RADIONUCLIDE CONTENT OF SAND USED FOR CONSTRUCTION IN KAKAMEGA COUNTY AND ASSOCIATED INDOOR RADON DIFFUSION DOSES SHIKALI N. COLLINS [B.Ed. (Sc)] I56/CE/15221/2008 A thesis submitted in partial fulfillment of the requirements for the award of the degree of Master of Science in the School of Pure and Applied Sciences of Kenyatta University. August, 2013. ii DECLARATION This thesis is an original work and has not been presented for the award of a degree at any other institution of higher learning. Shikali N. Collins Signature: ……………………. Date: ……………… I56/CE/15221/08 Department of Physics Kenyatta University Nairobi, Kenya ` Supervisors: Dr. W.J. Ambusso Signature ……….………….… Date ……….. Department of Physics Kenyatta University Nairobi, Kenya Dr. M. K. Munji Department of Physics Kenyatta University Nairobi, Kenya Signature …………………. Date ………….. iii DEDICATION This thesis is dedicated to my wife Lydia, son Dennis Ndenga and daughter Venus Irangi. iv ACKNOWLEDGEMENTS I sincerely thank my supervisors Dr. Ambusso and Dr. Munji (Kenyatta University) for their whole hearted continuous academic and moral support. Without them this study would have been impossible. I thank the whole Kenyatta University Physics Department for providing laboratory facilities, Internet Services for accessing scientific journals and technical staff that have made this research successful. Thanks to Dr. Angeyo (University of Nairobi) for providing useful literature materials, activated charcoal canisters and IAEA standard samples. I also thank fellow Kenyatta University Physics students particularly Tuwei A., Masinde T., Abuga V., Adero B, Businei M. just to name but a few for their moral support and academic support. Iam very much indebted to the National Council for Science and Technology (NCST) for their sponsorship. The encouragement and financial support I received from NCST through Prof. Shaukat Abdulrazak (Secretary/ CEO) is highly appreciated. I sincerely thank my wife Lydia for encouragement, patience and all forms of support during the research period. Sincere gratitude to all my family for their support during this period. Above all I thank the Almighty God for leading me this far. I confess that it is through his grace that I have reached this far. v TABLE OF CONTENTS DECLARATION ................................................................................................................ ii DEDICATION ................................................................................................................... iii ACKNOWLEDGEMENTS ............................................................................................... iv LIST OF TABLES ........................................................................................................... viii LIST OF FIGURES……………………………………………………………………..ix ABBREVIATIONS AND ACRONYMS .......................................................................... xi ABSTRACT ...................................................................................................................... xii CHAPTER ONE ................................................................................................................. 1 INTRODUCTION .............................................................................................................. 1 1.1 Background to the study ............................................................................................... 1 1.1.1 Radon… ..................................................................................................................... 2 1.1.2 Modeling of radon entry in houses ........................................................................... 3 1.2 Physiographical and geological outline of Kakamega County .................................... 3 1.3 Statement of the research problem ............................................................................... 4 1.4 Objectives ..................................................................................................................... 5 1.4.1 Main Objectives ........................................................................................................ 5 1.4.2 Specific Objectives .................................................................................................... 5 1.5 Rationale of the study ................................................................................................... 6 CHAPTER TWO ................................................................................................................ 7 LITERATURE REVIEW ................................................................................................... 7 2.1 Natural radioactivity and indoor radon ......................................................................... 7 2.2 Related studies on natural radioactivity of sand used for construction and indoor radon…… ........................................................................................................................... 7 2.2.1 Biological effects of ionizing radiation.................................................................... 10 CHAPTER THREE .......................................................................................................... 12 THEORETICAL CONCEPTS OF GAMMA RAY SPECTROMETRY AND INDOOR RADON DIFFUSION FLUXES ...................................................................................... 12 3.1 Theoretical background to gamma radiation .............................................................. 12 3.2 Secular equilibrium ..................................................................................................... 12 3.3 Gamma Ray Spectrometry .......................................................................................... 13 3.3.1 Interaction of Gamma ray with matter ..................................................................... 13 3.3.2 Photoelectric Effect .................................................................................................. 14 vi 3.3.3 Compton Scattering ................................................................................................. 15 3.3.4 Pair production ......................................................................................................... 17 3.4 Principal mechanism of NaI(Tl) gamma ray detector................................................ 17 3.5 Indoor radon ................................................................................................................ 18 3.5.1 Radon generation ..................................................................................................... 19 3.5.2 Radon transport in sand as a building material ........................................................ 21 3.5.3 Estimation of radiation dose in dwellings ................................................................ 23 3.6 Radiation quantity and exposure units ........................................................................ 24 3.6.1 Radiation concentration ........................................................................................... 24 CHAPTER FOUR ............................................................................................................. 26 MATERIALS AND METHODS ...................................................................................... 26 4.1 Materials and Equipment used in this study ............................................................... 26 4.2 Sample collection and preparation .............................................................................. 27 4.3 Radioactivity Measurements ....................................................................................... 27 4.3.1 Energy calibration in NaI (Tl) spectrometry ............................................................ 29 4.3.2 Determination of Gamma Activities ........................................................................ 32 4.3.3 Detector counting efficiency .................................................................................... 32 4.2.4 Detection limits of the analytical system ................................................................. 33 4.3.5 Energy Resolution of the detector............................................................................ 34 4.3.6 Gamma ray spectral data analysis ............................................................................ 36 4.3.7 Analysis of Certified Reference Materials (IAEA-RGK-1, RGTh-1 and RGU-1) . 36 4.4 Activity Concentrations .............................................................................................. 36 4.5 Radiological parameters.............................................................................................. 37 4.5.1 Gamma dose rate...................................................................................................... 37 4.5.2 The Annual Effective Dose Rate (AEDR) ............................................................... 38 4.5.3 Radium Equivalent Activity .................................................................................... 38 4.5.4 External hazard index (Hex) ..................................................................................... 39 4.5.5 Gamma Index (Iγ) ..................................................................................................... 39 4.6 Modeling of radon diffusion fluxes in a room ............................................................ 40 4.6.1 Theory of modeling.................................................................................................. 40 4.6.2 The governing equations .......................................................................................... 41 4.6.3 Program Structure .................................................................................................... 43 4.7 Estimation of uncertainties ......................................................................................... 44 4.7.1 Uncertainty due to sample preparation .................................................................... 45 vii 4.7.2 Uncertainty due to Efficiency calibration ................................................................ 45 4.7.3 Uncertainty due to measurement of samples ........................................................... 45 CHAPTER FIVE .............................................................................................................. 47 RESULTS AND DISCUSSION ....................................................................................... 47 5.1 Radioactivity concentration of building sand ............................................................. 47 5.1.1 Exposure due to gamma radiation............................................................................ 50 5.1.2 External hazard index (Hex) ..................................................................................... 52 5.1.3 Gamma Index (Iγ)..................................................................................................... 52 5.1.4 Statistical analysis of 226Ra, 232Th and 40K in this study .......................................... 54 5.2 Indoor radon Model Results........................................................................................ 56 5.3 Model validation ......................................................................................................... 62 CHAPTER SIX ................................................................................................................. 65 CONCLUSIONS AND RECOMMENDATIONS ........................................................... 65 6.1 Conclusions ................................................................................................................. 65 6.2 Recommendations ....................................................................................................... 66 REFERENCES ................................................................................................................. 68 APPENDICES .................................................................................................................. 74 viii LIST OF TABLES Page Table 4.1: The parameters of polynomial used for calibration of the detector…………………………………………………..30 Table 4.2: Efficiencies of emission of K-40, Th-232and U-238 in NaI(Tl) spectrometry……………………………………………..…..33 Table 4.3: The fit parameters for the Caesium- 137 photo peak Measured in this work………………………………………………......35 Table 4.5: Dispersion of measured activities from certified activities For (RGK-1, RGTh-1 and RGU-1) …………………………..36 Table 5.1: Average activity concentration of radionuclide in sand from Old gold mining zones of Kakamega County………………..48 Table 5.2: Comparison between radium equivalent activities, indoor Gamma Dose rates and annual effective dose in the present Study and those reported in other countries…………………49 Table 5.3: Radium equivalent activity, external hazard indices, dose rate and Annual effective dose …………………………………...51 Table 5.4: Comparison of hazard indices in present study and those for Other countries………………………………………………..51 Table 5.5: Statistical summary of radionuclide…………………. ............54 Table 5.6: Limits of kurtosis for normal distribution (Taylor, 1990)…….55 Table 5.7: Limits of skewness factor for normal distribution (Taylor, 1990)…………………..…………………………………….…5 ix LIST OF FIGURES page Figure 3.1: A schematic diagram illustrating Photoelectric-effect………14 Figure 3.2: Schematic diagram illustrating Compton Scattering process………………..……………………………………....15 Figure 3.3: Radiation detection using Thallium activated Sodium Iodide [NaI(Tl)] detector…………………………………….………18 Figure 3.4: Schematic representation of advective and Diffusive transport of radon in sand as a porous material…………………………22 Figure 3.5: Possible uncertainties that could be considered in determination of activity concentrations of NORM in sand samples………...……………………………..……………….28 Figure 4.1: A map showing the sampling sites in old gold mining region of Kakamega County…………………….…………………..28 Figure 4.2: Schematic diagram of NaI(Tl) spectrometer used To measure radioactivity concentration…………………..……………….29 Figure 4.3: Energy calibration of NaI(Tl) detector used….…………...…31 Figure 4.4: A typical gamma ray spectrum of construction Sand sample…………….………………………………………....31 Figure 4.5: Gaussian fitting of Caesium -137 spectrums measured in this work…………………….…………………………………....35 Figure 4.6: A schematic chart showing the main parts of the Program………………………………………………………44 Figure 5.1: Activity concentration and radium equivalent Activity distribution in all the sampling sites……………..…………..50 Figure 5.2: A scatter plot of the external hazard indices and Gamma hazard indices for different samples ……………….54 Figure 5.3: Two dimensional gridding of the model room…………..….57 Figure 5.4: Different build-up curves for the exhaling source block…….58 Figure 5.5: Radon Concentration profiles in the blocks [diffusion only] ………………………………………………………………59 x Figure 5.6: Radon Concentration profiles in the blocks [diffusion with decay] …………………………………………………………….....61 Figure 5.7: A comparison of concentration profiles in blocks where Radon diffuses with and without decay……………………………..61 Figure 5.8: A comparison of measured and modeled radon concentration ………………………………………………………………63 Figure 5.9: Radon growth curve obtained by fitting measured radon Concentration for monitoring station 1………………………63 xi ABBREVIATIONS AND ACRONYMS ADC Analogue to Digital Converter EPA Environment Protection Agency EFDM Explicit Finite Difference Method FWHM Full Width at Half Maximum HBRA High Background Radiation Area HV High Voltage IAEA International Atomic Energy Agency ICRP International Commission on Radiological Protection IUPAC International Union of Pure and Applied Chemistry MCA Multichannel Analyzer NaI(Tl) Thallium activated sodium Iodide Detector NCRP National Council on Radiation Protection NORM Naturally Occurring Radioactive Material OECD Organization for Economic Cooperation and Development PM Photomultiplier TAP Total Absorbed Dose TENORM UNSCEAR W HO Technologically Enhanced Naturally Occurring Radioactive Material United Nation Scientific Committee of the Effects of Atomic Radiation World Health Organization xii ABSTRACT The greatest portion of radiation received by world‟s population comes from natural radioactive sources. Everyone on earth receives natural radiation; some get much more than others depending on where they live. Primordial radionuclide in building sand and gravels from quarries are some of the sources of radiation hazards common in dwellings and working places. In this study, activity concentrations of naturally occurring radionuclide in mineral sand used for construction collected in old gold mining belt of Kakamega County were measured using gamma ray spectrometry technique, [NaI(Tl)]. The results of the concentrations of naturally occurring radionuclide were as follows: 226 Ra ranged from 36.79±8.89 to185.21±5.89 Bqkg-1, 232Th ranged from 51.12±2.56 to 158.92±7.95 Bqkg-1 and 40K ranged from 322.38±16.12 to 960.53±48.03 Bqkg-1. The calculated radium equivalent activity (Raeq), the absorbed dose rate (D), and the external hazard index (Hex) were within the international recommended values. Hence construction sands from the study region do not pose any risk to the inhabitants in terms of the acceptable limits. The movement of radon by diffusion from the walls of classrooms constructed from such sand into indoor air was modeled based on radiological parameters. The posed model predicted an ambient indoor radon concentration of 9 Bqm3 , 15.6 Bqm-3 and 28.7 Bqm-3 in three monitoring stations (classrooms) in the region. The modeled radon concentrations were lower than measured; the model reproduced the general trends associated with diffused indoor radon fluxes. Thus it can be helpful in estimating radon concentrations for other similar processes such as estimating radon concentration in caves and mines. 1 CHAPTER ONE INTRODUCTION 1.1 Background to the study Natural radioactivity is widespread in human immediate environment. It can originate from terrestrial radiation, cosmic radiation or indoor radiation from building materials. Researchers have shown that the presence of natural radioactive sources such as Radium226 (226 Ra) and Thorium-232 (232 Th), and their progenies, and Potassium-40 (40K) in building materials result in harmful external and internal effects to occupants. The external effect is caused by direct gamma radiation from the natural occurring radionuclide (NORM) affecting external organs like skin. The internal effect normally affects internal organs mainly the respiratory tract, is due to radon and its daughters which are released from building materials (European Commission, 1999). For instance, high concentration of radon gas has been identified to cause lung cancer among persons exposed to high doses of radon. Good examples are people working in mines. Indoor radon is released from the radium trapped in mineral grains of the building materials. The gas then escapes to air because the radon diffusion length is comparable to the thickness of the material (Rizzo et al., 2001). This contribution depends on concentration of radium, which is generally low in materials of low activity (UNSCEAR, 1999). The harmful effects of gamma radiation from building materials and radon in dwellings are generally well known, but information on concentration levels of radon in dwellings and work environment in Kenya is not readily available. There is therefore a 2 need to study building materials from areas perceived to have higher concentration of NORM with the aim of measuring and documenting their actual levels in dwellings. This is aimed at estimating the actual risk of exposure due to ionization radiation that people are exposed to. In this study, a theoretical model to estimate the contribution of mineral sand used for construction to the indoor dose rate and to radon air contribution is developed. Knowledge of the level of natural activity in mineral sand is thus important to assess the possible radiological hazards to human health and to develop standards and guidelines for use and management of sand used as building material. 1.1.1 Radon Radon is a colorless odorless noble gas with atomic number 86. It is one of the decay products of uranium and thorium decay series. It has three isotopes; 235 220 Rn and Rn that originate from 222 Rn is considered important due to its longer life as compared to the others. The other Th and 238 Rn, 222 U, 232 219 U decay series, respectively. In this work isotopes of radon will be mentioned explicitly. Radon is believed to originate from materials that are rich in uranium. Such materials are soil, sand, rocks, gravels and many others. Since it is a gaseous product, it responds to temperature and pressure gradients. It may succeed in escaping out of such materials and get mixed with air because of its relatively long life. If it escapes to a confined space with limited ventilation, its concentration may become fairly high. Humans living in such confined places inhale air which may be rich in radon and its daughters. The radioactive heavy metal daughters of radon including 218 Po, 214 Pb, 214 Bi and 214 Po are short lived. 3 Thus, once inhaled; they remain in the “mucus” lining and may be lodged in lungs (James, 1987). On decaying, they deposit large amount of energy in the surrounding tissues, causing cancer. Several techniques can be applied for measurement of radon and its daughters. These techniques are based on active and passive methods. The criterion for selection is based on objective behind the measurement, available equipment, and the costs among others. 1.1.2 Modeling of radon entry in houses A model is a representation of a real process or system. In an effort to understand indoor radon concentration this study focuses on radon entry into houses which depends on the following factors: radon generation from the source; transport properties of the source; transport properties of the interface between the source and indoor air and the driving forces. There are three approaches applied when modeling radon entry in houses; these are analytic modeling, lumped parameter modeling and numerical modeling (Carmen, 1992). In this study, a numerical model for estimating the contribution of mineral sand used for building to the indoor dose rate and to the radon air concentration is developed. Knowledge of the level of natural activity in mineral sand is thus important in assessing the possible radiological hazards to human health and in developing standards and guidelines for use and management of sand used as building material. 1.2 Physiographical and geological outline of Kakamega County Kakamega county is located in Western Kenya about 30 km north of equator, 52 km 4 north of Kisumu at latitude N 00 30 – N00 0 and longitude E340 30 – E350 0. The average elevation of kakamega is 1535m (ISRIC, 2012). It borders the indigenous Kakamega forest on the west and has three main rivers i.e. R. Nzoia, R. Yala and R. Isiukhu flowing across the county to Lake Victoria. The construction sand deposits are mainly found from these rivers and they are sources of domestic water supply in the county. The underlying rocks in this area are associated with ancient gneisses of Kavirondo and Nyanzian systems as well as basalt, phenolites and gold – bearing quartz veins. They are referred to as Kisumu- Kakamega- Mumias granite- greenstone complex. The main inhabitants of this region are the Luhya. Their main economic activities include small scale subsidence farming, large scale sugar – cane and tea growing, small scale artisanal gold mining and small scale trading. 1.3 Statement of the research problem There is inadequate knowledge about the levels of naturally occurring radionuclide that result from sand used for construction in Kakamega County; though, several studies on risks of human exposure and impact of ionizing radiations from NORM due to sand used for construction from other places have been documented (Xinwei et al., 2006 and Cervic et al., 2009). Similarly, there is scanty or no data and records on levels of radon in dwellings and work places in this region. Adequate data is important for regulatory and advisory purposes in protection of the general public from unnecessary exposure to radiation. Thus, measuring the activity concentration of naturally occurring radionuclide in mineral sand used for construction in this region is important for evaluation of the 5 impact of radiation on the environment and in the assessment of radiation effects on human population (Tuo et al., 2010). This is particularly important for building materials since most people spend 80% of their time indoors (UNSCEAR, 1999). 1.4 Objectives 1.4.1 Main Objectives This research sets to achieve two main objectives. The first one is to measure the activity concentration of 226 Ra, 232 Th and 40 K in mineral sand used for construction in old gold mining belt of Kakamega County. The activity concentration values are used to assess the external annual dose for individuals living in dwellings constructed using such sand in this region. Secondly, the research aims to develop a theoretical model for estimation of the contribution of mineral sand to the indoor radon dose rate. 1.4.2 Specific Objectives The specific objectives are as follows; i. To determine the radioactivity concentration of naturally occurring radionuclide present in the mineral sand used for construction in old gold mining zones of Kakamega County. ii. To estimate the radiation doses that people are exposed to due to indoor gamma radiation and indoor radon in the region. iii. To develop predictive models for the diffused radon concentrations fluxes in a room, assuming that all dwellings, classrooms and other buildings in the region are constructed using mineral sand. 6 1.5 Rationale of the study Environmental impact due to effect of ionizing radiation from NORM in this region is difficult to assess due to inadequate data. In this study, measured data about levels of naturally occurring radionuclide has been provided and modeling of radon fluxes in a room has been done. Availability of such information is helpful in understanding the doses that people are exposed to. It is envisaged that the results of this study will be useful to the relevant scientific committees, government and non-governmental organizations in making decisions about mineral sand as a building materials in this region. 7 CHAPTER TWO LITERATURE REVIEW 2.1 Natural radioactivity and indoor radon There has been concern about the effects of radon and gamma radiation exposure to people especially in dwellings, schools and working places in Kenya (Mustapha et al., 1997). Due to insufficient information about the concentrations and harmful effects of gamma radiation and radon, many people have continued to work and leave in dwellings unaware of the dangers posed by these radiations in their lives. Besides, remedial action even when possible is never undertaken because of lack of sufficient and relevant information. In this study concentration level of NORM in construction sand from old gold mining belt of Kakamega has been measured. Radon concentration fluxes in a room were modeled using activity concentration of 226 Ra measured from sand. The assessment of natural radioactivity in this region is important because industrial, agricultural, artisanal gold mining, etc have resulted in Technologically Enhanced Naturally Occurring Radionuclide Materials (TENORM) that have elevated the levels of NORM in the environment (Bliss, 1987; Salman and Amany, 2008). These naturally occurring radionuclides emit ionizing radiations that cause somatic and genetic effects in human beings. 2.2 Related studies on natural radioactivity of sand used for construction and indoor radon Worldwide a number of studies have been undertaken to assess the hazards posed to 8 humans due exposure to radiation from naturally occurring radionuclide in the environment. In Pakistan, natural radioactivity and radiological hazards have been assessed for soils and building materials in six district of Punjab Province (Faheem et al., 2008). The annual effective dose equivalents were found to vary from 0.10 to 0.37mSv. These results showed that the materials are safe to be used as building materials. In Turkey, an assessment natural radioactivity of sand used for construction in the whole country has been done (Cervic et al., 2009). The measured activity in sand samples ranged from 17 to 97 Bq/kg, 10 to 133 Bq/kg and 16 to 955 Bq/kg for 40 226 Ra, 232 Th and K respectively. The study showed that measured sand samples do not pose any significant source of radiation hazard and are safe to be used as building materials. In Greece, measurement of indoor radon levels and natural gamma radiation in public work places was done in north - western part of the country (Papachritodouloou et al., 2010). They found that the radon concentration followed a log- normal distribution with arithmetic mean of 95±5 Bq/m3, which is within the European Commission recommendation. In Algeria, natural radioactivity in building materials has been assessed (Amran and Tahtat, 2001). The radium equivalent activities were below the gamma radiation dose rate (1.5 mSvy -1 ). Therefore, the use of the materials in construction of dwellings is considered safe for inhabitants according to Organization for Economic Cooperation and Development (OECD, 1979). 9 In Kenya, a number of studies have been undertaken to assess the hazards of human exposure to indoor external doses due to NORM in building materials and indoor radon. Natural radioactivity in some building materials and the contributions to the indoor external doses has been studied (Mustapha, 1999). It was reported that the activity concentration of 40 K was much higher than that of 226 Ra and 232 Th which is a common occurrence in normal geological materials. Measurement of indoor 222Rn concentration in dwellings of Kenyatta University has been documented (Chege, 2007). The measured average concentration during the sampling period was found to be 188 Bq/m3. A further investigation of the effects of meteorological parameters on indoor radon in model traditional huts has also been undertaken in Kenyatta University (Chege et al., 2007). The radon concentration in these huts correlated positively with rainfall, but negatively with outdoor air temperature and wind speed. The average radon concentration reported was 170±39.6 Bqm-3 indicating that radon might pose radiological problems in such dwellings. ICRP (1993) recommends action levels for 222 Rn concentration of 200-600 Bqm-3. Other studies include the investigation of radon concentration in coastal and Rift valley regions (Maina et al., 2004). Higher concentration were reported in coastal region (43-704 Bqm-3) while Rift valley regions reported radon concentrations of less than 100 Bqm-3. Sarvovic and Djordjevic (2008) devised a model describing the flow of radon through concrete. The method allowed for the calculation of radon diffusion through concrete walls and hence estimation of indoor radon concentration. 10 None of these studies in Kenya has adequately investigated the effects of building materials and indoor radon in old gold mining belt of Kakamega County. It is envisaged that the results of this study will be helpful for setting limits of radionuclide concentration in construction sand or propose a ban on use of sand from this region in case the sand contain abnormally high activity concentrations. Furthermore none of these studies in Kenya have attempted to determine the backward or forward variation in radiation levels. This study introduces this aspect by developing a finite difference numerical model which estimates the variation of indoor radon levels in a room. 2.2.1 Biological effects of ionizing radiation Exposure to ionizing radiations can produce harmful effects on human health. Radon and its decay products is the main producer of harmful health effect. Others include ionizing radiation from NORM in building materials and soil. For instance lung cancer is mainly attributed to inhalation of radon. The Environment Protection Agency (EPA) estimate that radon may cause between 5000 – 20000 lung cancers (NCRP, 1984) in U.S.A. Biological effect starts when molecules in living cell interact with radiation energy through deposition and or exposure. If a large dose is delivered in a short period, symptoms of a cute radiation injury occurs. When delivered dose is much smaller and repeated for longer time, the biological effects may not appear for many years. These effects can be classified as direct or indirect effects. Direct effects occur when ionizing radiations cause excitation in the same molecule where the radiation is primarily deposited and absorbed. While indirect effects occur when ionizing radiation is absorbed (for example) in water molecule in human body and produces short lived chemically 11 reactive products i.e. radicals that react with other molecules in other parts of the body (Thermod and Maille, 2003). In an effort to minimize radiation exposure to members of the public, limits on exposure to ionizing radiation have to be set (ICRP, 1991). Hence, it is necessary to measure radiation dose in order to monitor the effects of nuclear radiation on biological tissue. 12 CHAPTER THREE THEORETICAL CONCEPTS OF GAMMA RAY SPECTROMETRY AND INDOOR RADON DIFFUSION FLUXES 3.1 Theoretical background to gamma radiation Gamma rays are the most energetic and harmful form of electromagnetic radiation that are produced when radioactive nuclei undergoes transitions. Gamma radiation is mostly produced alongside other forms of radiation such as α and β. Unstable atomic nuclei spontaneously decay to produce stable nuclides, the daughter nuclei are sometimes produced in excited states. The subsequent decay of excited state results in emission of γrays. They can also be produced when there is positron annihilation in matter. 3.2 Secular equilibrium The total activity of a radionuclide undergoing radioactive decay can be calculated by considering a long lived parent decaying into a shorter lived daughter which in turn, decays into a stable nuclide. Secular equilibrium is a condition in which the decay rates of the parent radionuclide and that of the daughter radionuclide are equal. This is only possible if the half-life of the parent radionuclide is longer. It should be long enough that there is no noticeable decay during the time interval of interest. If the parent radionuclide half-life is longer, but short enough so that there is noticeable decay of parent nuclei during the time interval of interest, a condition of transient equilibrium is reached. When state of secular equilibrium is reached, the activity of daughter radionuclide is determined by the activity of the parent radionuclide. 13 3.3 Gamma Ray Spectrometry Gamma ray spectrometry refers to the process of detection and measurement of gamma ray energy emitted during nuclear de-excitation process. Some radioactive sources produce gamma rays of various energies in the range 0.1 to 10 MeV. The energy produced is characteristic of the emitting nucleus hence used to identify the type of the radioactive nuclei. When these radiations are detected and analyzed using gamma ray spectrometry, a gamma ray energy spectrum is produced. A detailed analysis of the spectrum is used to identify the type and quantify gamma emitters present in the source. 3.3.1 Interaction of Gamma ray with matter Gamma rays are photons that originate from the nuclei of a radioactive atom undergoing decay. They have no mass and no charge. They are quanta of electromagnetic energy that travels at the speed of light and can travel long distances in air un-attenuated. When these photons interact with matter, free electrons are generated and as these electrons are slowed down by matter, they create charge pairs. The photon detectors use the charge pairs generated to determine the photon energy by measuring the quantity of charge produced by these pairs (Debertin and Helmer, 1988). Knowledge of interactions of gamma rays with detector matter is essential for the understanding of how the gamma photons are detected and attenuated in the detectors. There are three main mechanisms through which gamma photon interact with matter; photoelectric effect, Compton scattering and pair production. These mechanisms are discussed in the preceding subsections: 14 3.3.2 Photoelectric Effect Figure 3.1 shows a schematic diagram of a gamma ray photon absorption by an electron within an atom. When the incident gamma ray photon interacts with tightly bound electron in matter, the electron absorbs the incident photon energy and is emitted as a photoelectron. The emitted photoelectron leaves a vacancy in the shell of the atom making the atom excited. During de-excitation, X-rays or an Auger electron is emitted. If the absorber material is large enough, the X- rays will be absorbed in the surrounding matter. The kinetic energy of the ejected electron is given by Eq.3.1; Ee− = hν − Eb , (3.1) where Eb is the binding energy of the photoelectron‟s original shell, hν is the incidence gamma energy and Ee- is the kinetic energy of ejected photoelectron. Photoelectron E K-Shell hv Incident gamma photon Atomic Nucleus L-Shell Figure 3.1: Schematic diagram of gamma ray photon absorption by an electron in an atom Photoelectric effect is the most dominant mode of interaction of γ or x- ray photons with 15 matter for relatively low energy. Photoelectric effect is enhanced in absorber material of high atomic number. This can be illustrated by the interaction cross section τ, described in Eq. 3.2 (Knoll, 1989); 𝑍𝑛 𝜏 = 𝑐𝑜𝑛𝑠𝑡𝑎𝑛𝑡 × 𝐸 3.5 , (3.2) 𝛾 where, n varies between 3 and 5 over the gamma- or x-ray photon energy of interest. 3.3.3 Compton Scattering Figure 3.2 shows a schematic diagram illustrating Compton Scattering process in an atom where the incidence photon energy is greater than the binding energy of the bound electron in the atom. E h Scattered photon E h ss s s Recoil electron angle Figure 3.2: Schematic diagram illustrating Compton Scattering process In Compton Scattering the binding energy of the electron becomes less significant and the electron is considered free. Thus Compton scattering is the process of collision between incident gamma photon and an electron in the absorber. During the collision the gamma photon is deflected through angle θ with respect to its original direction as shown. 16 The total incident photon energy is not deposited at the initial interaction site, but there are series of Compton scattering events, which reduces the secondary photon energy before the sequence ends up with photoelectric absorption event. The energy of scattered photon is given by Eq. 3.3; h h , h 1 m0 c 2 (1 cos ) (3.3) where hν is the incident gamma ray energy, m0 is rest mass of ejected electron (0.511 MeV) and θ Scattering angle. If a head-on collision occurs, the incident gamma photon is scattered towards its direction of origin, leading to the energy transferred to the recoil electron in a single Compton interaction reaching a maximum value. This forms a special spectral feature known as the „Compton Edge‟. In normal situations, all scattering angles occur in a finite sized detector volume. Therefore, a continuum of energies is transferred to the recoil electron. The Compton interaction cross section is given by Eq. 3.4; cons tan t Z , E (3.4) where Z is the absorber atomic number and E is the incident gamma energy (hν). The interaction cross section increases linearly with the atomic number, Z of the absorber atom. 17 3.3.4 Pair production This is the process through which a gamma photon is transformed into an electronpositron pair. The process occurs close to the nuclei of the absorbing material due to high electric field at this point. A minimum gamma ray energy of 2m0c2 (1.022Mev) is required for any incident photon to undergo this process. Any excess energy above this value is transferred into kinetic energy which is shared by electron-positron pair. The electron and positron travels a few mm before losing their energy in the absorbing medium due to collisions within the medium. As the positron slows down due to collisions, the positron can combine with an electron from absorbing medium; this is followed by annihilation of both particles. The annihilated particles are replaced by two annihilation photons, each of energy m0c2 (0.511Mev) which are emitted back-to-back. The probability of pair production, k varies approximately as the square of the atomic number Z of the absorber material (Knoll, 1989) given in Eq. 3.5; f k = kαZ 2 , (3.5) 3.4 Principal mechanism of NaI(Tl) gamma ray detector The NaI(Tl) gamma ray detector used in this study operates on the principle of emission of light by florescent materials (scintillation) when illuminated by incident gamma radiation. Figure 3.3 shows a schematic diagram of the detection system of NaI(Tl) detector. The detector consists of a scintillation counter, a photocathode, a photomultiplier tube and associated electronics. When the incident gamma photon enters the scintillation counter, the photons deposit their energy in the scintillation counter 18 resulting in the elevation of detector atoms to excited states (the electrons of the atom jump from valence band, which is generally full to empty conduction band across energy band gap of ≈ 4eV). Eventually, the excited atoms lose their energy by emitting visible radiation and the electrons drop back to valence band. The visible radiation hit a photosensitive surface and photoelectrons are generated. Electrical pulses are formed by multiplying and accelerating the photoelectrons using a photomultiplier tube. Figure 3.3: Radiation detection using Thallium activated sodium Iodide [NaI(Tl)] detector 3.5 Indoor radon The main factors considered in determination of radon and progeny activities in dwellings include geology, climate, building materials, design and construction (especially single or multi-storey), building age, barometric pressure effects and lifestyle of the residents (Mudd, 2008). In this study, building sand contribute to gamma dose rate 19 through inhalation of radon and external irradiation by NORM in buildings constructed from such sand (Rizzo et al., 2001). Thus, the measurement of the radionuclide concentrations of sand was used to evaluate both indoor radon concentration and gamma dose rate. Indoor radon in dwellings can be studied in three levels; radon generation, transport and distribution inside dwellings via airflows. 3.5.1 Radon generation In dwellings indoor radon originate from presence of trace elements of 238 U in soil and building materials. Depending on the properties of building material, radon can be transferred through the building material and enter the dwelling space. Building materials such as sand in this case can generate radon by the decay of radium minerals in their components. The radon generated in building materials depends on the age of the building material, relative humidity, type and amount of building material (Michel van der Pal, 2003). The rate of radon generation is proportional to the amount of radium in the sand as a building material. Not all the radon generated is available for transport, part of it remain in the solid matrix of the sand. The ratio of the amount of radon that becomes available for transport to the total amount of radon generated is called emanation coefficient, η. The emanation coefficient is determined using Eq. 3.6; η = amount of radon available for transport total amount of radon generated (3.6) The rate at which radon atoms decay is also proportional to the number of radon atoms. Thus the total rate of change of the number of radon atoms per unit time due to 20 generation and decay is described by Eq. 3.7: dN Rn Rn N Rn Ra N Ra , dt (3.7) where: NRa Number of radium atoms; NRn Number of decaying radon atoms; λRa Radium decay constant (3.6× 10-12 s-1); λRn Radon decay constant (2.1×10-6 s-1). The first term on the right hand side of Eq. 3.7 describes the loss of radon due to decay and the second term describes the amount of radon atoms gained by generation from radium. The activity (number of atoms decaying per second) is calculated from the number of atoms and the decay constant. Hence, activity for radium and radon respectively are given by Eq. 3.8a and 3.8b. ARa Ra N Ra , (3.8a) ARn Rn N Rn , (3.8b) Where ARa and ARn is radium activity (Bq) and radon activity (Bq) respectively. The radon activity concentration is expressed as activity of radon per unit volume, while radium activity concentration is expressed as the activity per unit mass as given by Eq. 3.9a and 3.9b. C Rn ARn , V C Ra ARa , Ms (3.9a) (3.9b) 21 where CRn is radon activity concentration (Bqm-3), CRa is radium activity concentration (Bqkg-1), V is volume (m3) and ms is the mass of the sample (kg). The rate of change in radon activity concentration can be written as described in Eq.3.10. dC Rm C Rn b C Ra dt , (3.10) where 𝜌𝑏 is the bulk density (kgm-3). The decay constant of radium is not explicitly present in Eq. 3.10 as it is included in the radium activity concentration. Thus we get the following expressions for the decay and generation of radon: js = ηλRn ρb CRa , (3.11a) jb = βλRn , (3.11b) where β , is the partition corrected porosity. The Eq. 3.11a and 3.11b shows that the radium concentration, the partition corrected porosity, the emanation coefficient and the density of the sand are material properties required to describe the generation of radon in sand as a porous building material. 3.5.2 Radon transport in sand as a building material To gain insight on the mechanisms that play major roles in the transport of radon in sand as a building material, we considered the sand to be porous and isotropic. Two mechanisms were assumed to play a role; a) Radon can be transported due to differences in radon concentration (diffusive transport). This mode is considered one of the main processes for exhalation of radon atoms in sand as a building material from the walls in houses. 22 b) Radon can be transported by the flow of air (advective transport). Advection is not limited to exchange of air between open spaces but can also be the flow through porous media such as building sand (Fig. 3.4). Thus porous concrete fabricated from sand can act as sources of advective radon. Advective transport is also an important mechanism for entry of radon from soil to the crawl space and further to the living space. where ∆C= change in radon concentration and ∆P= change in Pressure Figure 3.4: Schematic representation of advective and diffusive transport of radon, respectively, in sand as a porous building material In this study diffusive transport of radon in sand as a building material will be considered important. To describe the diffusive transport of radon in porous sand we relate it to the diffusion transport in air. The transport of radon through air is described by Fick‟s law of diffusion as shown in Eq. 3.12. 𝑗 = −𝐷𝑚 𝛻𝐶𝑎 , (3.12) 23 where; 𝑗 is flux (Bqm-2s-1), Dm is molecular diffusion coefficient (m2s-1) and 𝛻𝐶𝑎 is radon concentration gradient (Bqm-4). The left hand side of Eq. 3.12 describes the amount of radon that is transported per surface area per unit time. The term on the right hand side gives the driving force, 𝛻𝐶𝑎 and the negative sign describe the effect of the driving force on the flux. The law assumes a mixture of ideal gases and very low radon concentration. For porous media like building sand the Eq. 3.12 is modified as given by Eq. 3.13. 𝑗𝑑,𝑎 = −𝐷𝑏 𝛻𝐶𝑎 (3.13) where; 𝑗𝑑,𝑎 is flux of radon as a result of diffusion in the air–phase (Bqm-2s-1) and Db is bulk diffusion coefficient of porous sand (m2s-1). It is assumed all pores in the sand are oriented in same direction as applied concentration gradient. 3.5.3 Estimation of radiation dose in dwellings In principle, it is possible to evaluate the indoor radon concentration provided the radon sources and airflows are given. In practice, this is not possible, due to many timedependent and unknown parameters. Thus we make many assumptions to simplify the description. Several models have been documented to describe the entry of radon in dwellings (Rodgers et al.,1991), but in this study we consider a model that aims at estimating the radiation dose in dwellings based on building plans rather than actual measurements. Thus the building plans can be adjusted to meet the radiation requirements prior to the building of the dwellings. In this model, the radiation dose in dwellings is considered to be the sum of contribution of gamma radiation and the contribution of alpha radiation from radon and its decay products. The assessment of the behavior of indoor radon will depend on the mass-balance between 24 the entry rate and the removal rate in living room. For a given entry rate, the accumulation of radon in a room will depend on the room volume, ventilation rate and inter-zone flows (Carmen,1992). 3.6 Radiation quantity and exposure units Ionizing radiation is measured in terms of the strength of the radiation source, energy of the radiation, level of radiation in the environment and the radiation dose or amount of radiation energy absorbed by the human body (Nemangwele, 2005). When ionising radiation interacts with human body, the body tissue absorb the radiation energy. The amount of energy absorbed per unit mass of tissue is known as absorbed dose. It is expressed in units called the Gray (Gy). One Gray is equivalent to one joule radiation energy absorbed per kilogram of tissue (Mudd, 2008). Equal doses of all types of ionising radiation are not equally harmful. In order to compare effects of radiation, an equivalent dose in unit of Sievert (Sv) is required which allows for differing biological effects of alpha, beta and gamma radiation (Allisy- Roberts, 2005). Dose equivalent (Sv) = Absorbed dose (Gy) × Radiation weighting factor (WR) 3.6.1 Radiation concentration The amount of radioactive material is expressed by mass or activity. The activity in Bequerrel (Bq) is the rate at which radioactive atoms decays per second. For radon, potential alpha energy concentration (PAEC) is expressed in Working Level (WL). Potential alpha energy concentration (PAEC) is a measure of the total alpha energy per 25 volume emmitted by a radon atom as it undergoes complete decay. A PAEC of 1 WL is approximately the PAEC of radon progeny in radioactive equilibrium with radon concentration of 3700 Bq/m3 (Nazaroff and Nero,1988). 26 CHAPTER FOUR MATERIALS AND METHODS 4.1 Materials and Equipment used in this study The following materials and equipment were used in this study: a) Garmin GPS supplied by Titan Avionics Limited, Nairobi. b) 1.0 Liter marinelli beakers manufactured by Nuclear Technology Services, Roswell. c) Metallic buckets and 1mm wire mesh sieve manufactured by Jua Kali artisans, Kakamega. d) Hot air oven manufactured by Omega Oven limited, Nairobi. e) 76mm×76mm Thallium activated Sodium Iodide [NaI(Tl)] detector manufactured by Oxford Instruments Inc. Tennessee. f) PCA-P software manufactured by Nuclear Measurements Group, Tennessee. g) Oxford win-MCA and Assayer Software version 3.80 manufactured by American Nuclear Systems, Inc. Ork Ridge. h) Microsoft professional C++ software supplied by Specicom Technologies, Nairobi. i) Standard IAEA reference Samples, preparation and certification of IAEA Gamma Spectrometry Reference material, Vienna. j) Dell D620 Computer laptop supplied by Stewan Computer Garage Limited, Nairobi. 27 4.2 Sample collection and preparation In this survey, the construction sand samples were collected along the main rivers in the old gold mining region of Kakamega county i.e. R. Yala and R. Isiukhu. The most suitable sampling approach that was employed involved a combination of grid sampling and systematic random sampling. The distance between neighboring grid centres was approximately 1 km. All sampling points were selected randomly within a particular grid. Figure 4.1 shows a map of the sampling sites. From the grids, 19 sampling positions S1S19 were randomly identified. A total of 38 construction sand samples were collected, two from each sampling site. The collected samples weight was approximately between 1.5 kg and 2.0 kg. The exact positions for the sampling sites were recorded using hand held Garmin GPS (Global Position System, model number 12). Each collected sand sample was crushed to fine powder, thoroughly mixed to ensure homogeneity and placed in a drying oven at a temperature of 110 0C for 24 hours to ensure that any significant moisture was removed. To obtain uniform particle sizes, a 1×1 mm meshed sieve was used. Accurate weights of 500±1 g of each sample was taken and stored in sealed plastic bags for four weeks prior to counting. This was meant for the samples to achieve a secular equilibrium between Radium-226 and its short lived decay products. 4.3 Radioactivity Measurements Radioactivity measurements in this work was done by a shielded 76mm × 76mm NaI(Tl) detector coupled to a computer based MCA. The detector was used to determine the 28 concentration of 226Ra, 232 Th and 40K in the construction sand samples. The detector was shielded by 15cm thick lead on all four sides and 10cm thick on top to reduce the gamma-ray background. Figure 4.1: A map showing the sampling sites in old gold mining region of Kakamega County. 29 The samples in sealed marinelli beakers were placed on the detector and counted for 30000 seconds. The same sample‟s and reference‟s geometry was used to determine the peak area to minimize uncertainties due to measurements (Turhan et al., 2008). Background counts were taken under the same conditions of sample measurements and subtracted in order to get net counts for the sample. At the end of the counting period, the spectrum recorded was displayed on the screen of the MCA with the horizontal axis representing the photon energy (channel number) while the vertical axis representing the photons recorded per channel (intensity). This gave the information regarding the type and the concentration of the radionuclide present in the sample. 4.3.1 Energy calibration in NaI (Tl) spectrometry The purpose of energy calibration of the NaI(Tl) gamma ray spectrometer was to obtain a relationship between peak position in the spectrum against the corresponding gamma ray energy. Energy calibration was done at the start of every measurement to cater for changes in weather, vibrations and heating up of the detector. Energy calibration involved measuring sources that emits gamma rays of known energy and comparing the measured peaks with energy. In this work, International Atomic Energy Agency (IAEA) certified reference materials ( a standard soil of known radioactivity, soil -6, Uranium ore sample, RGU1 and a thorium ore sample RGTh1) were used and calibration done in the energy range of 350 keV to 3000 keV. The following energy peaks were used: 214 Pb (1125 keV) and 214 214 Bi (609 keV), Bi (1765 keV) which correspond to uranium activity; 228 Ac 30 (911.2 keV), 208Tl (583 keV) and 208Tl (2615 keV) which correspond to thorium activity; and 40 K (1460 keV) which correspond to potassium activity. The peak positions were used to deduce the energy-channel relationship. The photon energy was represented as a function of channel number using a second order polynomial of the form shown in Eq. 4.1 (Debertin and Helmer, 1988); E E0 B(channel .no.) A(channel .no.) 2 , (4.1) Where A, B and E0 are constants. The polynomial was generated by Least Square fit to the calibration points using micro cal origin software. Figure 4.3 shows a graphical representation of the calibration parameters. The fit parameters are tabulated in Table 4.1. Table 4.1: The fit parameters of the polynomial used for calibration obtained by fitting a second order polynomial Fit parameter Fitted Value A -77.8614 B 3.50 E0 2.3715E-4 31 Figure 4.3: Energy calibration of the NaI (Tl) detector used Several spectra for all samples were recorded and stored. Figure 4.4 shows a sample spectrum curve for construction sand sample collected from Site S9 from old gold mining Tl -2615 keV 208 214 0.1 Bi -1765 keV K -1460 keV 40 Bi- 609 keV 214 0.2 228 Intensity (c/s) 0.3 Ac -911 keV zones of Kakamega County on the spectrometer. 0.0 500 1000 1500 2000 Energy (KeV) Figure 4.4: A gamma ray spectrum of construction sand sample 2500 3000 32 4.3.2 Determination of Gamma Activities In determination of the γ activities of the NORM in the samples, the focus was placed on the identification of three regions of interest (ROI) in the spectrum, which were centered on the three characteristic photo-peaks, at approximate 1460 keV (40K), 1765 keV (214Bi) and 2615 keV (208Tl). These were used to evaluate activity levels of 40K, 226Ra and 232Th series, respectively (Suresh et al, 2010). The process was as follows: i. Every sample was counted for 30,000s on a calibrated NaI(Tl) spectrometer and its spectrum recorded and stored in text files of a PC based MCA. ii. Average Background count was subtracted from the sample count to obtain the net count. (Two background readings were taken at the end of two weeks for 30,000s each). iii. The activity concentration of the sample was then calculated as explained in section 4.4. 4.3.3 Detector counting efficiency The performance of the detector was determined by relating the amount of radiation emitted by the source to the amount of radiation measured by the detector (Mustapha, 1999). The relationship is as shown in Eq. 4.2. 𝜀𝑖 = 𝐼𝑠 −𝐼𝑏 𝜌𝑐 𝑚 𝑠 , (4.2) where, 𝜀𝑖 is the efficiency of the detector corresponding to the radionuclide of interest in 33 RGMIX-2., Is is the intensity of the radionuclide of interest in RGMIX-2., Ib is the background intensity of the radionuclide of interest in distilled water, ρ is the photon emission probability of the radionuclide of interest in RGMIX-2. and ms is the mass of the sample RGMIX-2. The gamma lines emission probabilities ρ of the IAEA reference material RGMIX-2 used in equation 4.2 were as follows: ρ=0.11 at 1460 keV, 0.161 at 1765keV and 0.36 at 2615 keV (IAEA, 1992). The calculated efficiencies corresponding to the three radionuclides are given in the Table 4.2. Table 4.2: Efficiencies of emission of K-40, Th-232and Ra-226 in NaI(Tl) spectrometry Radionuclide Intensity of radionuclide of interest in RGMIX2, Is (c/s) K-40 U-238 Th-232 1.926 0.057 0.243 Background Is-Ib intensity of (c/s) radionuclide of interest in water, Ib(c/s) 1.066 0.860 0.018 0.039 0.115 0.128 Emission probability, (ρ) Concentration Efficiency, (Bq/kg) (ε) (10-3%) 0.110 0.161 0.360 5400 1260 1160 8 11 17 The measured efficiency values are in line with values obtained by other researchers (Knoll, 2000). Thus the detection efficiency was good. 4.2.4 Detection limits of the analytical system The detection limits of the detector were computed using the Eq. 4.3 (Mustapha, 1999); 34 LD 2.71 I 4.65 b ms i T T 1 , (4.3) where, T is the counting time (30000s) of the detector. Other symbols are defined by equation 4.2. The detection limits for 40K, 232Th and 226Ra were found to be 93.5 BqKg-1, 40.76 BqKg-1 and 33.86 BqKg-1 respectively. The detection limits are above the natural background activity concentration levels. 4.3.5 Energy Resolution of the detector The ability of the detector to distinguish two close lying photo peaks was determined by Gaussian fitting of radioactive ceasium-137 photo peak as shown in figure 4.5. The peak shape for the detector is usually a Gaussian distribution. 3 Measured spectrum Gaussian fitting Intensity (c/s) 2 1 0 550 600 650 700 750 800 Energy keV) Figure 4.5: Gaussian fitting of ceasium-137 spectrum measured in this work 35 The Gaussian model equation applied during fitting is shown by Eq. 4.4 2( x x0 ) y y0 exp w2 w 2 A 2 (4.4) where y0 is the base line offset, A is the area under curve, x0 is the centre of the peak and w is the width of the curve at half height. The fit parameters used are given in table 4.3. Table 4.3: The fit parameters for the Caesium- 137 photo-peak measured in this work Parameter Description Fitted value y0 Vertical shift of peak 0.03673±0.0042 xc Centroid of peak 661.67±0.1069 W Full width at half maximum 46.54±0.2454 A Area of the peak 134.588±0.7482 The detector resolution was 7.03% obtained from equation 4.5; R FWHM 100% , XC (4.5) where R is the resolution, FWHM is full width at a half maximum and Xc is the Caesium centroid peak energy. Wang (2003) reports the best resolution achievable to be 7% for the 662 keV gamma ray from Cs-137 for a 76mm×76mm NaI(Tl) detector which is in good agreement with the resolution determined in this work. 36 4.3.6 Gamma ray spectral data analysis The naturally occurring radionuclide 226 Ra, 232 Th and 40 K in the collected samples were detected and quantified by the method of comparison given in section 4.4. 4.3.7 Analysis of Certified Reference Materials (IAEA-RGK-1, RGTh-1 and RGU-1) For quality assurance in the measurement of radionuclide using NaI(Tl) detector, dispersion (Ai)disp of measured activity values (Ai)m from the certified values (Ai)c was calculated using Eq. 4.6 and recorded in table 4.4. Ai disp Ai m Ai c 100% Ai c (4.6) Table 4.4: Dispersion of measured activities from certified activities for (RGK-1, RGTh1 and RGU-1) RGU-1 RGTh-1 RGK-1 Measured value (Bq/kg) 5360 3379 12886 Certified value (Bq/kg) 4900 3280 13400 Dispersion (%) 9.39 3.02 -3.84 It was found out that the performance of the detector was good since the dispersion value was within ± 10 % as recommended by IAEA, 1987. 4.4 Activity Concentrations The specific activity for each detected radionuclide in the 232 Th and 226 Ra decay series 37 and 40K was determined using the Eq. 4.7. As .M s AR .M R , Is IR (4.7) where, AS is the activity of the radionuclide in the sample, MS, is the mass of the sample to be analyzed, IS is the intensity of the radionuclide in the sample to be analyzed, AR is the activity of the radionuclide in the reference sample, MR is the mass of the reference sample, IR is the intensity of the radionuclide in the reference sample. 4.5 Radiological parameters 4.5.1 Gamma dose rate The gamma dose rate (D) in the indoor air 1m above the ground was calculated using Eq. 4.8, (Faheem et al., 2008): 𝐷= 𝑥 𝐴𝑥 × 𝐶𝑥 , where Ax (Bqkg-1) is the mean activity of (4.8) 226 Ra, 232 Th or 40 K and Cx (nGyh-1/Bqkg-1) are the corresponding dose conversion coefficients which transform the specific activities into absorbed dose. The conversion factors with respect to building sand used in this study are 0.462, 0.604 and 0.0417 for 226Ra, 232Th and 40K respectively. These conversion coefficients were determined by Monte Carlo simulation assuming a standard room (4m×5m×2.8m) model (UNSCEAR 1993, 2000). In determination of the conversion coefficient; it is assumed that all the decay products of 226 Ra and 232Th are in radioactive 38 equilibrium. The published permissible dose rate is 55 nGyh-1 (UNSCEAR, 1993). 4.5.2 The Annual Effective Dose Rate (AEDR) In order to estimate the annual effective dose rate in air due to construction sand, the conversion coefficient from absorbed dose in air to effective dose received by an adult must be considered. This value is 0.7 SVGy-1 (UNSCEAR 1993, 2000) for environmental exposure to gamma rays of moderate energy. For indoor measurements, the occupancy factor of 0.8 is considered. Thus the annual effective dose rate equivalence in this work was calculated using Eq. 4.9 below. 𝐴𝐸𝐷𝑅 𝑚𝑆𝑣 𝑦 = 𝐷( 𝑛𝐺𝑦 ℎ ℎ 𝑆𝑣 ) × 8760(𝑦 ) × 0.8 × 0.7(𝐺𝑦 ) × 10−6 (4.9) The world average AEDE from outdoor or indoor terrestrial gamma ray radiation is 0.460 µSv/y. 4.5.3 Radium Equivalent Activity Radium equivalent activity (Raeq) was used to assess hazards associated with construction sand since it was found to contain assuming that 370 Bq/kg of 226 226 Ra, 232 Th and Ra, or 260 Bq/kg of 40 K in Bq/kg. It was determined by 232 Th or 4810 Bq/kg of 40 K produce same gamma dose rate. The Radium equivalent activities, Raeq in Bq/kg in sand samples were calculated using Eq. 4.10: 39 Raeq = AK × 0.0077 + ARa + (ATh × 1.43), (4.10) where 𝐴𝐾 , 𝐴𝑅𝑎 and 𝐴𝑇ℎ are activity concentration for 40K, 226Ra and 232Th respectively. Maximal admissible Raeq is 370 Bq/kg to keep the external dose below 1.5 mSvy-1. 4.5.4 External hazard index (Hex) To limit the radiation dose to permissible dose equivalent limit of 1 mSvy-1, the external hazard index (Hex) was calculated using Eq. 4.11: H ex ARa ATh A K 1 370 259 4810 (4.11) The Eq. 4.11 is obtained from the expression for radium equivalent activity through the supposition that its maximum allowed value corresponds to the upper limit of radium equivalent activity (370 BqKg-1) so that the external annual dose rate does not exceed 1.5 mGy (Tufail et al., 2007). 4.5.5 Gamma Index (Iγ) Gamma index is a criterion for assessment of the radiological suitability of a building material. It has been defined by European Commission (EC, 1999) as; I ARa ATh A K , 300 200 3000 (4.12) 40 Values of index Iγ ≤2 corresponds to a dose rate criterion of 0.3 mSvy-1, whereas 2<Iγ≤6 corresponds to a dose rate criterion of 1 mSvy-1 (Anjos et al., 2005). 4.6 Modeling of radon diffusion fluxes in a room 4.6.1 Theory of modeling Modeling is a method of describing and simplifying a process that one tries to understand (Paul et al., 2008). The model proposed in this work is used to estimate and predict the concentration of indoor radon emitted from the walls in dwellings constructed from sand. This will assist in the formulation of effective control strategies to reduce emission of indoor radon. This model assumes that; i. Radon is not released from materials inside the room, ii. radon is homogeneously mixed with room air, iii. and it does not react with any substance or disappear by any process other than physical decay. In this study, finite difference numerical methods are employed to solve equations that govern the transport of radon in a room. Due to the complex nature of the model, a computer code was developed to solve the equations using numerical methods. Numerical methods yield approximate solution to the governing equation through discretisation of space and time (Munene, 2007). Numerical models can relax the rigid idealized conditions of analytic models; hence they are more realistic for simulating field conditions. In this model, radon concentration values are mapped on a fixed grid as will be described latter in section 5.2. The finite difference numerical method is applied to calculate the 41 concentration variation over time and in space. The finite difference method is based on the principle that any complex function [f(x)] can be approximated with a simple linear function for a small increment of independent variable (x) which could be space or time. There are three categories of finite difference numerical methods i.e. explicit, implicit and Crank-Nicholson method. In this work explicit finite difference method was used since it has the advantage of calculating the concentration at grid i at time t+∆t, using only known concentration at time t. The numerical schemes for solving the transport equation were to meet convergence conditions, correctly model the conservation, dissipation and dispersion properties of the governing equations (Celia et al., 1990). 4.6.2 The governing equations In this model the concentration of indoor radon, C at time t and space r = (x,y) in a room is calculated by solving the transport expression given by Eq. 4.13. The equation describes the change in radon concentration due to creation, decay, ventilation and diffusion; i.e. it takes into account the formation of new radon atoms as well as removal due to decay, ventilation and diffusion during the transport process. Radon diffusion occurs when radon atoms migrate due to concentration gradients as is described by Fick‟s law, which relates the concentration gradient to the flux. C S q Rn C v (C C0 ) t V V , (4.13) where C is the concentration of radon (Bqm-3), the first term on the right-hand side 42 represents the source, second represents the decay, third represents advection and the last term represents diffusion. There are two main processes that govern radon transport in living space of buildings i.e. diffusion and advection. Advection is not considered in this study, its role depends on pressure changes that tend to average out for a closed room (Speelman et al., 2009). Thus the transport equation reduces to Eq. 4.14 shown below; C S q Rn C t V V , (4.14) The explicit finite difference method is used to solve Eq. 4.14. In difference form, the Eq. 4.14 is transformed to Eq. 4.15. 𝑆 𝐷 𝐶𝑗𝑛+1 = 𝐶𝑗𝑛 + 𝑉 ∆𝑡 − 𝜆𝑅𝑛 ∆𝑡𝐶𝑗𝑛 + 𝑉 ∆𝑡 𝐶𝑗𝑛+1 −2𝐶𝑗𝑛 +𝐶𝑗𝑛−1 (∆𝑥)2 , (4.15) where indexes j and n refer to the discrete position and times determined by step lengths ∆x and ∆t for the coordinates x and time t respectively. Using a small enough value of ∆t and ∆x, the truncation error can be reduced until the accuracy achieved is within the error tolerance (Andersen, 1995). To compute the numerical solution of Eq. 4.15 a computer code was developed in which all the parameters had to be transferred to the code in a manner that it would recognize each and every part of the equations to be used (Ambusso, 2007). 43 4.6.3 Program Structure The computer program that simulates the radon transport in a room has the following parts; the data that defines the physical properties of the room and the source, the procedures or codes that process the data and the results that indicate the changes that have taken place in the room. The main parts of the program are represented by the schematic chart shown in figure 4.6. Figure 4.6: Schematic chart showing the main parts of the program 44 4.7 Estimation of uncertainties One of the main aim of this study is to determine the activity concentration of 232 Th (and their decay progeny) and 40 226 Ra, K in building sand from old gold mining belt of Kakamega County. The activity concentration are deduced indirectly by the comparison method, as discussed in section 4.4. The uncertainties of the parameters in the determination of activity concentration by comparisson method can be statistical (random) or systematical. The uncertainty, u, characterizes the range around the final value x where the unknown true value is expected to lie, usually written as x ±u. Identifying sources of uncerntaity in gamma ray spectrometry involving the sand samples in this study is an essential step for determining high quality results. The sources of uncertainty can be classified according to their origin as shown in figure 4.7. Some of the uncertainties are quantifiable before the start of the measurements such as uncertainties due to nuclear data or energy and efficiency calibrations. While others are quantified directly from the measurements. Sources of uncertainty Sample preparation Energy and efficiency calibration Measurement of test samples Nuclear data Figure 4.7: Possible uncertainties that could be considered in determination of activity concentrations of 226Ra and 232Th (and their progeny) and 40K in sand samples 45 4.7.1 Uncertainty due to sample preparation During sand preparation process, the sand samples were dried and sieved in order to achieve uniform distribution of radionuclides and then stored in air/gas tight containers. One source of uncertainty in such case is the mass of the sample. This was estimated from the precision of weighing balance used (±0.01g). 4.7.2 Uncertainty due to Efficiency calibration Efficiency calibration was aimed at deriving a relationship between absolute full energy peak efficiency of gamma ray spectroscopy system and the energy (Huda Al- Sulaiti, 2011). The uncertainty associated with the number of counts in peaks; along with the uncertainty in the nuclear data contribute to the combined uncertainty of the efficiency calibration. 4.7.3 Uncertainty due to measurement of samples The most important uncertainties in the final combined uncertainty are those originating from measurements. These uncertainties may arise due; to differences in counting geometries of the samples and standards, random coincides, decay time effects, dead time effects and due to counting statistics. In summary, the activity concentration distribution of 226 Ra, 232Th and 40K in the earth‟s crust is variable and the same applies to the sand samples drawn in the study region. In this study, γ-ray activities due to 226 Ra, 232 Th and 40 K were measured in building sand samples. This involved crushing, drying and sealing of samples in marinnelli beakers. The samples together with standard samples obtained from IAEA were stored for more 46 than four weeks to achieve secular equilibrium between 226 Ra and its short lived decay products. The activity measurements were performed using PC based NaI(Tl) gamma ray spectrometer. The detector was shielded to reduce the background. The combined uncertainty of the activity concentrations was calculated by applying Gauss error propagation law. The proposed model was meant to predict the transport and distribution of indoor radon in living rooms in the study region. This was accomplished by solving the transport equation using explicit finite difference numerical method. 47 CHAPTER FIVE RESULTS AND DISCUSSION 5.1 Radioactivity concentration of building sand The building sand used to construct houses/buildings in the study area was assumed to come from various streams in the region. The two main sources of sand deposits along the river banks are Rivers Yala and Isiukhu. The specific gamma ray activity concentrations of radionuclide 40K, 226 Ra and 232 Th were calculated in Bq/kg by method of comparison and recorded in Table 5.1. The minimum activities of 226Ra, 232Th and 40K recorded were 36.79±5.89 Bq/kg, 51.12±2.56 Bq/kg and 322.38±16.12 Bq/kg and the maximum values were 185.21±5.89 Bq/kg, 158.92±7.95 Bq/kg and 960.53±48.03 Bq/kg. The average concentrations of 226 Ra, 232 Th and 40K in samples were 128.05±8.89 Bq/kg, 98.37±6.41 Bq/kg and 756.39±35.99 Bq/kg respectively. It is observed that the activity concentrations are above the world‟s accepted average values of 33 Bq/kg for 226 Ra, 45 Bq/kg for 232Th and 420Bq/kg for 40K as reported in UNSCEAR (2000). A summary of the activity concentration in sands from old gold mining zones of Kakamega County compared with other parts of the world are presented in Table 5.2. These high levels of natural radionuclide concentration in this region might have resulted from artisanal gold mining. During gold mining concealed radioactive rich igneous rocks, sand stones, monazites and quartzite are exposed to the agents of weathering and dispersed in the region. Gold extraction processes might have enhanced the transport of Uranium and thorium minerals as sediments in river beds. The continuous application of phosphate fertilizers in the sugar cane, tea and maize plantations as TENORM has also 48 contributed to the high concentration levels in some parts of the old gold mining zones (Sangura, 2012). The uncertainties in the specific activities of individual samples in Table 5.1 include uncertainties in gamma emission probability, detector efficiency, peak area and sample weight (Malik et al., 2011). Table 5.1: Mean Specific γ –ray activity of 226Ra, 232Th and 40K in the sand samples (n=2) SITE LOCATION LATITUDE LONGITUDE 226 232 40 S1 Shikhombelo 0.24223 34.70618 121.02±6.05 97.27±4.86 879.86±43.99 S2 Mukhonje 0.25406 34.72791 185.21±9.26 80.48±4.02 960.53±48.03 S3 Shieywe 0.27461 34.77672 107.92±5.40 87.28±4.36 812.68±40.63 S4 Mwibatsilu 0.24204 34.65198 89.45±4.47 62.53±3.13 821.89±41.10 S5 Kakamega 0.25396 34.75005 74.05±3.70 89.92±4.50 753.77±37.69 S6 Ematsayi 0.27671 34.62762 150.45±7.52 51.12±2.56 815.86±40.79 S7 Esalasala 0.29726 34.67118 155.29±7.76 95.05±4.75 322.38±16.12 S8 Eshibakala 0.26686 34.63300 36.76±1.84 82.11±4.11 760.00±38.00 S9 Imbale 0.22936 34.64335 163.38±8.17 75.90±3.70 696.11±34.81 S10 Mukulusu 0.29210 34.82379 118.48±5.92 96.15±4.81 485.36±24.29 S11 Shirulu 0.17712 34.79537 177.17±8.86 92.12±4.61 618.78±30.94 S12 Litambiza 0.16035 34.74432 138.02±6.90 84.90±4.25 877.98±43.90 S13 Shikokho 0.16993 34.71121 183.87±9.91 91.32±4.57 854.26±42.71 S14 Mwitabakha 0.16528 34.72227 99.98±5.00 100.69±5.03 648.13±32.41 S15 Lwanungu 0.17364 34.78089 115.10±5.76 158.92±7.95 725.21±36.26 S16 Isulu 0.17091 34.69703 108.55±5.43 142.28±7.11 778.95±38.95 S17 Bushiangala 0.16877 34.67945 113.26±5.66 147.15±7.36 762.68±38.13 S18 Ikonjero 0.15966 34.64159 143.14±7.46 105.15±5.26 914.99±45.75 S19 Iguhu 0.16097 34.74722 151.80±7.68 128.76±6.44 881.32±44.07 Maximum 185.21±5.89 158.92±7.95 960.53±48.03 Minimum 36.79±2.03 51.12±2.56 322.38±16.12 Average 128.05±8.89 98.37±6.41 756.39±35.99 Ra (Bq/kg) Th (Bq/kg) K (Bq/kg) 49 Table 5.2: Average activity concentration of radionuclide in sand from old gold mining zones of Kakamega County compared to other parts of the world Country 226 Ra (Bqkg-1) 232 Th (Bqkg-1) 40 K (Bqkg-1) References Turkey 44 26 441 Cervic et al.,2009 Netherlands 8 11 200 Ackers et al.,1985 India 44 64 456 Kumar et al.,1999 China 23 36 891 Xinnwei and xiaolan, 2008 Zambia 24 26 714 Hayumbu et al.,1995 Kenya 11 5 802 Mustapha et al., 1999 Present study 128 98 756 Figure 5.1 shows the specific activities distribution of 226 Ra, 232 Th, 40 K and Raeq in all the sampling sites in the study area. From figure 5.1, highest concentration values of 226 Ra, 232 Th and 40 K were reported from sites S13, S15 and S2 respectively. This is attributed to presence of radioactive rich igneous bed rocks in the region. Gold mining, an economic activity common in this region, has enhanced the breakdown and dispersal of these rocks as sand sediments. The highest concentration value of 40 K recorded was at site S2. This was attributed to continuous application of fertilizers rich in potassium in tea plantations along the slopes of River Isiukhu. 50 Ra-226 Th-232 K-40 Ra(eq) Activity Concentration (Bq/kg) 1000 800 756.39 600 400 321.67 200 128.05 98.37 0 S2 S4 S6 S8 S10 S12 S14 S16 S18 Sampling Sites Figure 5.1: Activity concentration and radium equivalent activity distribution in all the sampling sites 5.1.1 Exposure due to gamma radiation The distribution of 226Ra, 232Th and 40K is not uniform in the sand samples, thus Radium equivalent activity (Raeq) was introduced, which represents weighted sum of specific activities of 226 Ra, 232 Th and 40 K. Exposure due to gamma radiation in terms of Radium equivalent activity originating from building sand in the study region was calculated and 51 the results obtained are shown in Table 5.3. Based on finding in table 5.3, the Radium equivalent activity in the studied samples ranged from 121.43 Bq/kg at sampling site S5 (Kakamega) to 397.62 Bq/kg at sampling site S19 (Iguhu) with a mean value of 321.67±12.4 Bq/kg. The indoor dose rates ranged from 99.6 nGyh-1 to 186.84 nGh-1 with a mean value of 151.76±5.65 nGh-1. The calculated values for annual effective dose in the present study ranged from 0.488 mSvy-1 to 0.916 mSvy-1. The mean value was found to be 0.744±0.02mSvy-1. For comparison purposes, data published by other researchers for some regions is given in table 5.4. From table 5.3, the average radium equivalent activity obtained is lower than the recommended limit of 370 Bqkg-1 although this value is higher than the values reported in other regions. Table 5.3: Radium equivalent activity, external hazard index, dose rate and annual effective dose for sand samples in this work Site no. Raeq(Bqkg-1) Dose Rate (nGyh-1) S1 S2 S3 S4 S5 S6 S7 S8 S9 S10 S11 S12 S13 S14 S15 S16 S17 S18 S19 321.71 367.53 289.62 236.40 121.43 280.66 313.78 207.37 320.64 289.94 352.21 320.88 374.25 289.33 393.12 366.53 377.07 357.55 397.62 Maximum Minimum Mean 397.62 121.43 321.67±12.4 152.95 175.47 137.88 114.31 119.95 135.13 144.31 99.60 151.58 134.73 162.86 153.00 177.20 135.75 182.20 171.03 175.57 169.51 186.83 Annual Effective Dose (mSvy-1) 0.75 0.86 0.68 0.56 0.74 0.66 0.71 0.49 0.74 0.66 0.81 0.75 0.86 0.67 0.89 0.83 0.86 0.83 0.92 External Hazard index 0.88 1.01 0.79 0.65 0.70 0.77 0.85 0.57 0.87 0.79 0.96 0.88 1.02 0.79 1.07 1.00 1.03 0.98 1.09 186.84 99.6 151.76±5.65 0.92 0.48 0.74±0.02 1.09 0.57 0.88±0.03 52 Table 5.4: Comparison between the radium equivalent activities, indoor gamma dose rates and annual effective dose in the present study and those reported in other countries Country Turkey Radium Equivalent activities Dose in air Annual effective Dose (Raeq) Bq/kg (nGyh-1) (mSvy-1) 112 104 0.51 (Cervic et al. ,2009) Northern Pakistan 143.8 0.20 (Malik et al., 2011) ------- Kenya 66 0.24 152 0.74 (Mustapha et al., 1997) ------ This study 321.7 5.1.2 External hazard index (Hex) The calculated values of external hazard index (Hex) for the sand samples in this study ranged from 0.57 to 1.09 with a mean value of 0.883±0.03 as shown in table 5.5. This average value is lower than unity; therefore, according to European Commission on Radiation Protection report (1999), sand from old gold mining zones in Kakamega County is safe and can be used as construction material without posing any significant radiological threat to the general public. 5.1.3 Gamma Index (Iγ) From the indices calculated, it was found that none of the sand from the study region posed significant exposure hazard as shown in table 5.5. The gamma index was estimated using Eq. 4.12. The distribution of values of the gamma index for mineral sand analyzed 53 in this work is presented in table 5.5. The scatter plot of external hazard index and gamma index as shown in figure 5.2 indicates that the sand from site S8 have the least risk of the exposure hazard while sand from site S19 has the highest. The entire values of indexes Iγ are < 2.0. Therefore, the annual effective dose delivered by the building made of such sand is smaller than the annual effective dose constraint of 0.3 mSv, hence the sand can be exempted from all restrictions concerning radioactivity (Tufail et al., 2007). Table 5.5: The hazard indices of the sand samples collected from old gold mining zones of Kakamega Sampling sites S1 S2 S3 S4 S5 S6 S7 S8 S9 S10 S11 S12 S13 S14 S15 S16 S17 S18 S19 Maximum Minimum Mean Raeq (Bq/kg) 321.71 367.53 289.62 236.40 121.43 280.66 313.78 207.38 320.65 289.95 352.22 320.89 374.26 289.34 393.12 366.54 377.07 357.55 397.62 397.62 207.38 321.67±12.4 Hazard indices External hazard (Hex) 0.88560 1.01099 0.79762 0.65406 0.70371 0.77361 0.85371 0.57438 0.87934 0.79236 0.96316 0.88336 1.02713 0.79373 1.07544 1.00467 1.03282 0.98308 1.09064 1.0906 0.5744 0.883±0.03 Gamma index (Iγ) 1.183 1.340 1.067 0.885 0.948 1.029 1.100 0.786 1.156 1.037 1.257 1.177 1.354 1.053 1.420 1.333 1.368 1.308 1.444 1.44 0.79 1.17±0.19 54 external hazard index Gamma index 1.6 1.5 1.4 Hazard indices 1.3 1.2 1.1 1.0 0.9 0.8 0.7 0.6 0.5 0 2 4 6 8 10 12 14 16 18 20 Sampling sites Figure 5.2: A scatter plot of the external hazard indexes and gamma hazard indexes for different sampling sites in this study 5.1.4 Statistical analysis of 226Ra, 232Th and 40K in this study The activity concentrations of 226 Ra, 232 Th and 40 K in this study were compared using Statistical Product and Service Solution (SPSS) computer software (version 11.5) for the determination of ordinary statistics. The computed statistics are shown in table 5.6. From the table, the positive value of the skewness coefficient for 232 Th indicates that its distribution is asymmetric with right tail longer than the left tail. However, the low kurtosis coefficient for 226 Ra suggests that the distribution is close to normal. According to Taylor (1990), the distribution of 226Ra, 232Th and 40K is within the normal distribution limits as shown in table 5.7. 55 Table 5.6: Statistical summary of radionuclide in this work 226 232 Ra 40 Th K Mean conc. (Bqkg-1) 128.05 98.37 756.35 Standard deviation 38.74 27.92 154.68 Skewness coefficient -0.478 0.778 -1.443 Kurtosis coefficient 0.220 0.356 0.469 Table 5.7: Limits for kurtosis for normal distribution (Taylor, 1990) Size of the sample 5% 1% 5 -1.058-1.058 -1.342-1.342 10 -0.950-0.950 -1.397-1.397 15 -0.862-0.862 -1.275-1.275 20 -0.777-0.777 -1.152-1.152 25 -0.771-0.771 -1.061-1.061 30 -0.661-0.661 -0.982-0.982 35 -0.621-0.621 -0.921-0.921 40 -0.587-0.587 -0.869-0.869 45 -0.558-0.558 -0.825-0.825 50 -0.533-0.533 -0.787-0.787 100 -0.389-0.389 -0.567-0.567 200 -0.280-0.280 -0.403-0.403 1000 -0.127-0.127 -0.180-0.180 5000 -0.057-0.057 -0.081-0.081 56 Table 5.8: Limits of skewness factor for normal distribution (Taylor, 1990) Size of sample 5% 1% 200 -0.49-0.57 -0.63-0.98 400 -0.36-0.41 -0.48-0.67 600 -0.30-0.34 -0.40-0.54 800 -0.26-0.29 -0.35-0.46 1000 -0.24-0.26 -0.32-0.41 5.2 Indoor radon Model Results The model room was divided into discrete blocks of equal dimensions during the gridding process as shown in figure 5.3. The blocks dimensions can be varied. The program then distributes the radon emitted from a source within a room to all the blocks depending on prevailing conditions. Before radon was exhaled, the concentration in all the blocks including the source equal to zero. However, within the first 150 hours the concentration in the room rose to 9 Bq/m3. As the time increased more radon was exhaled into neighboring blocks as shown by the different build up curves for exhaling source block (Fig. 4). From the curves, the radon atoms exhaled from the walls (sources) in a model room increases exponentially until radioactive secular equilibrium is reached. 57 49 50 51 52 53 54 55 42 43 44 45 46 47 48 35 36 37 38 39 40 41 28 29 30 31 32 33 34 21 22 23 24 25 26 27 14 15 16 17 18 19 20 7 8 9 10 11 12 13 0 1 2 3 4 5 6 Figure 5.3: Two dimensional gridding of the model room The exhalation rate E0 from the source is described by Eq. 5.1: E0 C V , S (1 e t ) (5.1) where C is net concentration (Bq/m3), λ is decay constant (h-1), V is effective air volume (m3) and S is source surface area (m2). 58 14 12 Leakage Activity 10 Curve 3 Curve 2 Curve 1 Leakage and backdiffusion 8 6 4 2 0 0 2000 4000 6000 8000 10000 Growth Time Figure 5.4: Different build up curves for the exhaling source block The above equation is valid if there is no leakage of radon into or out of the walls, and if there is no back diffusion effect. If there is leakage and back diffusion, the decay constant is modified by replacing it with an effective decay constant (λeff). The resulting effective decay constant is described by Eq. 5.2. λeff =λ+λa+λb, (5.2) where λa and λb are leakage and back diffusion time decay constants. Thus if the exhalation is depressed due to back diffusion and/or leakage, the equilibrium value will be lower than the maximum expected as depicted by curve 1 and curve 2 of figure 5.4. 59 Figure 5.5 show radon concentration profiles in the blocks assuming that the radon atoms diffused into the room without undergoing radioactive decay. From the profiles, blocks that are adjacent to the source (any block on the periphery, for instance block 55) receive radon atoms radially and symmetrically by diffusion; hence have high peak concentration in the build up phase. 0.05 0.045 0.04 Radon COnc, (kBq/m3) 0.035 0.03 NDBlnum10 0.025 NDBlnum24 0.02 NDBlnum38 0.015 NDBlnum44 0.01 0.005 0 -0.005 0 1000 2000 3000 4000 5000 6000 Time (minutes) Figure 5.5: Radon concentration profiles in the blocks (diffusion only) From figure 5.5, during the build up phase, blocks that are further away from the source have a lower peak radon concentration than those that are adjacent. This process is similar to a chemical diffusion; radon atoms migrate from the source due to concentration 60 gradient without loss until the room achieves uniform concentration (36 Bq/m3). The peak concentration in the blocks widens and flattens as the blocks distance increases further from the source. This is attributed to increase in mixing of radon atoms with air molecules as the distance and time increases which results in dilution of radon „puff‟ as it moves away from the source. The sharpness and the value of the peaks decrease further away from the source block because the front blocks are receiving the radon atoms from most of the blocks behind them. The peaks in the profiles results from blocks receiving more radon atoms than they are losing but this changes after sometime when they lose more radon than they receive. After build up phase, the radon concentration in the blocks diminishes slowly with time and in all profiles the concentration converges at same equilibrium concentration (36Bq/m3) at late time. This shows that with time the concentration becomes uniform throughout the room. This confirms that diffusion process dominates. Similar observations are noted when radon gas from the source decay as it is transported in the room space except the equilibrium concentration in the room is greatly reduced (5.46Bq/m3) and the sharpness of the peaks in the profiles is increased. This is because decay involves loss of radon atoms. Thus, the rate at which the blocks loose radon atoms is higher than in the previous case. In this case, the radon concentration within a block starts from zero to a maximum value and then reduces to equilibrium concentration at late times. Figures 5.6 and 5.7 illustrate these features in the concentration profiles. 61 0.04 0.035 Radon COnc, (kBq/m3) 0.03 0.025 Blnum10 0.02 Blnum24 0.015 Blnum38 0.01 Blnum44 0.005 0 -0.005 0 1000 2000 3000 4000 5000 6000 Time (minutes) Figure 5.6: Radon concentration profiles in the blocks (diffusion with decay) 0.05 0.045 Radon COnc, (kBq/m3) 0.04 0.035 Blnum10 0.03 Blnum24 Blnum38 0.025 Blnum44 0.02 NDBlnum10 0.015 NDBlnum24 0.01 NDBlnum38 0.005 NDBlnum44 0 -0.005 0 1000 2000 3000 4000 5000 6000 Time (minutes) Figure 5.7: A comparison of concentration profiles in blocks where radon diffuses with and without decay 62 5.3 Model validation For the purpose of validating the model, the indoor radon concentrations measured at some selected classrooms (monitoring stations) were used for comparison with the model data. The field data measurements for indoor radon were carried out using activated charcoal canisters, US Environmental Protection Agency (EPA) type. Measurements were taken for a period of 2-5 days in a week. After the exposure, the cans were sealed and reweighed. The gamma rays emitted by 214Pb (295 and 352 keV) and 214Bi (609 keV) following the attainment of secular equilibrium between radon and its short lived decay products were counted on a 76mmx76mm NaI(Tl) detector. Figure 5.8 shows a comparison of the measured and modeled radon concentration in this work. In general the model underestimated all the concentrations compared to measured values when using charcoal canister (EPA). This can be attributed to a number of factors. The most significant factor was that the model did not include other sources of radon such as radon entry from the soil and the flooring material. These local sources contribute a significant portion of radon in the indoor atmosphere. Despite the disparity between the measured and modeled values, the model reproduced the general trends associated with diffused radon fluxes as illustrated by figure 5.9. Therefore, the proposed model can serve as a tool for predicting indoor radon concentration in projects that require the assessment of impact of radiological pollution. 63 45 Radon conc. [Bq/m3] 40 35 30 25 20 modeled 15 measured 10 5 0 1 2 3 monitoring stations Figure 5.8: A comparison of measured and modeled radon concentration Figure 5.9: Radon growth curve obtained by fitting measured radon concentration for monitoring station 1. 64 In summary, the suitability of a material to be used for building purposes is evaluated basing on the radium equivalent activity and hazard indices. In this study, the average value of radium equivalent activity in the sand samples is less than the limited value of 370 BqKg-1. The external hazard indices determined in this work are less than unity. Therefore, it can be concluded that building sand sampled do not pose a major source of radiation hazard. A predictive model has been developed for estimation of indoor radon diffusion fluxes in living rooms in the study region. The modeled radon concentrations are in good agreement with the measured values using activated charcoal canisters. 65 CHAPTER SIX CONCLUSIONS AND RECOMMENDATIONS 6.1 Conclusions Activity levels of natural radionuclide of uranium, thorium and potassium in construction sand sampled from old gold mining zones of Kakamega County, a suspected High Background Radiation Area (HBRA), was measured using NaI (Tl) gamma ray spectrometry. The radiological effects on humans due the natural radiations from sand were also estimated by use of radiological parameters. The measured mean activity concentration levels of 226 Ra, 232 Th and 40 K was found to be 128.05±8.89 Bqkg-1, 98.37±6.41 Bqkg-1 and 756.39±35.99 Bqkg-1 respectively. These levels were found to be higher than worldwide accepted average values of 33, 45 and 420 Bqkg-1 for 226Ra, 232Th and 40K respectively. The activity levels in NORM in this region are high due to artisanal gold mining. The mining activities have been found to influence the activity concentration of radionuclide in sand due to the introduction and interaction of rocks from different profiles to the earth surface. The calculated hazard indices: radium equivalent activity and external hazard was found to range from (207.38 to 397.62) Bqkg-1 and 0.57-1.09 respectively. This indicates that construction sand from old gold mining zone are fit to be used as building material and so do not pose any risk to the inhabitants in terms of the acceptable limits. The indoor absorbed dose rate ranged from (99.6- 186.84) nGyh-1 which is above the world average of 60 nGyh-1 (UNSCEAR, 2008). The effective dose rate for the indoor radiation ranged from (0.48-0.92) mSvy-1. These values are above the world average 0.07 mSvy-1, 66 however all the indoor dose rates are below the accepted limit of 1 mSvy-1. A deterministic model was developed using the mass conservation law, taking into account diffusion, sources and sinks (decay) of radon atoms in indoor air. Differential equations that govern the transport of radon were set up; discretized and solved numerically using developed computer codes. Experimental data for indoor radon concentration measurement using passive detectors was obtained and compared with simulated results. The simulations show that with some modifications, the model can be used by policy makers to pass legislations on the quality of indoor air in terms of radon concentration. 6.2 Recommendations Other than building sand, there are several natural and artificial building materials that may contribute to radiation exposure. These include bricks, cement, clay paints, ballast and stones. Thus it is essential to assess the contribution of each of these building materials to external and internal dose rate to minimize the risk of exposure to high doses to the occupants in the dwellings. To avoid risks of prolonged exposure to indoor radon in this region, people are advised to ventilate their houses properly, not to build residential houses on mining tailings, and seal the walls and floors well to prevent radon entry into the living room from soil, building materials and to spend little time indoors as compared to outdoors. 67 An epidemiological study on effects of radiation on the artisanal gold miners is also recommended. This will help to ascertain the percentage of miners who are likely to suffer from cancer related diseases. The transport equation with advection term should be solved implicitly and in three dimensions to eliminate the instability problem during the simulations. 68 REFERENCES Ackers J.G, den Boer J.F, de Jong P and Wolfschrijin N. 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(2005): Radioactivity concentrations in soils of Xia Zhuang granite area, China; Journal of Applied Radiation and Isotopes, 63: 255-259. 74 APPENDICES APPENDIX I Comparison of International Radon Action Levels (European Commission, 1998) International Radon Action Levels Existing Dwellings (Bq/m3) New Buildings (Bq/m3) EU 400 200 ICRP 200-600 WHO 800 200 Canada 800 800 Finland 400 200 Czech Republic 400 200 Germany 250 250 Ireland 200 200 Norway 400 200 Sweden 400 200 SpainSwitzerland 400 185 United Kingdom 1000 400 200 200 1 APPENDIX II 222 Rn Decay series (Dumont et al., 1988) Decay by product Half-life 222 Alpha particle 3.82 days 218 Alpha particle 3.05 minutes 214 Beta particle and gamma radiation 26.8 minutes 214 Beta particle and gamma radiation 19.7 minutes 214 Alpha particle 0.000003 minutes Rn Po Pb Bi Po 1
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