the
activity at a time t = 0.
2.3 Activity
One of the most important quantities associated with a sample of radioactive material
is its activity. Activity is the rate at which the nuclei within the sample undergo
23
seconds (dps). The Becquerel (Bq) is the S.I unit and is equivalent to 1dps. The
probability that a nucleus will decay in a certain time interval does not depend on the
age of the nucleus, the state of the chemical combination, temperature, pressure or the
presence of other atoms or nuclei but it is a property of the individual isolated nucleus.
The rate of radioactive decay from a sample of any radioactive substance must be
isolated nuclei.
a
2.4 Radioactive equilibrium
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Radioactive equilibrium or disequilibrium is an important consideration in all
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gamma ray spectrometric measurement. Gamma ray spectroscopy can be used to
determine the concentrations of uranium, thorium and potassium in the rock or soil
M
samples because gamma rays of specific energies are associated with each
of
radioelement. By looking at the peak in the energy spectrum of gamma rays being
emitted by the source, the radioelement content of the source can be inferred. The
ty
method involves the counting of gamma ray photons with specified energies. The
si
gamma ray count rate can then be related to the amount of parent by assuming there is a
r
direct relation between the amount of daughter and parent. The assumption is valid
ve
of each daughter being produced in a series is equal to the number of atoms the
daughter’(s) parent lost by radioactive decay. The rate of loss by decay is proportional
24
where N1 is the amount of element 1 (parent) and 1 is the decay constant for element 1
(parent)
a
(daughter)
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In a radioactive series N1 is decaying into N2 at the above rate while at the same time
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N2 will decay with decay constant 2 into N3 and so on. For a parent with a relatively
long half-life, after a long period of time, the amount of any given daughter becomes
M
constant. The rate of production from its parent becomes equal with its rate of decay.
of
The series is then said to be in the state of secular equilibrium and it requires that;
ty
si
When this condition is obtained, it is possible to determine the amount of the parent
r
of the decay series by measuring the radioactivity from any of the daughter elements. i.e
ve
activity of the parent is equal to the activity of the daughter. It is important to know the
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length of time required for a secular equilibrium to be established in a case of soil and
U
rock samples, which are crushed and sealed for laboratory analysis using gamma ray
spectrometry.
The instability of the atomic nucleus in certain atoms makes their nuclei to
25
bulk phenomenon, because the rate of emission does not depend on the state of
chemical composition of the radioactive element concerned. Also, it was found that
radioactive substances emits three (3) kinds of radiations; alpha particles (helium
nuclei), beta particles (electrons and positrons) and gamma radiations. These rays could
be distinguished from one another basically in two ways; the difference in the case with
which the rays could pass through matter and by the direction in which their path was
a
2.5.1 Alpha ( ) particles.
ay
These helium (He) nuclei of two protons and two neutrons and a charge of +2,
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which can be stopped in its path by a thin sheet of paper. Alpha particles exist as a
M
tightly bound entity within the nuclei and it is heavier than helium, which may be
where P, , X and Y are the number of protons, alpha particle, initial element and
si
particle is rather small and the mechanism for the energy loss by α particles passing
significant feature of α particle is its discrete energy and such energy is used to identify
These are electrons with a charge of -1. They are ejected when a neutron splits into a
26
P+N
PX → P+1YP+N-4+ e- (2.14)
The proton stays in the nucleus and the electron is ejected in certain radioactive
disintegration. The result of transmutation is that there will be a gain in charge +1 with
no change in mass. The penetrating power of β particle is about 100 times that of α
a
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2.5.3 Gamma ( ) radiation
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These are not discrete particles but pure electromagnetic radiation of the same kind
like x-rays, light and radio waves but of shorter wavelength. The gamma-ray photons
M
are of high energy. They have much more penetrating power compared with beta-
of
particles. Sizeable thick lead (Pb) is required to stop gamma rays. Their emission does
not affect the charge and mass of the nucleus but only a decrease in its energy content.
ty
Alpha and beta particles lose their energy in passing through matter collision,
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ionization etc. they are brought to a virtual stop within certain distance, which is called
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their range. The range of alpha particle is only a few centimeters or about 30µm in
denser particles, while a thin sheet of lead or a few centimeters of sand will stop beta
particles. The intensity of gamma rays traversing matter decreases exponentially with
27
2.5.5 Characteristics of alpha beta and gamma rays
a
Uranium -
Changes from Radium - Polonium unchange
Plutonium
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Charge (C) 2 -1 0
Mass (kg) 4 5.41x10-4 0
9
Speed (km/s) 15000 3x10 300,000
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% of speed of
5% Approx. 100% 100
light
-3
Kinetic energy 5.0x10 MeV – 1
5 0.1 MeV - < 10MeV
(MeV)
Low- has
large mass and
M MeV
neutron-induced fission which occurs in reactors, but the difference is that at the starting
U
point of this fission process, neutron is not important. Heavy nucleus undergo through
this kind of radioactive decay by splitting into two lighter nuclei releasing many
(2.15)
The determination of spontaneous fission products is not consistent like alpha and
28
2.7 Intensity
Radiation intensity is the amount of energy that goes through a known area which is
at right angle to the direction of radiation travel at a given time unit. The strength of
radioactive sources is not easy to be measured using its activity. The detector makes it
easier and convenient to measure the intensity of gamma ray or X-ray sources. The
intensity of a source is measured by sampling the number of photons emitted from the
source at a given time, which is directly related to the number of disintegrations at the
a
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2.8 Interaction of gamma rays with matter
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The earth contains many radionuclides that decay and emit charged particles such as
alpha, beta radiations and neutral particle like gamma radiations. To calculate the
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radioactivity in the soil, we need to focus on detecting the emissions of charged and
of
neutral particles from the decaying radionuclides. The emitted particles are easily
observed when they interact with the matter through the excitation and ionization
ty
effects they cause in the matter. The methods in which these effects are used for
si
radiation detection depend on the mode of interaction, type and energy of radiation.
r
lose their energies in matter since the main objective in radiation spectrometry is to
U
measure the energy distribution of the incident radiation. Gamma ray photon is
uncharged and creates no direct ionization or excitation of the material they pass
through. Therefore, the detection of gamma ray hang on causing the gamma-ray photon
to undergo an interaction that transfer all or part of the photon energy (hv) to electron in
29
Absorption of gamma rays in matter occurs by mechanisms that are completely
different from the absorption of charged particles. There are many modes of interaction
but only three mechanisms (Photoelectric effect, Compton scattering and pair
The experience of ejecting electrons from an atom after the absorption of light
photon is called photoelectric effect. Here, the incident gamma rays interact (collide)
a
with atomic electron in the absorber matter and transfer all of its energy to the electron.
ay
The atom gets ionized if the absorbed energy is enough to release the electron from its
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atomic shell. The kinetic energy of the emerging electron equals to the total energy of
where K.Ee , E , and EB are kinetic energy of the photoelectron, energy of incident
ty
equal to the binding energy of the electron (EB) in the material. The tightly bound shells
like K- shell always have vacancy due to the photoelectrons production. The immediate
ni
filling of the vacancy by electrons from the higher shells leads to the production of X-
U
ray characteristics. As stated by Tait (1980) and James (1995), Photoelectric effect has a
where, , ρ and Z are the constant, density of the absorbing material and the atomic
30
At lower frequencies, light is incapable of ejecting electrons, thus the critical
frequency for light to eject an electron is called the threshold frequency. It is evident
from equation (2.16) above that photoelectric effect is more for materials at low photon
energies (<0.1 MeV) and photons are absorbed more strongly in high atomic number
(Z) materials. i.e, the absorption due to the photoelectric effect decreases sharply with
increasing gamma ray energy but increases rapidly with increasing absorbing material’s
atomic number. Example, lead (Pb) used in gamma ray spectroscopy shields the
a
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2.8.2 Compton effect
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The interaction takes place between the incident gamma ray photon with energy (0.1-
10 MeV) and an electron in the absorbing materials. Here, the photon undergoes elastic
M
scattering with a free or loosely bound electron in the outmost atomic shell. After
of
transferring some portions of its energy to the electron, the energy of the photon reduces
from hv to hv’ with also a change in frequency and wavelength (λ to λ’). Some part of
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the original photon remains as lower energy which may undergo a further photoelectric
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or Compton interaction but in a different direction from the parent photon. The energy
r
of the electron scattered at different angle is written as hv-hv’. The energy hv-hv’ that is
ve
deposited in the material in the interaction can be calculated by applying the law of
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where ∆ λ, λ’, λ, , h and are the change in wavelength, wavelength of the scattered
photon, wavelength of the incident photo, the initial mass of the electron, the plank’s
31
The energy of the scattered gamma ray, E’ γ in terms of the scattering angle ϴ is
given by;
E’ γ = (2.19)
K.Ee = E γ - E’ γ (2.20)
a
Thus,
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K.Ee = (2.21)
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where m0 is the initial mass and m0c2 is the initial energy of the electron. Taking from
of
equation 2.6, the minimum value of K.Ee is zero when = 0. And the maximum value
Ec = [ (2.22)
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U
Note, the probability of Compton scattering per atom of the absorber depends on the
number of electrons available as scattering agent, and therefore increases linearly with
atomic number (Z) and decreases with increasing energy. Thus, Compton scattering
32
2.8.3 Pair production
rays. The process occurs in the field of a nucleus of the absorbing material. Because the
a
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positron will be subsequently annihilated after slowing down in the absorbing medium,
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interaction.
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Unlike the other two photon interactions, pair production has a cross section σpp
of
which increases, although slowly with photon Eᵧ and the interaction tends to be
c = constant.
ni
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The net effect of the above three interactions is an exponential attenuation in the
I = Io (2.25)
where Io is the initial intensity at t = 0 and σ is the linear absorption co-efficient due to
33
2.9 Review of existing knowledge
The existence of natural radioactivity in the soil and rock has long been recognized.
It has been found that uranium-238, thorium 232 and potassium are present in the earth
crust in parts per million (ppm) levels. There has been rapid increase in human
population. Human activities can increase the natural radioactivity of the surface soil
through waste dumping that contain radioactive material and opening of the earth crust
2000), mining of all kinds affect the environment adversely, this made mining one of
a
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the major sources that enhance the natural radioactivity level of the environment.
Gamma radiation emitted from primordial radionuclides and their progeny is one of the
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main external sources of radiation exposure to the human. Terrestrial radioactivity, and
M
associated external exposure due to gamma radiation depend primarily on the
geological formation and soil type of the location; and these factors greatly influence
of
the dose distribution from natural radiation.
ty
Since natural radiation is the largest contributor of external dose to the world
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232 226 40
importance. The concentration of Th, Ra and K vary widely depending on the
ve
location. In addition, soil acts as a source of transfers of radionuclides through the food
ni
chain depending on their chemical properties and the uptake process by the roots to
U
plants and animals; hence it is the basic indicator of radiological status of the
determine their mobility and availability for biological uptake. The major potential
hazard from natural radiation is from external exposure either by direct exposure to the
soil or as they enter in many building materials. [UNSCEAR, 1993; Beir VII, 2006;
UNSCEAR, 2000; Klein, C.K and Hurlbut, C.S., 1985; Jabbar, A., et al., 2010; Mandic,
34
Nowadays, studies on health effects due to ionizing radiations have produced
substantial evidences that exposures to high level of radiation can cause illness or even
death. Despite a well known effect of cancer, scientists have long known that ionizing
radiations with high doses may cause mental retardations in children’s mother exposed
to radiations during pregnancy period. Radium and its ultimate parent uranium in the
ground lead to the production of radon a radioactive gas. The inhalation of radon
progenies at a high level may cause an increase of lung cancer (UNSCEAR, 1993).
a
In an earlier work done by Ravisankar et al 2012, on activity concentration of natural
ay
radionuclides that are in different locations of Yelagiri hills shows that thorium-232 is
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1.19 times higher than world median value. And the spatial distribution and lifetime
cancer risk due to gamma radioactivity in the same Yelagiri hills in India by
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Chandrasekaran A., et al 2014 reported Th/U concentration to be 5.074 and U/Th ratio
of
0.43 which are higher that the global ratio of 3.5 and 0.26 respectively. In their further
work on natural gamma radiation in beach sediments of north east coast of Tamilandu,
ty
India 2014, they reported that average concentration of natural radionuclides, all
si
calculated radiological parameters and hazard indices except external hazard index are
r
higher than the recommended level. Therefore the sediments of this beach pose
ve
Nisar et al 2015, one of the major health problems in Malaysia is cancer (Stomach,
breast, lungs, liver, leukaemia and thyroid). Medically, it been certified that the fourth
leading cause of death is cancer. Taking from the progress and development that has
been achieved in Malaysia, cancer has become a very serious health concern. The result
of a study done in 1994 in Penang, Malaysia showed that the age standardized incidence
rate was 119.3 per 100,000 for all types of cancers. From 2004-2008, about 9692 cases
35
were identified in Penang, Malaysia. Sequel to the above, a study was carried out by
Almayahi et al in 2012 and reported in his conclusion that high concentration of natural
radioactivity and 226Ra/238U disequilibrium are the main cause of cancer in Penang
every environment and monitor the radiation hazards that may appear to the inhabitants
due to the use of soil; which happen to be the aim of the present study.
a
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of
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36
CHAPTER 3: MATERIALS AND METHODS
with matter which produces ionization and electronic excitation. The radiation either
gives off some or all its energy to the medium of the detector by either ionizing it
directly or causing emission of charged particles which later produces ionization of the
medium.
a
ay
Ionizing radiation can be measured through the physical and chemical effects of its
al
interaction with matter. Field and laboratory methods are based mainly on the ionizing
properties of radiation and the use of instruments that convert the radiation to electrical
M
signals. Ionization chambers, proportional counters, Geiger-Muller tubes, scintillation
of
counters, semiconductor detectors (for instance HPGe), thermoluminescence detector
and various mechanical and chemical track detectors are used to monitor and quantify
ty
specific energy photons (gamma rays), in environment and geological samples thereby
ni
energy of an incoming gamma ray and the pulse amplitude at the output of the detector.
The interaction between the gamma rays from the sample and the detector atoms are
amplified and converted into a voltage pulse proportional to the photon energy. Then,
the pulse amplitudes are analysed, and the output of the spectrometer is an energy
37
energies, the spectrum can be used to identify and quantify specific radionuclide that
system, data readout capability and shield sample enclosure. The pulse height analyser
consists of a linear amplifier, an analog to digital converter (ADC), memory storage and
logic control mechanism which allows the storage of data in various modes and displays
or recall. The amplitude gain stabilization in gamma ray spectrometers helps to the
a
effect of energy spectrum drift
ay
Main Multi-channel
Detector Preamplifier
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amplifier analyzer
M
High voltage
Display
of
supply
unit
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the properties of theoretical true intrinsic semiconductor material and < 10 10 atoms/cm3
with 1000 volts of reserve bias. The germanium detector diode has the ability to endure
38
The detector used in this experiment is a P-type Coaxial ORTEC, GEM-25 high
purity germanium gamma ray detector which has 57.5mm crystal diameter and 51.5mm
thickness, shielded with a cylindrical shaped lead which helps to minimize background
radiation intrusion with the measured spectrum. The operating voltage of this detector is
set at +2800V. The HPGe detector is cooled with Ortec X-Cooler II. The detector
element absorbs the energy from incident gamma ray and produces a current pulse
these types of detector present a more uniform, efficient cross-section of the active
a
ay
detector volume to the samples that are counted at a short distance from the detector.
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3.2.2 Preamplifier
The preamplifier is the first element in a signal- processing chain. It converts the
M
ionization charge developed in the detector during each absorbed nuclear event to a step
of
function output pulse whose amplitude is proportional to the total charge accumulated
in that particular event. The preamplifier is located very close to detector to achieve
ty
good performance. This will reduce the attenuation of the output signal in a way that
si
maximizes the electronic signal to the noise ratio, hence amplifying the signal before
r
The primary function of the amplifier is shaping of the pulse from the preamplifier.
U
The amplifier enlarges the amplitude of the pulse coming from the preamplifier into
adequate amplitude that can be easily and accurately measured. It shapes and filters the
pulse to improve the signal–to noise ratio. It also prevents overlapping. The amplifier
must be non-overloading, which means that it must amplify equally well at high count
39
3.2.4 Multi-channel analyser (MCA)
The multi channel analyser does a great job in this experiment. It performs the
function of pulse height analysis. The operation of multi channel analyser is basically
on the principle of converting analog to digital. The analogy to digital converter (ADC)
in MCA measures and sorts out the incoming pulses according to their amplitudes
(Paschal, 2006). The output is then stored in the computer-type memory, which has
many addressable locations and the number of channels into which recorded spectrum
can be divided. The channels storage is done in counts per seconds. The output
a
ay
information is either displayed as data to be analysed or final result form in real time.
al
3.3 Detector resolution
given by the sharpness of the photo peak. The energy resolution (R) is defined as full
ty
width of the photopeak at half maximum amplitude (FWHM) divided by its energy (E)
si
expressed as a percentage.
ve
i.e
ni
U
(3.1)
The resolution of the detector used in this study was 28.2% and 1.67keV FWHM
energy resolution at 1.33 MeV (60Co). This an excellent resolution to distinguish the
40
3.4 Calibration of the detector
The calibration of the detector is a very important aspect of gamma ray spectroscopy
for radioactivity measurements. This is to ensure that the gamma ray spectra are
for the measurement of gamma emitters is the exact identity of photopeaks present in a
spectrum produced by the detector system. The procedure for identifying the
radionuclides within a spectrum relies upon methods which match the energies of the
a
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3.4.1 Energy calibration
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The energy calibration was done so to establish a relationship between peak position
in the spectrum and the corresponding gamma ray energy. The height of each pulse
M
output from a photomultiplier tube and hence the channel corresponding to it is directly
of
proportional to the initial gamma energy producing the pulse. The calibration process
involved different gamma emitter sources of known energies, these includes Cobalt-60
ty
Tin-113 (391.698keV). The gamma emitter sources were exposed to the HPGe detector
ni
and gamma spectra were obtained under suitable counting time. The gamma source and
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41
Table 3.1 Energy calibration
a
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3.4.2 Efficiency calibration
al
In gamma ray spectrometry, the peak in the spectrum is related to the amount of
radioactivity it represents. This requires the absolute full-energy peak efficiency. This
M
gives a relationship between the peak area and the number of gamma rays emitted by
of
the source. The efficiency was determined by using Ra-226 source only with energy
range 186.211 to 1764.491 keV. It was ensured that the calibration standard reference
ty
sample represented the soil samples to be counted. The counting was done for 1 hour to
si
determine the detector efficiency. The detection efficiency was determined for each of
r
the gamma energies under investigation in this study and their values are tabulated in
ve
table 3.2. The dependence of the detection efficiency on the gamma ray energy is shown
ni
42
Table 3.2 Radionuclide, Energy and Detection efficiency
a
Ac228 968.97 0.0095398
ay
TI-208 583.18 0.0127546
al
0.035
M
of
0.03
0.025 y = 0.4872x-0.572
ty
0.02
Efficiency (cps/Bq)
si
0.015
r
0.01
ve
0.005
0
ni
operating capacity without the influence of any sample. The detectable limit is
43
concentration in a sample at 95% confidence level, using equation 3.1 (Khandaker et al,
2012)
(3.2)
where Kα, NB, M, η (E) and Pγ are the statistical coverage factor equivalent to 1.645, the
background count (cps), the sample mass (kg), the photo-peak efficiency, the
a
ay
With the measurement system used in this study, the minimum detectable activity
(MDA) for the targeted radionuclides was calculated to be 0.60Bq/kg, 0.70Bq/kg and
al
2.40Bq/kg for Radium-226, Thorium-232, and potassium-40 respectively. Any activity
M
concentration values below these numbers are taken in this study as below detection
Background radiation are the radiations that arise due to the presence of natural
si
present in the building materials used in building the laboratory, electronic noise and
ve
other sources.
ni
In this work, the environmental background was reduced with the help of the
U
cylindrical shaped lead that shielded the detector. The background radiation was
and research centres which covers the whole spectrum of learning from Arts, Science,
Humanities, Engineering and Medicine. The university dates back 1957 and the first
44
choice of Malaysia’s top students with international students population from more than
80 different countries. University of Malaya is seized 750 acre (309 hectare) with 12
residential colleges and strategically located (N3 7’15’’E101 39’23’’) within the heart
of Kuala Lumpur which makes it attractive and advantageous for her international
a
Thirty six (36) soil samples were randomly collected from the twelve (12) residential
ay
college areas (samples from three sampling sites of each college) of University of
al
Malaya, Malaysia, at a depth of 0-5 cm using hand auger as shown in figure 3.4 in page
48. The sampling sites (hostel, car park and recreational areas) were chosen due to
M
dense human activities in the areas The soil sample from each sampling site were
of
thoroughly mixed together to provide a representative sample for the site. Thereafter,
about 1kg of the composite sample were packed in a polythene bag and labeled with a
ty
sample identity using a coding that reflects both the area name, college and sample
si
matrix. Then the collected soil samples were taken to the laboratory for preparation and
r
sampling site in a college was about 200-300 metres. The map showing the locations
ni
where the soil samples were collected across University of Malaya (UM) is shown in
U
figure 3.3. The location of each sampling point was taken by means of a Global
45
“ C1R N03 07’ 03’’ E 101 39’ 35’’
a
5 C5C N03 07’ 37’’ E 101 39’ 29’’
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“ C5H N03 07’ 40’’ E 101 39’ 30’’
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6 C6C N03 06’ 55’ E 101 39’ 18’’
7
C6R
C7C
M
N03 06’ 53’ E 101 39’ 20’’
46
a
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Figure 3.3 Location of University Malaya (N3 7’15’’E101 39’23’’) Kuala Lumpur,
Malaysia
47
a
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Figure 3.4 Collection of samples at the sample sites
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3.7 Sample preparation
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In order to remove excess moisture, the soil samples were air dried in the laboratory
si
at room temperature for 24 hours. They were further dried in the oven at 45-600 degree
Celsius. The dried soil samples were pulverized to fine powder and sieved with a 1mm
r
ve
mesh sieve to achieve homogeneity. Then 500g of the homogenized soil sample were
labeled and kept for a period of four (4) weeks to achieve secular radioactive
U
equilibrium between short lived members of radium and thorium series as shown in
48
a
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Figure 3.5 Photos of samples preparation (oven drying, weighing and storage)
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49
CHAPTER 4: MEASUREMENTS AND RESULTS
high purity germanium gamma ray detector connected to an ADCM data acquisition
system, coupled with PCAII multichannel analyser and gamma vision computer system
was used for analysis in this study. The detector has a good resolution of about 28.2% at
energy of 1.33 MeV. This is sufficient enough to distinguish the gamma energies of
a
ay
interest in this study.
al
Each of the samples were placed in the detector and measured for a period of 86400
214
seconds (24hrs). Then, the activity concentration of daughter radionuclides Pb
M
(determined from its 295.22 keV and 351.93 keV gamma ray peak) and 214
Bi
of
(determined from its 609.32keV and 1120.29 keV gamma ray peak) were used to
226 228
calculate the Ra in the soil sample. While Ac (determined from its 338.32keV,
ty
208
911.20keV and 968.97keV gamma ray peak) and TI (determined from its 583.18keV
si
232 40
gamma ray peak) were taken as indicators of Th, K was determined by measuring
r
40
the 1460.82keV gamma rays emitted during the decay of K. The photo of P-type
ve
Coaxial ORTEC, GEM-25 high purity germanium gamma ray detector is shown in
ni
figure 4.1.
U
50
a
ay
al
M
Figure 4.1 Photo of P-type Coaxial ORTEC, GEM-25 high purity germanium gamma
of
ray detector with the MCA and gamma vision PC
ty
The radioactive source is described by its activity, which is the number of nuclear
r
Ac (Bq/kg) = (4.1)
U
where Ac (Bq/kg), CPS, εγ, Iγ and W are specific activity, net counts per second for
peak, the corresponding gamma-ray intensity and the mass of sample in gram
respectively.
51
226 232 40
The mean activity concentration for Ra, Th and K in the soil samples from
a
C6 50.38±1.89 69.58±1.48 212.55±1.32
ay
C7 43.41±2.15 65.45±1.70 303.82±1.21
C8 57.7±2.24 78.16±1.48 270.09±1.42
C9 53.5±2.81 81.8±1.93 294.55±1.59
al
C10 54.09±2.67 52.89±2.58 262.41±1.76
C11 42.73±2.65 57.13±2.03 270.18±1.24
C12
Mean
60.15±2.05
52.31±2.40
M 79.4±1.75
68.42±1.92
73.07±4.91
224.58±2.28
of
Note: Total mean is the value of the average of the concentrations of particular
ty
226 232 40
In order to represent the activity concentrations of Ra, Th and K by a single
quantity, radiation hazards associated with them must be taken into consideration,
ni
which includes radium equivalent activity (Raeq), Absorbed dose rate (DR), Annual
U
effective dose equivalent (AEDE), Annual gonadal dose equivalent (AGDE), Activity
utilization index (AUI), External and Internal hazard indices (Hex and Hin),
According to Agbalagba and Onoja 2011; Dabayneh et al. 2008, radium equivalent
232 226
activity (Raeq) it has been assumed that 259 Bq/kg of Th or 370 Bq/kg of Ra or
52
40
4810 Bq/kg of K produces the same gamma-ray dose. Radium equivalent index is
where Raeq is the radium equivalent activity and CRa, CTh and CK are the measured
a
ay
226 232 40
The radium equivalent activity for Ra, Th and K in the soil samples from
al
Table 4.2 Mean of radium equivalent activity for 226Ra, 232Th and
M 40
K in the soil
samples from residential college areas of University of Malaya.
of
College Raeq (Bq/kg)
C1 160.95
C2 187.31
ty
C3 131.28
C4 187.4
si
C5 157.93
C6 166.25
r
C7 160.4
ve
C8 190.27
C9 193.15
C10 149.93
ni
C11 145.23
C12 179.32
U
of the radionuclides present in the soil sample but do not represent the effect of such
dose rate should be calculated. The absorbed dose rates (DR) of gamma radiations in air
53
226 232 40
at 1 m above the ground due to the concentrations of Ra, Th and K was
DR is the absorbed dose and CRa, CTh and CK are the measured specific activity
The absorbed dose rate is measured in nanogray per hour and the calculated values
a
are presented in table 4.3.
ay
Table 4.3 Mean of absorbed dose rate values in the soil samples from residential
college areas of University of Malaya.
al
College DR (nGy/h)
C1
C2
C3
M 72.96
83.2
58.33
of
C4 83.48
C5 70.22
C6 74.17
C7 72.26
ty
C8 85.13
C9 86.41
si
C10 67.88
C11 65.51
r
C12 78.79
ve
exposure to radiation, gray is converted to Sievert with 0.7 SvGy-1 used as conversation
factor for the biological effectiveness of the dose causing damage in human tissue and
the occupancy factor of 0.2 that specifies the proportion of the total time spent outdoors
indoor. The annual effective dose equivalent (AEDE) in outdoor air is measured in
54
millisievert per year (mSvy-1) and the formula for its calculation as stated by
. (4.4)
The calculated values of Annual effective dose equivalent (AEDE) is show in table
4.4
Table 4.4 Mean of annual effective dose equivalent (AEDE) values in the soil samples
from residential college areas of University of Malaya.
a
College AEDE (mSvy-1)
ay
C1 0.09
C2 0.1
C3 0.07
al
C4 0.1
C5 0.08
C6
C7
M 0.09
0.09
C8 0.1
of
C9 0.1
C10 0.08
C11 0.08
ty
C12 0.1
Total Mean 0.09
r si
In Ravisankar et al., 2014, annual gonadal dose equivalent (AGDE) is seen as the
ni
reproductive organs (gonads). Moreover, active bone marrow and bone surface cells
Using the formula stated by (Chandrasekaran et al., 2014; Ravisankar et al., 2014),
232 226
annual gonadal dose equivalent (AGDE), due to the specific activities of Th, Ra
55
Where AGDE is the annual gonadal dose equivalent and CRa, CTh and CK are the
226 232 40
measured specific activity concentration of Ra, Th, and K respectively. The
annual gonadal dose equivalent measured in microsievert per year (μSvy-1) and its mean
Table 4.5 Mean of annual gonadal dose equivalent (AGDE) values in the soil samples
from residential college areas of University of Malaya.
a
C2 573.78
C3 402.47
ay
C4 577.96
C5 484.15
C6 513.26
al
C7 503.12
C8 589.81
C9
C10
M 599.73
470.62
C11 455.68
of
C12 540.7
Total Mean 518.18
ty
si
The activity utilization index (AUI) is the dose rates in air from different
r
ve
combination of 226Ra, 232Th and 40K (natural radionuclides) in soil samples. The formula
AUI = [ ] + [ ] + [ ] (4.6)
226 232
where CRa, CTh and CK are the measured specific activity concentration of Ra, Th,
40
and K respectively and fTh (0.604), fK (0.041) and fU (0.462) are the individual
fractional contributions to the total gamma radiation dose rate from the actual
56
OECD(1979) recorded that Typical activities per unit mass of primordial radionuclides
in soils are 50 Bq/kg for 232Th , 50 Bq/kg for 226Ra and 500 Bq/kg for 40K.
The calculated mean value of activity utilization index (AUI) in the soil samples
Table 4.6 Mean of activity utilization index (AUI) in the soil samples from residential
college areas of University of Malaya.
College AUI
a
C1 1.23
C2 1.53
ay
C3 1.07
C4 1.49
C5 1.29
al
C6 1.32
C7 1.22
C8
C9
M 1.5
1.51
C10 1.16
of
C11 1.11
C12 1.52
Total Mean 1.33
ty
si
estimate the radiological hazard caused by external exposure to gamma radiation from
ni
the soil samples. As stated by UNSCEAR (2000), external hazard index (Hex) can be
U
Hex = (4.7)
Furthermore, radiations from radon and its short-lived daughter radionuclides present
57
Hin = (4.8)
226 232
where CRa, CTh and CK are the measured specific activity concentration of Ra, Th,
40
and K respectively. The radiation hazard is considered insignificant when the
calculated values of Hex and Hin are less than unity. Table 4.7 shows the Hex and Hin
Table 4.7 Mean of external and internal hazard indices values in the soil samples from
residential college areas of University of Malaya
a
College Hex ≤ 1 Hin ≤ 1
ay
C1 0.43 0.58
C2 0.51 0.67
al
C3 0.35 0.47
C4 0.51 0.65
C5 0.43 0.57
C6
C7
M 0.45
0.43
0.59
0.55
C8 0.51 0.67
of
C9 0.52 0.67
C10 0.4 0.55
C11 0.39 0.51
ty
to gamma radiation hazards. The representative gamma index (Iγr) estimates the
U
radiation hazard of gamma rays due to the individual radioactivity levels of the targeted
primordial radionuclides in the soil samples. (Iγr) can be computed using the equation
Iγr = (4.9)
58
226 232
where CRa, CTh and CK are the measured specific activity concentration of Ra, Th,
and 40K respectively. The representative gamma index of this study is reported in table
4.8
Table 4.8 Mean of representative gamma index indices values in the soil samples from
residential college areas of University of Malaya
College Iγr ≤ 1
C1 1.15
C2 1.31
C3 0.92
C4 1.32
a
C5 1.11
C6 1.17
ay
C7 1.15
C8 1.35
al
C9 1.37
C10 1.06
C11 1.04
C12
M
Total Mean
1.24
1.18
of
The significance of exposure from natural radioactivity in soil and the possible
si
health risk especially cancer, has gained global attention. Some regulatory bodies make
r
use of quantitative risk assessment process to determine excess cancer risk over a
ve
lifetime (ELCR). Two of these bodies are United Nations Scientific Committee on the
ni
Ionizing Radiation (BEIR) Both organizations agreed that their risk estimates should be
reduced for a low dose exposures protracted over several months or years to account for
Therefore, there is need to determine the excess cancer risk over a lifetime (ELCR).
The probability of developing cancer over a lifetime at a given exposure level can be
59
cancers expected in a given population exposure to carcinogen (effective cancer causing
(2014) excess lifetime cancer risk (ELCR) can be estimated using the following formula
where AEDE, DL, and RF are annual effective dose equivalent, average lifetime
duration (70 years) and risk factor (0.05 Sv−1). i.e fatal cancer risk per Sievert
respectively.
a
ay
The excess lifetime cancer risk (ELCR) of this study is reported in table 4.9
al
Table 4.9 Mean of excess lifetime cancer risk (ELCR) values in the soil samples from
residential college areas of University of Malaya.
M
College ELCR (x10-3)
C1 0.31
C2 0.35
of
C3 0.25
C4 0.35
C5 0.3
ty
C6 0.31
C7 0.31
si
C8 0.36
C9 0.37
r
C10 0.29
ve
C11 0.28
C12 0.33
ni
Table 4.10 below is the summary of activity concentration and radiological hazard
parameters in the soil samples from residential college areas of University of Malaya.
60
Table 4.10 summary of activity concentration and radiological hazard parameters in the soil samples from residential college areas of University of
a
Malaya
ay
College Activity concentrations Dose Hazard indices (≤ 1)
(Bq kg-1)
al
226 232 40
Ra Th K Raeq DR (nGyh-1) AEDE (mSvy-1) AGDE AUI Hex Hin Iγr ELCR (x10-3)
(µSv y-1)
M
C1 54.6 57.87 306.43 160.95 72.96 0.09 506.83 1.23 0.43 0.58 1.15 0.31
C2 61.27 78.44 180.19 187.31 83.2 0.1 573.78 1.53 0.51 0.67 1.31 0.35
C3 42.16 55.24 131.5 131.28 58.33 0.07 402.47 1.07 0.35 0.47 0.92 0.25
of
C4 54.33 80.27 237.43 187.4 83.48 0.1 577.96 1.49 0.51 0.65 1.32 0.35
C5 53.41 64.85 152.99 157.93 70.22 0.08 484.15 1.29 0.43 0.57 1.11 0.3
C6 50.38 69.58 212.55 166.25 74.17 0.09 513.26 1.32 0.45 0.59 1.17 0.31
ty
C7 43.41 65.45 303.82 160.4 72.26 0.09 503.12 1.22 0.43 0.55 1.15 0.31
C8 57.7 78.16 270.09 190.27 85.13 0.1 589.81 1.5 0.51 0.67 1.35 0.36
C9 53.5 81.8 294.55
i
193.15 86.41 0.1 599.73 1.51 0.52 0.67 1.37 0.37
C10 54.09 52.89 262.41
rs
149.93 67.88 0.08 470.62 1.16 0.4 0.55 1.06 0.29
C11 42.73 57.13 270.18 145.23 65.51 0.08 455.68 1.11 0.39 0.51 1.04 0.28
ve
C12 60.15 79.4 73.07 179.32 78.79 0.1 540.7 1.52 0.48 0.65 1.24 0.33
Mean 52.31 68.42 224.58 167.45 74.86 0.09 518.18 1.33 0.45 0.59 1.18 0.32
ni
U
61
Table 4.11 shows a summary of 226Ra, 232Th and 40K activity concentration,
absorbed dose rates, annual gonadal dose equivalent and excess lifetime cancer risk in
Table 4.11 Summary of activity concentration 226Ra, 232Th and 40K, absorbed dose
rates, annual gonadal dose equivalent and excess lifetime cancer risk in different areas
of Malaysia and world values.
a
(µSv y-1)
Pontain 53 293 158.36 Muneer et al
37 69 237 0.344
ay
District 2013
UluTriram Abdulrahma
44 200 245 1
Johor n et al 2007
Melaka Sahrone et
183 225 0.915
al
State al 2005
Kinta
Lee et al
District 112 246 277 222 272 1.11
2009
Perak
Sungai
Kampung
196 628 475
M 458 562 2.29
Apriantoro
et al 2009
Khalik et al
Palong 500 614 2.5
2005
of
174.64 Abdel et al
Johor State 163 200 0.815
2001
Selama Ramli et al
178 353 296 273 335 1.36
District 2009b
ty
2000
r
ve
ni
U
71
CHAPTER 5: DISCUSSION
concentration and radiation hazard indices in the soil collected from the residential
out and results obtained. The results of the study are discussed under the following
subheadings;
a
226 232 40
5.1 Radioactivity levels of Ra, Th and K in the residential college areas
ay
of University of Malaya
al
Comparing the activity concentration values of the radionuclides in the twelve (12)
226
residential college areas of University of Malaya, (Table 4.1), Ra was highest at
M
college two (C2) with mean concentration value of 61.27±2.35 Bq/kg, followed by
of
colleges; C12, C8, C1, C4, C10, C9, C5, C7, C11 and lastly C3 with concentrations values of
Bq/kg, 53.5±2.81 Bq/kg, 53.41±1.88 Bq/kg, 43.41±2.15 Bq/kg, 42.73±2.65 Bq/kg and
si
226
42.16±2.86 Bq/kg respectively. The high level of Ra recorded in C2, C12 and C8 may
r
be due to the clay nature of the soils and fertilizer applied for horticultural purposes.
ve
226
The total average concentration of Ra in all the twelve (12) residential colleges is
ni
226
52.31±2.40 Bq/kg. Average concentrations of Ra in all the colleges are higher than
U
the world average of 33 Bq/kg but lower than the Malaysian average value of 66 Bq/kg
recorded in college nine (C9) and least value in college ten (C10). The total average
232
activity concentration of Th was 68.42±1.92 Bq/kg. The study showed that the mean
232
activity concentration values of Th in all the areas studied are higher than the world
72
average but lower than Malaysia average of 82 Bq/kg. The range of average activity
40
concentration of K was 306.43±4.77 Bq/kg to 73.07±4.91 Bq/kg with total mean
activity concentration of all the colleges at 224.58±2.28 Bq/kg. Colleges one (C1) and
40
twelve (C12) had the highest and lowest values of K activities respectively. The
average radioactivity level of 40K in this study was seen lower than the world average of
420 Bq/kg and Malaysia average of 310 Bq/kg. The high values in the average
226
concentration of Ra, 232Th and 40K recorded in some colleges may be due fertilizer
applied for horticultural purposes. The loamy and clay nature of the soils may also
a
ay
affect the concentration of the radionuclides.
Comparing the result obtained from this study with results from other surveys in
al
Malaysia, as shown in table 4.11, it was observed that the values of 232Th, 226Ra and 40K
M
in this study were lower than values in most of the previous studies. UNSCEAR (2000),
reported crustal concentrations of areas with normal background radiation levels around
of
238 232 40
the world as 16-110Bq/kg for U, 11-64 Bq/kg for Th and 140-820Bq/kg for K.
ty
Therefore, the activity concentrations of the three radionuclides obtained in this study
were consistent with world range and the soil can be classified under area of normal
si
background radiation.
r
ve
The radioactivity levels of natural radionuclides in the area of this study were in
agreement with the global trend on the distribution of natural radionuclides in soil. The
ni
and conditions of the soil of the study area. Besides these natural factors, human
improve the soil nutrients for plant growth had been known to be a contributor to the
73
5.2 Radium equivalent Index
Examining table 4.2, the highest mean value of activity was recorded at college nine
(C9) 193.15Bq/kg while the least mean value was observed in college three (C3) with
131.28 Bq/kg. The overall mean value of radium equivalent activity in all the twelve
(12) residential college areas of University Malaya was found to be 167.45 Bq/kg.
Report from (Sam & Abbas, 2001; Shiva Prasad et al., 2008) stated that the use of
order to avoid radiation hazards. The radium equivalent of 370 Bq/kg corresponds to the
a
ay
dose limit of 1mSv for the general public. As it is evident in table 4.3, none of the
colleges had mean radium equivalent activity value that exceeds 370Bq/kg. Therefore,
al
soil from residential college areas of University of Malaya is safe from radiation
M
hazards since the radium equivalent is less than 370Bq/kg.
ground due to the concentrations of 226Ra, 232Th and 40K were found to be 72.96 nGy/h,
83.20 nGy/h, 58.33 nGy/h, 83.48 nGy/h,70.22 nGy/h, 74.17 nGy/h, 72.26 nGy/h, 85.13
si
nGy/h, 86.41 nGy/h, 67.88 nGy/h, 65.51 nGy/h, 78.79 nGy/h for colleges one to twelve
r
ve
respectively. The range of the mean gamma absorbed dose rate of all the college areas
was 86.41 nGy/h to 58.33 nGy/h with highest and lowest values recorded at C9 and C3
ni
respectively. The overall mean gamma absorbed dose rate from University Malaya
U
residential college area soil was 74.86 Bq/kg. This value is higher than the global
standard average value of 59 nGy/h but lower than maximum permissible value. The
In table 4.4, the highest values of outdoor annual effective dose equivalent values
were recorded in C2 , C4, C8, C9, & C12 at 0.10 mSvy-1 and the least value reported in C3
74
at 0.07mSvy-1 soil samples from residential college areas of University of Malaya. The
calculated mean values of all the colleges ranged 0.07 to 0.1 mSvy-1 and the overall
mean was 0.09 mSvy-1 which is lower than the global average value of 0.45 mSvy-1 and
also less than the dose criterion limit of 1.0 mSvy-1. Since the result obtained from this
survey is less than the criterion limit, the soil from the area of study does not pose any
The mean values of Annual gonadal dose equivalent are presented in table 4.5.
a
ay
College nine (C9) and College three (C3) showed highest and lowest values in this study
with 599.73 μSvy-1 and 402.47 μSvy-1 respectively. The overall mean value of annual
al
gonadal dose equivalent was 518.18 μSvy-1. This value was far higher than the
M
USCEAR value of 72 μSvy-1 reported as global average but within the range of
Malaysia values.
of
5.6 Activity utilization index
ty
Table 4.5 presented the mean values of the activity utilization index of residential
college area of University of Malaya. The values varied from 1.07 to 1.53 with the
si
highest value observed in college two (C2) and least in college three (C3). The overall
r
ve
average mean of all the colleges was 1.33. This value is above 1 which is the value of
AUI that corresponds to an annual effective dose safety limit. Although the mean value
ni
of AUI in this study was high but it is still below the maximum permissible limit.
U
From table 4.7, the overall average of the external hazard index calculated from the
twelve residential college areas of University of Malaya was 0.45, while individual
college values varies from 0.35 to 0.52. The highest value was observed in College nine
(C9) and least value in college three (C3). Since the world safe limit is put at 1,
75
therefore, the soil of University of Malaya college areas with 0.45 average values is safe
Table 4.7 reported the highest values of internal hazard indices at colleges; two (C2),
eight (C8) and nine (C9) with values of 0.67. The least values was college three (C3)
with 0.47 and the overall mean value of all the colleges was found to be 0.59. The
global recommended safe limit value for internal hazard indices was reported at 1 and
a
all the values from the colleges are lower.
ay
5.9 Representative gamma index
al
Considering all the values in table 4.8, the highest mean value of the representative
M
gamma index was found at college nine (C9) with 1.37 value and he least value was at
college three (C3) with 0.92. The total average value of representative gamma index for
of
University of Malaya residential college areas soil was calculated to be 1.18. The value
ty
was above the recommended unit value to keep the effective dose rate below or at
1.0mSvy-1.
r si
Making reference to table 4.9, the excess lifetime cancer risk values of University of
ni
Malaya residential college areas soil ranged from 0.25 x10-3 to 0.37x10-3. The highest
U
value was observed at college nine (C9) and least value at college three (C3). The total
value of excess lifetime cancer risk for University of Malaya residential college areas
soil was calculated as 0.32x10-3. The excess lifetime cancer risk for UM college areas
was a higher when compared with the world average value of 0.29 x10-3. The chances
of developing cancer over a lifetime by members of the public utilizing the environment
are 10.3%.
76
CHAPTER 6: CONCLUSION
have been measured using a gamma-ray spectrometer with high purity germanium
(HPGe) detector. The activity concentrations of the three radionuclides have been used
to calculate the radium equivalent activity, absorbed dose rate, annual effective dose
equivalent, annual gonadal dose equivalent, activity utilization index, external hazard
a
ay
index, internal hazard index, representative gamma index and excess lifetime cancer
al
The following conclusions were made from the survey:
2. The average value for each of the assessed radiological hazard parameter in the
areas was found to be below world safety limit set by UNSCEAR; therefore, the
si
3. The calculated overall mean concentration ratio was 1.308 which is lower
ni
compared with the world’s ratio of 3.5. And the concentration ratio is 0.765
U
4. The values of absorbed dose rate, annual gonadal dose equivalent, activity
utilization index, representative gamma index, and excess lifetime cancer risk
were higher than the world average values but were below the permissible limit.
internal hazard indices values were lower than the world’s values which shows
77
that the soil of residential college areas of University of Malaya, Malaysia pose
7. The results of this study provide a general background level for the area studied
and can be used as baseline data and guide for future evaluation and assessment
8. The analysis provides good experience and skills for naturally occurring
a
ay
6.1 Limitation and suggestion for further studies
al
The major constraint encounter in this study was the frequent breaking down of the
detector. This limitation affected the expected time of completion of this research. With
M
the experiences gained from this survey, the following suggestions are recommended
of
for further study:
them about the survey, so to grantee the safety and integrity of the researcher.
si
78
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