Journal of Radiation Research and Applied Sciences xxx (2016) 1e14

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Journal of Radiation Research and Applied Sciences

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Distribution of natural radionuclides and assessment of the associated hazards in the environment of -Shalateen area, coast,

* A.A. Arafat a, , M.H.M. Salama a, S.A. El-Sayed a, A.A. Elfeel b a Nuclear and Radiological Regulatory Authority, Egypt b Mineral Resources Authority, Egypt article info abstract

Article history: Radiological aspects of water, soil and shore sediments resources in Marsa Alam-Shalateen area, Red Sea Received 4 October 2016 coast, Egypt, were investigated with the aim of presenting background about the radiological levels and Received in revised form assessing the associated hazards. The results of study are intended to support the governmental au- 26 November 2016 thorities as regards the future-natural resources management. Sixty nine environmental samples (30 Accepted 29 November 2016 water, 33 soil and 6 shore sediments samples) were collected in 2015 and analyzed for Ra-226 (U-238) Available online xxx series, Th-232 series, K-40 and Cs-137 radionuclides using Hyper-Pure Germanium (HPGe) detector. For all samples, the activity concentrations of Cs-137 radionuclide are under the detection limit of the used Keywords: Water analytical procedures. As regards the water resources, the Th-232 activity concentrations in the major Soil part of water samples were under the detection limit. The Ra-226 activity concentrations ranged from 1 1 Shore sediment <0.7 to 7.6 Bq L and from <0.7 to 6.31 Bq L for groundwater and sea water samples, respectively. All Ra-226 the desalinized water and 50% from wastewaters were clear of Ra-226 activity concentration. The K-40 Th-232 ranged from <3 to 32.84 Bq L 1, from <3 to 38.17 Bq L 1, from <3 to 54.31 Bq L 1 and from <3to K-40 40.91 Bq L 1 for groundwater, sea water, desalinized water and wastewater samples, respectively. Cs-137 Radiologically, all fresh waters, safe for drinking except Al Gaheliya well showed Ra-226 activity con- Hazard indices centration higher than the guidance level recommended by the WHO. For soil cover, the average activity concentrations of Ra-226, Th-232 and K-40 of the carbonaceous soil samples were 18.45, 16.78, and 334.35 Bq kg 1, respectively. While for the siliceous soil samples, they were 10.24, 8.68 and 234.47 Bq kg 1, respectively. For shore sediment samples having calcareous nature, the average concentrations of Ra-226, Th-232 and K-40 were 10.76, 9.86 and 304.74 Bq Kg 1. There are no risks for people health based on the calculated radiological hazard indices. However, people could be affected by radiation in one site (Marsa Alam-Shelateen Road km 33), where the representative level index (1.052 Bq kg 1) and absorbed gamma dose rate (66.5 nGy h 1) exceed the maximum permissible limits. © 2016 The Egyptian Society of Radiation Sciences and Applications. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/ by-nc-nd/4.0/).

1. Introduction Sea Coast. The area is rich in its natural resources, cultural heritage and archaeological sites. Wadi El Gemal (24 400 E- 35 100 N), Qulan For the time being, the Egyptian governments have undertaken (34 220 E- 35 230 N) and Abraq (23 250 E- 34 480 N) are important a number of tourism, resort, mining and industrial projects to sites in the area because of their unique flora and fauna, and develop Marsa Alam-Shalateen area lying along the southern Red therefore, they have been declared as natural protectorates (Baha El Din, 2001, pp. 241e264). The diverse in geology and climate within the area provide favorable habitat for a wide variety of coastal and desert plants having valuable ecological benefits (FAO, 2002; IRG/ * Corresponding author. EEAA, 2004). E-mail address: [email protected] (A.A. Arafat). Peer review under responsibility of The Egyptian Society of Radiation Sciences Indeed, the development process must include some measures and Applications. to conserve the environmental-natural resources (air, water, soil, http://dx.doi.org/10.1016/j.jrras.2016.11.006 1687-8507/© 2016 The Egyptian Society of Radiation Sciences and Applications. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006 2 A.A. Arafat et al. / Journal of Radiation Research and Applied Sciences xxx (2016) 1e14 shore sediment and plant) for the existing and future generations. A groundwater resources. rational approach, which balances between executing such projects The main concern of this work is to study the environmental and the natural resources, should be applied. In this context, it is radiological aspects in the environment of Marsa Alam-Shalateen important to have knowledge about the natural background base- area. The overall objectives are (1) to determine the activity con- lines of the radiological aspects so that potential environmental centrations and distributions of gamma ray emitter radionuclides, changes for the natural resources in future could be determined Ra-226 (U-238 series), Th-232 series, K-40 and Cs-137, in water, soil with a proper manner. and shore sediments, and (2) to assess their possible associated The activity concentrations of various radionuclides in natural hazards. The radiological obtained data and information from this resources play an essential role as regards the public and envi- study are highly needed to provide a basis for the sustainable ronmental health. The naturally occurring radioisotopes K-40 as development strategies. well as U-238 series and Th-232 series are the main sources of gamma radiation in rocks, soils and water. Human body could be 2. Methodology and techniques subjected to such radiation sources, either externally or internally (through inhalation and/or ingestion ways). From the radiological 2.1. Physical setting of the study area standpoint, the area under study attracted the attention of several workers. Ahmed et al., 2006 measured the activity concentrations Physical setting of an area (location, geomorphology, geology in different basement rocks in Wadi El Gemal area. The range of hydrogeology and climate) is of the important factors influencing mean activities was 3.9e49.1 Bq kg 1,6e47.9 and 84.5e1211.7 Bq the mobility of radionuclides through the environmental compo- kg 1 for Ra-226, Th-232 and K-40, respectively. Harb, El-Kamel, nents (IAEA, 2003; Harb et al., 2008, pp. 109e117). Some details Abd El-Mageed, Abbady, & Rashed, 2008, pp. 109e117, investi- about these factors in the study area are presented herein below. gated the radioactivity levels in granitic rocks along Idfu-Marsa Alam road. They found that the activity concentrations ranged from 2.1.1. Location 9.69 to 18.97 Bq kg 1 for Ra-226, from 9.99 to l7.65 Bq kg 1 for Th- Marsa Alam-Shalateen area lies along the southern Red Sea 232 and from 298.58 to 955.78 Bq kg 1 for K40. Yousef and Saleh, coast, Egypt, 700 km from the capital Cairo. It is situated between 0 0 2013, found that the activity concentrations of Th-232 and Ra- latitude 23 07 N in the south, latitude 25 47 N in the north, the 226 and K-40 in cataclastic rock samples taken from Abu Rusheid Red sea in the east, and the Red Sea Hills in the west (Fig. 1). The area (45 km southwest of Marsa Alam) ranged from 2.40 to area runs parallel to the coast for about 370 km. Access to the area is 487.40 ppm, from 42 to 277 ppm and from 0.1% to 6.8%, respec- through a number of paved roads, such as Cairo-Halayeb interna- tively. In addition, the natural background radioactivity was tional coastal road and, Idfu- Marsa Alam road. Several thousands determined for some unconsolidated shore sediment, soil, sea of people live in the coastal urban regions (Marsa Alam and Sha- water and plant samples by El Mamoney & Khater, 2004, Abdel- lateen cities) and as inland-Bedouin communities. The main eco- Razek, Bakhit, & Nada, 2008, EL Saharty and Dar, 2008, El-Taher nomic activities of inhabitants are tourism, herding (camel and & Madkour, 2011 and Salama, 2012). sheep), fishing, mining works (such as gold, antimony and phos- It was obvious from these studies that an attention was given to phate), goods trading and craft productions. determine the natural radioactivity of the rocks, shore sediments, sea water and plant, while a little one was paid to the soil cover. 2.1.2. Climate Moreover, review the previous works revealed, also, that there is no As part of the Eastern Desert, the study area lies within the arid baseline data or information regarding the radioactivity of the belt of Egypt. It has dry-continental climate with scarce rainfall,

Fig. 1. Geographic location of Marsa Alam-Shalateen area, Egypt.

Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006 A.A. Arafat et al. / Journal of Radiation Research and Applied Sciences xxx (2016) 1e14 3

Fig. 2. Surficial geologic map of the study area and its surroundings showing the main geomorphologic units and surface water divide (collected after, EGSMA, 1991 and INECO, 2009). abundant sunshine, high evaporation, and low humidity. The elevation attains about 1970 m above mean sea level. They have a annual average air temperature value is about 25.5 C. The total rugged topography dominated by huge number of drainage pat- rainfall intensity attains 17.4 mm/yr, with the greatest amount terns and wadis. (13 mm) in November. The annual average relative humidity and evaporation rate values are 43% and 16.8 mm, respectively (TDA/ 2.1.4. Geology RSSTI, 2003). The exposed geologic formations in the area include some of the Precambrian rocks (the oldest rocks on the earth) that are so 2.1.3. Geomorphology important for studying the earth's geologic history (TDA/RSSTI, The area is built of low and high topographic lands elevated 2003). The geology within the area under study and its extension above mean sea level (Fig. 2). The low topographic land is repre- to the west is, often, reflected in the terrain (Fig. 2). The Quaternary sented by the flat coastal plain (0.0e200 m above mean sea level) deposits dominate the coastal plain and wadis. They are repre- running parallel to the shoreline. The plain contains many land- sented by wadi deposits (detritals of sands and gravel), sabkhas forms including terraces, sand sheets, sand plains, sands and (fine sands, silts, silty clay, and evaporates) and terraces (gravels, gravels, sabkhas deposits, salt marshes and uplifted fossil reef sand and conglomerates, with evaporates deposits) (EGSMA, 1997). plateaus. The highlands comprise the uplifted relief high moun- The Precambrian basement rocks, as part of Arabian Nubian Shield, tains (Red Sea Hills) located to the west of the coastal plain. The are exposed widely in the highlands of the Eastern Desert (Said,

Fig. 3. Main water bearing formations in Egypt (after INECO, 2009).

Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006 4 A.A. Arafat et al. / Journal of Radiation Research and Applied Sciences xxx (2016) 1e14

1962;; Stern, 1979;; Greenwood, Anderson, Fleck, & Roberts, 1980). aquifers are hydraulically connected and found in contact with They consist, mainly, of granitic rocks, gneisses, schist and ophio- the Nubian sand stone aquifer system (Al-Gamal & Nada, 2000). lites, forming the mountain ranges known as the Red Sea Hills They represent important sources for drinking, agricultural (small (Hassan and Hashad, 1990; Said, 1990, pp. 259e293; Gharib, garden) and domestic uses. Farahat, & Ahmed, 2011). Structurally, the area is influenced by a Due to the scarcity of fresh groundwater, a number of desali- NW, NE, ENE and NNW trending faults. Folding is represented by nization plants were constructed to satisfy the increased demand major anticline folds associated with the ophiolitic rocks (Akaad & for water, especially for drinking and domestic purposes. These Abu El Ela, 2002; Gaafar and Abuelkhair, 2014). plants have been distributed, from north to south, along the shore line as follows; two plants in Marsa Alam city, one plant in Hamata 2.1.5. Hydrogeology area and one plant in Mars Homeira area. The study area is characterized by the presence of two main types of groundwater reservoirs, from east to west, they are Qua- 2.2. Sampling, treatment and in-situ measurements ternary alluvial aquifer and Pre-Cambrian fractured basement aquifer (Fig. 3). The Quaternary aquifer dominates the coastal plain Sixty nine environmental samples (water, soil and shore sedi- and wadis. It is composed of sands and gravels, with intercalations ments) were collected in May 2015 from the study area for radio- of silt and clay and fragments of materials of basement origin logical analysis, Ra-226, Th-232, K-40 and Cs-137. The coordinates (Shawky, Said, El-Aassar, Yousra Kotp, & Abdel Mottaleb, 2012). The of all sampling points were identified by the Global Positioning Precambrian basement aquifer is composed of highly weathered, System device (GPS, eTrex, Personal Navigator, Garmin Ltd). The jointed and faulted igneous and metamorphic rocks. It is charac- collected water samples (30 samples) represented all water re- terized by the presence of intersections of some dykes acting as sources in the coastal plain and wadis in the study area. Thirteen barriers against groundwater movement. The geometry of fractures groundwater samples were obtained from wells tapping the Qua- controls the direction of groundwater movement (Ismail, El Sayed, ternary alluvial aquifer and two samples were collected from the & Gomaa, 2005). The recharge to those aquifers is mainly from the available wells penetrating the fractured basement aquifer. Seven rainfall and occasional flash floods (Zagloul et al., 2000; ICEDP, sea water samples were collected from the Red Sea near the 2008 and; Azab, 2009). Moreover, a recharge from the deep shoreline. Four desalinized water samples were taken from the aquifers could, also, be occurred (Lankester, 2012). The two seawater desalination plants, two plants in Marsa Alam, one in

Fig. 4. Distribution of water samples in Marsa Alam-Shalateen Area.

Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006 A.A. Arafat et al. / Journal of Radiation Research and Applied Sciences xxx (2016) 1e14 5

Hamata and one plant in Marsa Homeira. Moreover, 4 samples were All samples were counted by HPGe detector coupled to 8192 collected from the discharged wastewater from those plants before multi e channel CANBERRA analyzer for data acquisition. The used the discharge to the sea. detector is P type and has 30% relative efficiency, resolution Specifications related to water wells such as well diameter, (FWHM) 2 keV for 1332.5 keV. The spectrum was analyzed by depths and heads above ground surface were determined. Depths GENIE-2000 software. The Th-232 was determined from the to water levels inside wells were measured using a suitable water average concentrations of 228- Ac (338.32 keV, 911 keV, level meter; model kurt, MIGGGE, Gm.b.H, 69 Heidelberg 1. 968.97 keV) and Tl-208 (583.19 keV) in the samples and the Ra-226 Hydrogen ion concentration (pH) and total water salinity (as total was determined from the average concentration of the Pb-214 dissolved solids, TDS) were measured for water samples using (351.9 keV) and Bi-214 (609.3, 1120, and 1764.5 keV) decay prod- Manta 2, Water-Quality Multiprobe device, Model Sub 3, USA. Then, ucts. The K-40 and Cs-137 were determined directly from every water sample was collected in 2 L labeled polyethylene bottle 1460.8 keV and 661.6 keV, respectively. and acidified by ultra pure nitric acid (Merck) to prevent bacterial To determine the background spectrum observed by the growth and adsorption of metal ions on the walls of the container. germanium detector, an empty marnilli beaker was counted from Additionally, 33 soil samples were collected from the soils time to another. The background was subtracted from the peak area covering the surfaces of wadis and plains and 6 shore sediments for the measured samples. The background was used to determine samples were obtained from sites adjacent to the sea shoreline. A the limit of detection and minimum detectable activity (MDA) ac- field description was carried out for samples and drops of dilute cording to Currie (1968). The minimum detectable activities at 95% hydrochloric acid were used to detect the presence of carbonaceous confidence level for the detecting system were 0.7, 0.6, 3, and 0.04 materials. The samples were obtained by template, in which a 25 Bq kg 1 for Ra-226, Th-232, K-40, and Cs-137, respectively. 25 cm2 area sample was cut out for guidance to a depth 10 cm. They Precision and accuracy of the measurements were checked by were collected in strong-labeled plastic bags after the field simultaneous measurement of the following IAEA reference ma- description. terials: RGU-1, RGK-1, Soil 6, IAEA-326, IAEA-152, IAEA-154, and IAEA-313 and by International Atomic Energy Agency inter- comparison runs. Activity concentration values are reported 2.3. Laboratory preparation, measurements and calculations as Bq L 1 for water and Bq kg 1 for soil and shore sediments 100 ml from the acidified water filed into polyethylene marnilli samples. and sealed carefully and stored for 4 weeks to reach secular equi- The radiological analysis was performed at Central Laboratory librium between Th-232 series and Ra-226 content of the sample for Environmental Radiation Measurement and Inter-comparison and their daughters. Each sample of soil and shore sediments, were (CLERMIT), Egyptian Nuclear and Radiological Regularity Author- dried at 105 C for 24 h in drying oven (Memmert) to insure ity (ENRRA). removal of moisture. After mixing thoroughly, the samples were sieved by 1 mm sieve and 100 ml was weighed, transferred into 2.4. Radiation hazard indices calculations polyethylene marnilli and sealed for 4 weeks to reach the secular equilibrium. For soil and shore sediment samples, the following radiation

Table 1 Inventory data of water resources, Marsa Alam-Shalateen Area.

Water type Area Sample No. Latitude Longitude Elevation, Depth, Well Well Depth pH TDS, mg/l m (amsl) m diameter, head, to m m water, m

Groundwater Quaternary Wadi Hafafit1 24 45.1000 34 31.5000 648 77 2.0 0.20 75 8.83 3148 aquifer Wadi Bezah 2 25 03.8160 33 54.6660 436 37 1.10 0.40 35 8.43 5301 Wadi Ghadeer 3 24 49.3500 34 59.6930 38 7 1.0 0.7 5 7.8 4119 Um El-Rus 4 25 26.6500 34 34.2330 341 101 1.0 0.85 100 7.76 5540 Um El-Rus 5 25 28.8500 34 37.8330 71 62 1.0 0.50 60 8.02 4176 Wadi El-Meyah 6 25 17.5830 34 00.9330 493 72 1.20 0.60 70 8.31 458.8 Wadi Abu Ghosoon 7 24 26.5330 35 11.6160 76 35.5 1.0 0.60 35 7.46 9745 Wadi Abu Ghosoon 8 24 25.5390 35 10.5610 164 12.40 1.0 0.20 11.20 7.05 13360 Wadi Abu Ghosoon 9 24 25.1860 35 09.6850 193 42 1.8 1.0 40 7.11 4936 Wadi Um Tendeba 12 24 56.7870 34 56.3090 43 e 1.10 0.20 2.10 6.99 8175 Idfo Road 13 25 01.9980 34 43.7250 274 e 2.0 1.0 19.20 8.3 8283 Idfo Road 14 25 03.0150 34 30.1070 464 e 1.0 0.20 18.5 7.79 3299 Idfo Road 15 25 46.8500 34 29.5060 46 50 0.30 1.0 15 7.14 32440 Basement Al Gaheliya 10 23 30.7170 35 08.3740 404 8.20 1.0 0.40 5.20 8.11 367.4 aquifer Al Gaheliya 11 23 30.6660 35 08.4450 387 7 1.5 0.20 5 7.92 556.3 Sea water Abu Ghosoon 16 24 26.3510 35 12.5990 0.0 ee ee 8.15 40790 Hamata 17 24 16.3210 35 22.7620 0.0 ee ee 7.6 39870 North Abu Ghosoon 18 24 36.9600 35 08.4660 0.0 ee ee 7.7 39960 North Abu Ghosoon 19 25 05.6160 34 53.2500 0.0 ee ee 7.61 39760 Homeira 20 23 28.2190 35 29.4950 0.0 ee ee 8.16 40250 Shalateen 21 23 08.7480 35 37.1800 0.0 ee ee 8.11 41070 Marsa Alam 22 25 46.8500 34 29.5060 0.0 ee ee 8.15 40020 Desalinized water Hamata plant 23 24 16.3210 35 22.7620 22 ee ee 6.88 443.6 Marsa Homeira plant 24 23 28.2190 35 29.4950 24 ee ee 7.07 474.8 Marsa Alam plant 1 25 25 46.8500 34 29.5060 28 ee ee 6.91 263.4 Marsa Alam plant 2 26 25 46.8500 34 29.5060 28 ee ee 6.61 524.7 Wastewater Hamata plant 27 24 16.3210 35 22.7620 22 ee ee 7.56 55690 Marsa Homeira plant 28 23 28.219 35 29.4950 24 ee ee 8.05 50530 Marsa Alam plant 1 29 25 46.8500 34 29.5060 28 ee ee 7.48 42960 Marsa Alam plant 2 30 25 46.8500 34 29.5060 28 ee ee 8.01 56600

Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006 6 A.A. Arafat et al. / Journal of Radiation Research and Applied Sciences xxx (2016) 1e14 hazard indices are estimated based on the measured activity K-40 activities in groundwater reservoirs. It is worth to mention concentrations: that in this figure instead of exclusion the activity concentrations under the detection limits of some groundwater samples, activity 1 1 1. Radium Equivalent Activity (Raeq); Raeq (Bq kg ) ¼ ARa þ 1.43ATh values equal to half the detection limits (0.7 Bq L for Ra-226 and 1 þ 0.077AK (1) (Beretka & Mathew, 1995) 3BqL for K-40) were used for those samples in contouring 2. Representative level Index (Iɤr); Iɤr(Bq kg 1) ¼ 0.0067 process. The activity concentrations vary from one locality to ARa þ 0.01ATh þ 0.00067Ak z 1 (2) (NEA-OECD, 1979) another. The contour maps indicate that there is compatibility, to 3. Absorbed gamma dose rate (D); D (nGy h 1) ¼ 0.49 some extent, as regards the trends of the increase or decrease of the ARa þ 0.67ATh þ 0.048Ak (3) (UNSCEAR, 1988) Ra-226 and K-40 activities. Generally, the highest values of Ra-226 4. Annual Gonadal Equivalent Dose (AGED); AGDE (mSv y 1) ¼ 3.09 and K-40 activities are recorded at the northern part of the area. ARa þ 4.18ATh þ 0.314AK (4) (Avwiri, Osimobi, & Agbalagba, 2012) To examine the factors controlling the variation in activity 5. Annual Effective Dose Equivalent (AEDE) outdoor; AEDE (mSv concentration in groundwater, a correlation analysis among the y 1) ¼ dose rate (in nGy h 1) x 24 h 365.25 d x 0.2 (occupancy measured physical, chemical and activity concentrations variables factor) x 0.7 Sv Gy 1 (conversion coefficient) x 10 3 (5) is made (Table 3). For samples having activity concentrations under (UNSCEAR, 2000) the detection limits, activity values equal to half the detection 1 1 6. External hazard index (Hex); Hex ¼ ARa/370 þ ATh/259 þ Ak/ limits (0.7 Bq L for Ra-226 and 3 Bq L for K-40) were used for 4810 < 1 (6) (UNSCEAR, 1988) those samples in the correlation analysis. The correlation analysis 7. Internal hazard index (Hin); Hin ¼ ARa ∕ 185 þ ATh ∕ 259 þ AK ∕ indicates K-40 is weakly correlated with Ra-226 (r ¼ 0.378) and TDS 4810 < 1 (7) (Beretka and Matthew, 1985) (r ¼ 0.368), and it has no relation with pH, depth to water and 8. Excess Lifetime Cancer Risk (ELCR); ELCR (mSv y 1) ¼ AEDE x DL x elevation. Moreover, the activity concentration of Ra-226 is weakly RF (8) (Taskin et al., 2009) correlated with elevation (r ¼ 0.271) and has no relation with the others variables. Where, ARa,ATh and AK, are the specific activities of Ra-226, Th- It seems from the correlation analysis that the Ra-226 and K-40 232 and K-40 in Bq kg 1. The DL is the average duration of life activities are not affected greatly by the hydrogeochemical factors (estimated to be 70 years) and RF is the risk factor (Sv), for sto- controlling the groundwater chemistry. Most probably, there are chastic effects, RF is used as 0.05 for the public (ICRP, 1990). others factors causing the irregular distribution of radionuclides in groundwater. Of these factors is the irregular distribution of ra- 3. Results and discussion dionuclides in the surroundings basement rock's catchments. As has been previously mentioned, the groundwater in the study area 3.1. Water resources is mainly recharged from the direct rainfall and occasional flash floods. Usually, the rains contain low concentrations of radioiso- In the area under study, water resources comprise groundwater, topes (Chau et al., 2011). The flash floods in the catchments areas desalinized water and Red Sea water. Distributions of sampling leach the exposed basement rocks, which are rich in radionuclides points are shown in Fig. 4. The inventory data of these points and (Ahmed et al., 2006; Harb et al., 2008, pp. 109e117; Yousef and the Ra-226, Th-232 and K-40 activity concentrations are listed in Saleh, 2013). As a result of that an amount of primordial Tables 1 and 2. For all water samples taken from the different types of water resources, the activity concentrations of Cs-137 radionu- Table 2 clide are under the detection limit of the used analytical Activity concentrations (BqL 1) for water resources, Marsa Alam-Shalateen Area. procedures. Sample No. Ra -226 ± err, Th-232 ± err, K-40 ± err, 3.1.1. Groundwater 1 <0.7 <0.6 <3 < < < Groundwater is available from wells tapping both the Quater- 2 0.7 0.6 3 3 <0.7 <0.6 <3 nary alluvial aquifer and fractured basement one. The primary re- 4 <0.7 <0.6 <3 sults of the field survey indicate that most wells tapping the 5 <0.7 <0.6 <3 Quaternary aquifer, but well No. 15, are hand-dug well an example 6 <0.7 <0.6 17.85 ± 0.88 as shown in Fig. 5, with total depths, diameters and depths to water 7 <0.7 <0.6 23.47 ± 1.14 8 <0.7 <0.6 29.09 ± 1.49 levels ranging from 12.4 m to 101 m, from 1 m to 2 m and from 2.10 9 <0.7 <0.6 <3 m to 100 m, respectively. Well No. 15 was drilled by normal-rotary 12 <0.7 <0.6 26.49 ± 1.32 method, with 50 m depth and 0.30 m diameter. 13 2.5 ± 0.23 <0.6 32.84 ± 1.61 The groundwater of the Quaternary alluvial aquifer has pH 14 7.09 ± 0.62 <0.6 13.95 ± 0.77 < < < conditions ranging from neutral (6.99) to alkaline (8.83). A wide 15 0.7 0.6 3 10 <0.7 <0.6 12.83 ± 0.76 range in total salinity of the groundwater is observed, where the 11 7.6 ± 0.7 <0.6 29.88 ± 1.53 1 total dissolved solids (TDS) varies between 3148 mg L (brackish 16 <0.7 <0.6 <3 water) and 32440 mg L 1 (saline water). The groundwater of the 17 6.31 ± 0.57 <0.6 34.42 ± 1.62 fractured basement aquifer is fresh (TDS < 560 mg L 1) and alkaline 18 <0.7 <0.6 37.6 ± 1.79 19 <0.7 <0.6 30.1 ± 1.49 (pH z 8) with respect to reaction conditions. 20 <0.7 <0.6 <3 The activity concentrations of Th-232 are under the detection 21 5.98 ± 0.59 <0.6 38.17 ± 1.92 limits of the used analytical procedures. The Ra-226 activities in all 22 2.95 ± 0.29 <0.6 11.06 ± 0.49 groundwater samples (except for samples 11, 13 and 14) are under 23 <0.7 <0.6 6.89 ± 0.43 < < ± the detection limit. The exceptional samples show Ra-226 activities 24 0.7 0.6 54.31 2.27 < < < ± ± 1 25 0.7 0.6 3 ranging from 2.5 0.23 to 7.6 0.7 Bq L . About 53% of the 26 <0.7 <0.6 <3 groundwater samples exhibit K-40 activities in the range of 27 <0.7 <0.6 <3 12.83 ± 0.76 to 32.84 ± 1.61 Bq L 1, while the rest of samples show 28 10.66 ± 0.92 2.33 ± 0.22 24.62 ± 1.18 activity concentrations under the detection limit. 29 <0.7 <0.6 7.11 ± 0.32 30 6.87 ± 0.66 <0.6 40.91 ± 1.99 Fig. 6 shows the lateral distribution of the measured Ra-226 and

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The increase of K-40 radionuclides in groundwater could be attributed to the high increase in K-40 radionuclides in the base- ment rocks. The very low content of Th-232 in groundwater could be attributed to (1) the low concentrations in the catchments areas and (2) to the rapid adsorption onto sediment (Bowen, 1979), either on the surficial soils through surface runoff or on the materials of the unsaturated zone during the subsurface seepage. More investigations dealing with the true content of radionu- clides in rains falling on the area, in the aquifer's materials and in the others hydraulically connected aquifers should be known to understand more about the true process affecting the variation in radionuclides concentrations.

3.1.2. Desalinized water and wastewaters Desalinized water samples have salinity varying between 263.4 mg L 1 and 524.7 mg L 1, with slightly acidity (pH ¼ 6.61) to neutral (pH ¼ 7.07). Of these samples, two samples 23 and 24 show 6.89 ± 0.43 and 54.31 ± 2.27 Bq L 1 of K-40 respectively. While the activity concentrations of Ra-226 and Th-232 are under the detection limit. Wastewaters discharged from desalinization plants are charac- 1 Fig. 5. Photographs showing heads of hand dug wells (Al Gaheliya and Abu Ghosoon terized by the highest salinity values, between 42960 mg L and wells), Marsa Alam- Shalateen Area. 56600 mg L 1, with slightly alkalinity (pH ¼ 7.48) and alkalinity (pH ¼ 8.05) in reactions. The Th-232 activities for all wastewater samples are under the detection limit except sample No 28 has fl radionuclides are transported to the overland ow in wadis and 2.33 ± 0.22 Bq L 1. The Ra-226 activities 10.66 ± 0.92 and fi plains and, consequently, to groundwater by in ltration and 6.87 ± 0.66 Bq L 1 are recorded, only for samples Nos 28 and.30 percolation. respectively. The major part of wastewater samples show K-40

Fig. 6. Lateral distribution of Ra-226 and K-40 in groundwater reservoirs, Marsa Alam-Shalateen Area.

Table 3 Pearson correlation coefficients (r) for some physical, chemical and activity Parameters, groundwater samples, Marsa Alam-Shalateen Area.

Groundwater samples Elevation, m (above mean sea level Depth to water, m pH TDS, mg L 1 Ra-226, BqL 1 K-40, Bq L 1

Elevation, m (above mean sea level 1 Depth to water, m 0.393 1 pH 0.743 0.403 1 TDS, mg L 1 0.522 0.220 0.533 1 Ra-226, Bq L 1 0.271 0.331 0.103 0.277 1 K-40, Bq L 1 0.394 0.466 0.500 0.368 0.378 1

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activities in the range of 7.11 ± 0.32 - 40.91 ± 1.99 Bq L 1. alkalinity (pH ¼ 8.16) in reaction conditions. The Th-232 activity in all samples is under the detection limit. Three sea water samples 3.1.3. Red Sea water (17 (Hamata area), 21 (Shalateen area), and 22 (Marsa Alam area) ± e Red Sea water samples show salinity values ranging from show Ra-226 activities in the range of 2.95 0.29 6.31 ± 1 39760 mg L 1 to 41070 mgL 1, with slightly alkalinity (pH ¼ 7.6) to 0.57 Bq L , and the rest of samples have concentration under the

Table 4 Field description of soil samples, Marsa Alam-Shalateen Area.

Area Sample No. Latitude Longitude Eleva-tion, Lithic description m (amsl)

W. Abu Ghusoon 1 24 25.5390 35 10.5610 27 Sand; , pale yellowish brown, m. to v. c. sand-sized, ill sorted, angular to sub-angular W. Abu Ghusoon 2 24 25.1860 35 09.6850 81 Sand, pale brown, f. to m. sand-sized, moderately sorted, angular to sub-angular, low amount of gravels Marsa Alam-Shelateen Road km 33 3 24 49.7160 34 59.6100 6 Sand, pale reddish brown, f. to v. c. sand-sized, ill sorted, angular to sub-angular W. Al Gemal 4 24 40.7180 35 05.0020 0.0 Sand, pale grayish brown, f. sand-sized, well rounded Marsa Alam-Shelateen Road km69 5 24 32.9850 35 08.4960 6 Sand, yellowish brown, f. sand-sized, well sorted Hamata Village 6 24 16.3210 35 22.7620 19 Sand, pale brown, v.f. to v.c. sand-sized, ill sorted, sub- angular to sub-rounded Baranis village 7 23 57.5130 35 24.7430 49 Gravelly sand; pale yellowish brown, v.f. to v.c. sand sized, ill sorted, sub-rounded to rounded, 20% gravel Marsa Homeira 8 23 28.1760 35 29.3240 12 Sand; dark greenish grey, f. sand-sized, well sorted, well rounded 10 km Al -Gaheliya-Abraq road 9 23 23.9130 35 24.8730 123 Gravelly sand; pale brownish grey, f. to v.c. sand-sized, ill sorted, 30% gravels 30 km Al Gaheliya-Abraq road 10 23 25.8130 35 14.3530 241 Sand; pale brownish grey, v.f. to m. sand-sized, moderately sorted, low amount of gravel 20 km Al Gaheliya-Abraq road 11 23 23.5510 35 17.9450 240 Gravelly sand; yellowish brown, f. to v.c. sand-sized, ill sorted, sub-angular to sub-rounded, with rock fragments 0.0 km Al Gaheliya-Abraq road 12 23 24.3690 35 30.2260 27 Sand; pale brown, v.f. to v.c. sand-sized, ill sorted, sub- angular to sub-rounded, low amount of gravels Shalateen 13 23 07.3860 35 33.7550 21 Sand; yellowish brown, f. to c. sand-sized, ill sorted, low amount of gravels 18 km Shalateen-Marsa Alam Road 14 23 10.0210 35 31.2870 23 Sand; pale brown, v.f. to f. sand-sized, moderately sorted, low amount of gravels and clay 10 km Baranis-Aswan Road 15 24 02.0950 35 19.3250 182 Sand; pale brownish grey, v.f. to m. sand-sized, moderately sorted, low amount of gravel 20 km Baranis-Aswan Road 16 24 01.4790 35 14.3670 313 Sand; pale brownish grey, v.f. to m. sand-sized, moderately sorted, low amount of gravel 30 km Baranis-Aswan Road 17 24 00.0310 35 09.7030 387 Sand; pale brown, v.f. to m. sand-sized, moderately sorted, low amount of clay 37 km Baranis-Aswan Road 18 23 57.2010 35 10.0720 475 Sand; pale brown, f. to m. sand-sized, moderately sorted, low amount of rock fragments and clay 47 km Baranis-Aswan Road 19 23 54.3820 35 06.7030 583 Sand; yellowish brown, v.f. to v.c. sand-sized, ill sorted, low amount of gravels and clay 5 km Shelateen-Marsa Alam Road 20 24 00.2380 35 22.7370 62 Sand; pale brown, v.f. to m. sand-sized, moderately sorted, low amount of clay and gravels W. Um Tendeba 21 24 56.7870 34 56.3090 6 Sand; pale brownish grey, v.f. to m. sand-sized, moderately sorted, low amount of gravel 10 km, Marsa Alam-Idfo Road 22 25 02.2730 34 46.3660 200 Sand; pale brown, v.f. to v.c. sand-sized, ill sorted, low amount of gravels 20 km Marsa Alam-Idfo Road 23 25 01.5290 34 41.3910 335 Sand; pale yellowish brown, v.f. to v.c. sand-sized, ill sorted, low amount of gravels 30 km Marsa Alam-Idfo Road 24 25 02.0890 34 36.0710 491 Sand; dark brown, f. sand-sized, well sorted, low amount of gravels 40 km Marsa Alam-Idfo Road 25 25 03.0150 34 30.1070 476 Sand; pale brown, f. to m. sand-sized, moderately sorted, low amount of clay and rock fragments W.Hafafit2624 45.1000 34 31.5000 558 Sand; pale brownish grey, v.f. to m. sand-sized, moderately sorted, low amount of rock fragments W. Bezah 27 25 03.8160 33 54.6660 415 Sand; pale brown, v.f. to v.c. sand-sized, ill sorted, angular to sub-angular, low amount of gravels W. Ghadeer 28 24 49.3500 34 59.6930 13 Sand; dark brown, v.f. to v.c. sand-sized, ill sorted, angular to sub-angular, 10% multicolored gravels, low amount of clay Beside Um El Rus Mine 29 25 26.6500 34 34.2330 120 Sand; pale yellowish brown, f. sand-sized, well rounded, low amount of clay Um El Rus 30 25 28.8500 34 37.8330 42 Sand; brown, f. to v.c. sand-sized, ill sorted, low amount of clay (10%) W. El Meyah 31 25 17.5830 34 00.9330 450 Clayey sand; pale yellowish brown, v.f. to f. sand-sized, 25% clay W.Abu Ghuson 32 24 25.5390 35 10.5610 35 Sandy gravel; yellowish brown, v.f. to c. sand-sized, 40% clay and 5% gravels Al Gaheliya 33 23 30.7170 35 08.3740 442 Sand; dark grayish brown, f. to v.c. sand-sized, ill sorted, low amount of clay and gravels

V.F.: very fine, f: fine, M. medium c: coarse v.c.: very coarse.

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Table 5 Field description of shore sediment samples, Marsa Alam-Shalateen Area.

Area Sample No. Lat. Long. Eleva-tion, Lithic description m (amsl)

Abu Ghuson 1 24 26.3510 35 12.5990 1.0 Sand; pale brown, v.f. to f. sand-sized, moderately sorted, well rounded Hamatta village 2 24 16.3210 35 22.7620 8.0 Sand; whitish brown, f. to v.c. sand-sized, ill sorted, low amount of gravels and shells North Abu Ghuson 3 24 30.0900 35 08.6550 7.0 Sand; pale yellowish brown, f. sand-sized, well rounded North Abu Ghuson 4 24 49.7140 34 59.6110 5.0 Sand; pale pinkish brown, f. to m. sand-sized, moderately sorted, low amount of gravels Marsa Homeira 5 23 28.2190 35 29.4950 6.0 Sand; dark greenish grey, f. sand-sized, well rounded Shelateen 6 23 08.7480 35 37.1800 2.0 Sand; pale yellowish brown, f. sand-sized, well rounded v.f.: very fine f: fine M. medium v.c.: very coarse.

detection limit. On the contrary of Ra-226 and Th-232, the K-40 (8.68 Bq kg 1, in average) for Th-232 and from 91.22 to 518.21 activities are recorded for most samples to be in the range of Bq kg 1 (234.47 Bq kg 1, in average) for K-40 radionuclide. For the 11.06 ± 0.49e38.17 ± 1.92 Bq L 1. two types of soils, the concentrations of radionuclides follow the order K-40>Ra-226>Th-232. 3.2. Soil cover and shore sediments The radionuclide contents in the calcareous soils (formed, mainly, of very fine to coarse sand-sized particles) are higher than fi 3.2.1. Sources of soil and shore sediments those in the siliceous ones (formed, mainly, of very ne to medium The field description may give a clue about the soil and shore sand-sized particles). This means that the chemical composition sediments resources and chemical compositions as well as the and grain size, partially, control the concentration of radionuclides main geological processes (weathering, erosion and deposition and in soils. The authors believe that, the variation in the concentration digenesis) responsible for their formation (Compton, 1962;; Bui, of radionuclides in the original rocks, representing the main source Mazullo, & Wilding, 1990; FAO, 2006; Rajganapathi, Jitheshkumar, of soils, is an important factor controlling the amounts of radio- Sundararajan, Bhat, & Velusamy, 2012). The filed description of nuclides in soil cover. The increase in K-40 contents, comparing soil and shore sediment samples collected from wadis and coastal with the others radionuclides, in soil samples could be attributed to plain in the study area is shown in Tables 4 and 5 respectively. The the increase in K-40 radionuclides in the surroundings basement description includes the soil and sediment's color, chemical nature rocks. It is important to remember that the K-40 content exceeds (calcareous or siliceous) and texture (particle size, shape, round- greatly the contents of Ra-226 and Th-232 radionuclides in the e ness, and sorting). exposed basement rocks (Harb et al., 2008, pp. 109 117; Yousef and The soil and shore sediments in the study area are unconsoli- Saleh, 2013). dated and differ widely in their color reflecting their various Fig. 8 indicates that the activity concentration levels in the soil sources and, to some extent their chemical composition. All sam- cover differ from place to place. The activity contour maps show ples (except for soil samples 7, 10, 15, 16 and 26) are of calcareous that the trends of the increase and decrease of Ra-226 and Th-232 nature. The exceptional samples are of siliceous nature. Approxi- contents are similar. The Ra-226 and Th-232 radionuclides are ¼ mately, all soil and shore sediments samples are made up of sand- strongly correlated (r 0.854) (Table 7). In the northern part of the sized particles mixed, in some places, with different amounts of area, the Ra-226 and Th-232 activities increase from W to E. These gravels, clay and rock fragments of basement rocks. The degree of trends match very well with the trend of the surface runoff from W sorting and rounding of grains vary from place to another. Most of samples are composed of ill sorted sand grains indicating the dif- ferences in grain densities and showing the effect of the high en- ergy of the transportation medium (flash flood and/or wind). Angular to sub-angular grains characterizing some samples indi- cate the short time and distance involved in the transportation of the weathered materials from the parent rocks (surroundings high mountains) to the place of deposition (wadis and plains). Accordingly, the basement complex (igneous and metamorphic rocks) and sedimentary rocks (limestone, sandstone and shale) of high mountains are the main sources of the soil cover and shore sediments in the study area. Primordial radionuclides associated to such rocks are often transported to soil and shore sediments under the action of the above mentioned geologic processes.

3.2.2. Distribution of activities in soil cover and shore sediments 3.2.2.1. Soil cover. Distribution of soil sampling locations is shown in Fig. 7 and the measured activity values are given in Table 6. For all soil samples, the activity concentrations of Cs-137 radionuclide are under the detection limit of the used analytical procedures. The carbonaceous soils show activity concentrations range from 8.13 to 34.71 Bq kg 1 (18.45 Bq kg 1, in average) for Ra-226, from 7.87 to 34.5 Bq L 1 (16.78 Bq kg 1, in average) for Th-232 and from 173.82 to 736.78 Bq kg 1 (334.35 Bq kg 1, in average) for K-40. The siliceous soils show activities ranging from 6.0 to 18.47 Bq kg 1 1 1 (10.24 Bq kg , in average) for Ra-226, from 2.42 to 16.03 Bq kg Fig. 7. Distribution of soil samples in Marsa Alam-Shalateen Area.

Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006 10 A.A. Arafat et al. / Journal of Radiation Research and Applied Sciences xxx (2016) 1e14 to E. Surface runoff leaches the rocks-forming minerals in the upper The K-40 is correlated with Ra-226 (r ¼ 0.643). This may indicates reaches of watershed, carries the eroded materials containing ra- that these radionuclides are originated from the same source and dionuclides and, eventually, deposits them in coastal plain as the their concentrations are, for the most part, affected by the same velocity of water flow decreases. In the other side, the activity geochemical processes. Moreover, the activity concentrations seem content of K-40 in soil samples has a weak relation with Ra-226 (r ¼ to be somewhat independent of the grain size (see Table 5&8). For 0.377) and Th-232 (r ¼ 0.48) as indicated in Table 7. It increases, instance, the shore sediment sample 2 (composed of very fine to generally, from SE to NW. The highest K-40 activity values are very coarse sand-sized particles) shows K-40 activity that is higher recorded in the area located between Marsa Alam and . than those recorded for sample 1 (composed of very fine to fine Such area is characterized by the existence of large number of sand-sized particles) and for samples 3 and 6 (composed of fine- mines, such as feldspars, granite, quartz, building materials (sands sand sized particles). and gravels) mines, which, usually, resulting in more potassium releases to the environment. 3.3. Associated hazards

3.2.2.2. Shore sediments. Distribution of shore sediment samples is 3.3.1. Water resources given in Fig. 9. The activity concentrations of Ra-226, Th-232 and K- From the salinity point of view, groundwater discharged from 40 radionuclides of the samples are listed in Table 8. For all shore the Quaternary aquifer in the study area is not suitable for drinking sediment samples, the activity concentrations of Cs-137 radionu- because of the high salinity, where the total dissolved solids 1 clide are under the detection limit of the used analytical exceeding the maximum permissible limit (TDS ¼ 1000 mg L ) procedures. reported by HCW (2007). The groundwater extracted from wells 10 The range and (average) of activity concentrations are and 11 and desalinized water (samples 23, 24, 25 and 26) are 4.42e23.46 Bq kg 1 (10.76 Bq kg 1) for Ra-226, 4.90e19.12 Bq kg 1 currently used for drinking. (9.86 Bq kg 1) for Th-232 and 198.00e547.79 Bq kg 1 (304.74 Radiologically, water from Al Gaheliya well (sample No.11) is not Bq kg 1) for K-40. Although they have the same order of radionu- safe for drinking, where it shows Ra-226 activity value attaining 1 1 clide dominance (K-40>Ra-226>Th-232), the activity values of 7.6 ± 0.7 Bq L , which exceed greatly the guidance level (1 Bq L ) shore sediment samples are, generally, lower than those recorded reported by WHO (2011). This water is not suitable for drinking, and for the calcareous soil ones. This, most probably, due to the action of needs to be treated to mitigate or remove the Ra-226 content sea water waves (tidal effect), which lead to continuous leaching of before consuming by public. such sediments. Table 9 indicates the significant positive relationships among 3.3.2. Soil and shore sediments the activities of the three radionuclides. The Th-232 is strongly The calculated hazard indices for soil and shore sediments correlated with both Ra-226 (r ¼ 0.98) and with K-40 (r ¼ 0.755). samples are listed in Tables 6 and 8 respectively. They include the

Table 6 Activity concentrations and calculated hazard indices for soil samples, Marsa Alam-Shalateen area.

Sample No. Ra -226 ± err Th-232 ± err K-40 ± err Raeq Ig r D AGDE AEDE Hex Hin ELCR x 103

1 8.13 ± 0.56 7.97 ± 0.74 387.06 ± 10.85 49.33 0.392 24.75 180.05 30.36 0.133 0.155 0.106 2 10.83 ± 0.59 7.87 ± 0.74 257.99 ± 8.54 41.95 0.323 20.51 147.42 25.15 0.113 0.143 0.088 3 33.50 ± 0.96 33.77 ± 1.72 736.78 ± 12.37 138.52 1.052 66.52 476.17 81.58 0.375 0.465 0.286 4 19.84 ± 0.97 19.17 ± 1.63 273.71 ± 6.32 68.33 0.506 32.06 227.44 39.32 0.185 0.238 0.138 5 30.99 ± 2.21 13.23 ± 1.02 109.33 ± 3.70 58.33 0.412 26.69 185.41 32.74 0.158 0.241 0.115 6 11.92 ± 0.59 13.01 ± 0.99 344.40 ± 10.17 57.04 0.439 27.72 199.43 33.99 0.154 0.186 0.119 7a 8.11 ± 0.39 9.71 ± 0.79 158.16 ± 7.78 34.17 0.257 16.17 115.34 19.84 0.092 0.114 0.069 8 20.79 ± 0.83 19.41 ± 1.50 184.14 ± 5.54 62.73 0.455 28.88 203.23 35.42 0.170 0.226 0.124 9 34.71 ± 0.69 32.49 ± 2.11 440.31 ± 10.97 115.07 0.850 53.85 381.41 66.04 0.311 0.405 0.231 10a 12.19 ± 0.61 12.83 ± 0.90 250.66 ± 8.45 49.84 0.377 23.80 170.05 29.18 0.135 0.168 0.102 11 19.99 ± 0.81 15.31 ± 1.06 363.36 ± 6.69 69.86 0.529 33.58 239.93 41.19 0.189 0.243 0.144 12 28.63 ± 0.80 19.59 ± 1.21 348.73 ± 10.21 83.50 0.619 39.48 279.92 48.42 0.226 0.303 0.169 13 18.26 ± 0.68 17.47 ± 1.09 396.43 ± 9.74 73.77 0.561 35.48 254.01 43.51 0.199 0.249 0.152 14 19.97 ± 0.73 20.00 ± 1.22 432.00 ± 10.58 81.83 0.621 39.27 281.04 48.16 0.221 0.275 0.169 15a 6.00 ± 0.46 2.42 ± 0.24 154.10 ± 4.40 17.87 0.143 9.21 66.96 11.30 0.048 0.064 0.040 16a 6.41 ± 0.38 2.42 ± 2.40 91.22 ± 3.89 16.89 0.128 8.21 58.58 10.07 0.046 0.063 0.035 17 8.51 ± 0.55 9.08 ± 0.77 173.82 ± 4.43 34.88 0.263 16.64 118.86 20.40 0.094 0.117 0.071 18 14.93 ± 0.97 19.24 ± 1.13 212.50 ± 5.00 58.81 0.434 27.29 193.32 33.47 0.159 0.199 0.117 19 28.81 ± 2.22 34.50 ± 1.85 269.14 ± 5.70 98.87 0.716 45.17 317.80 55.40 0.268 0.345 0.194 20 8.13 ± 0.45 10.57 ± 0.92 146.53 ± 6.79 34.53 0.258 16.21 115.34 19.88 0.093 0.115 0.069 21 15.35 ± 0.67 12.86 ± 1.09 358.43 ± 10.45 61.34 0.470 29.79 213.81 36.53 0.166 0.207 0.128 22 17.63 ± 0.73 13.60 ± 1.17 250.59 ± 6.91 56.37 0.421 26.74 190.06 32.80 0.152 0.200 0.115 23 22.11 ± 1.74 18.36 ± 1.18 298.81 ± 5.87 71.37 0.530 33.67 238.95 41.29 0.193 0.253 0.145 24 18.53 ± 0.98 18.87 ± 1.41 364.81 ± 6.89 73.60 0.555 35.11 250.76 43.06 0.199 0.249 0.151 25 17.204 ± 1.00 16.97 ± 1.14 235.11 ± 5.28 59.61 0.441 27.94 198.08 34.26 0.161 0.208 0.120 26a 18.47 ± 1.00 16.03 ± 1.59 518.21 ± 7.86 81.30 0.629 39.82 286.90 48.84 0.220 0.269 0.171 27 10.55 ± 0.72 9.25 ± 0.74 238.27 ± 5.67 42.13 0.322 20.38 146.15 25.00 0.114 0.142 0.087 28 18.09 ± 0.93 14.35 ± 1.70 463.00 ± 8.70 74.26 0.573 36.32 261.36 44.55 0.201 0.249 0.156 29 22.65 ± 0.95 19.10 ± 1.05 334.75 ± 6.30 75.74 0.565 35.87 255.00 43.99 0.205 0.266 0.154 30 15.7 ± 1.20 13.09 ± 1.22 383.11 ± 6.44 63.92 0.491 31.12 223.60 38.16 0.173 0.215 0.1335 31 17.81 ± 0.65 14.82 ± 1.47 326.27 ± 6.60 64.13 0.484 30.73 219.49 37.69 0.173 0.221 0.132 32 10.52 ± 0.816 9.60 ± 1.53 546.57 ± 7.29 66.33 0.531 33.52 244.37 41.11 0.179 0.208 0.144 33 12.5 ± 0.70 16.38 ± 1.30 485.82 ± 12.82 73.33 0.571 35.94 259.74 44.08 0.198 0.232 0.154 Unit Bq/Kg Bq/Kg Bq/Kg Bq/Kg Bq/Kg nGy h 1 mSv y 1 mSv y 1 mSv y 1

a Siliceous samples.

Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006 A.A. Arafat et al. / Journal of Radiation Research and Applied Sciences xxx (2016) 1e14 11

Fig. 8. Lateral distribution of Ra-226 Th-232 and K-40 in soil cover, Marsa Alam-Shalateen Area.

radium equivalent (Raeq), gamma radiation hazard index (Iɤr), containing different concentrations of Ra-226, Th-232 and K-40. It absorbed gamma dose rate (D), annual Gonadal equivalent dose is based on the assumption that 10 Bq kg 1Ra-226, 7 Bq kg 1 Th- (AGED), annual effective dose equivalent (AEDE), external hazard 232 and 130 Bq kg 1 K-40 produce the same gamma dose rate. 1 index (Hex), Internal hazard index (Hin) and excess lifetime cancer The Raeq ranges from 16.89 to 138.5 (30.56 Bq kg , in average) and risk (ELCR). from 27.32 to 82.05 Bq kg 1 (48.3 Bq kg 1, in average) for soil and 1 The Radium equivalent (Raeq,Bqkg ) is a radiation hazard shore sediment samples, respectively. These values are, greatly, index, which is used to compare the specific activities of samples lower than the maximum permissible limit (370 Bq kg 1)as

Table 7 Pearson correlation coefficients (r) for activity concentrations and elevations parameters, soil samples, Marsa Alam- Shalateen Area.

Ra-226, Bqkg 1 Th-232, Bqkg 1 K-40, Bqkg 1 Elevation, m (above mean sea level)

Ra-226, Bqkg 1 1 Th-232, Bqkg 1 0.854 1 K-40, Bqkg 1 0.377 0.480 1 Elevation, m (above mean sea level) 0.065 0.172 0.097 1

Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006 12 A.A. Arafat et al. / Journal of Radiation Research and Applied Sciences xxx (2016) 1e14

The gonads, the bone marrow and the bone surface cells are considered as organs of interest by UNSCEAR (2000) because of their sensitivity to radiation. An increase in AGED has been known to affect the bone marrow, causing destruction of the red blood cells that are then replaced by white blood cells. This situation results in a blood cancer called leukemia which is fatal. The annual gonadal dose equivalent (AGDE) values vary between 58.5 and 476.17 mSv.y 1 (218.1 mSv y 1, in average) and between 99.0 and 291.3 mSv y 1 (170.1 mSv y 1, in average) for soil and sediment samples, respectively. These results are below the maximum permissible value (3 x 105 m Sv y 1) recommended by UNSCEAR (2000). The annual effective dose equivalent (AEDE) values range from 10.0 to 81.5 (37.5 mSv y 1, in average) and from 16.7 to 49.4 mSv y 1 (28.9 mSv y 1, in average) for soil and sediment samples, respec- tively. These values are less than the maximum permissible value for public (1000 mSv y 1) according to ICRP (1990). The external hazard index is an evaluation of the hazard of the natural gamma radiation which obtained from Raeq expression through the assumption that its maximum value allowed (equal to 1 unity) corresponds to the upper limit of Raeq (370 Bq kg ). This index value must be less than unity in order to keep the radiation hazard insignificant. The external hazard index (Hex) values range Fig. 9. Distribution of shore sediment samples in Marsa Alam-Shalateen Area. from 0.0.046 to 37 and from 0.074 to 0.22 for soil and sediment samples with averages 0.13 and 0.17, respectively. Internal hazard recommended by NEA-OECD (1979) and UNSCEAR (2000). index (Hin) values range from 0.063 to 0.46 and 0.086 to 0.27 for soil Representative level Index (Iɤr) is used to estimate the radioac- and sediment samples with averages 0.16 and 0.22 respectively. tivity hazard due to gamma radiation associated with the natural Both the external hazard and internal hazard indices values are less radionuclides (Ra-226, Th-232 and K-40), The calculated values of than the world permissible value of unity (Orgun et al., 2007). This 1 Representative level Index (Iɤr) range from 0.128 to 1.05 Bq kg indicates that the values will not lead to respiratory diseases such (0.48 Bq kg 1, in average) and from 0.21 to 0.632 Bq kg 1 (0.37 as asthma and cancer and external diseases such as erythema, skin Bq kg 1, in average) for soil and sediment samples, respectively. cancer and cataracts. These values are less than the world permissible value of unity The excess lifetime cancer risk (ELCR) gives the probability of (Orgun et al., 2007), except one value (1.05 Bq kg 1) for soil sample developing cancer over a lifetime at a given exposure level, No 3. considering 70 years as the average duration of life for human being The external terrestrial g-radiation absorbed dose rate in air at a (Taskin et al., 2009). The results: values range from (0.28 10 3)to height of about 1 m above the ground was calculated by using (0.035 10 3) and (0.17 10 3) to (0.059 10 3) mSv y 1 for soil conversion factor to transform specific activities of Ra-226, Th-232, and sediment samples with means (0.13 10 3) and (0.10 10 3) and K-40, respectively, in absorbed dose rate (in nGy h 1 by mSv y 1, respectively. The values of excess lifetime cancer risk Bq kg 1) are calculated by the Monte Carlo method (UNSCEAR, (ELCR) for all samples are less than the world average of 1998). The absorbed gamma dose rate values range from 8.2 to (0.29 10 3)(Taskin et al., 2009). 66.5 and 13.63e40.34 nGy h 1 for soil and sediment samples with 1 averages 30.5 and 23.6 nGy h , respectively. All values are lower 4. Conclusion than the world average terrestrial dose rate (57 nGy h 1) 1 (UNSCEAR, 2000), except for soil sample No.3 (66.5 nGyh ). Currently (2016) few radiological data are available for the

Table 8 Activity concentrations and the calculated hazard indices for shore sediment samples, Marsa Alam-Shalateen Area.

Sample No. Ra -226 ± err Th-232 ± err K-40 ± err Raeq Ig r D AGED AEDE Hex Hin ELCR x 103

1 4.42 ± 0.30 4.90 ± 0.40 206.44 ± 4.48 27.32 0.216 13.63 99.00 16.72 0.074 0.086 0.059 2 8.36 ± 0.54 7.00 ± 0.70 317.97 ± 6.00 42.85 0.338 21.38 155.00 26.21 0.116 0.138 0.092 3 5.58 ± 0.33 5.12 ± 0.50 220.28 ± 4.66 29.86 0.235 14.87 107.86 18.24 0.081 0.096 0.064 4 16.13 ± 0.81 16.6 ± 0.82 547.79 ± 7.45 82.05 0.639 40.34 291.35 49.47 0.222 0.265 0.173 5 23.45 ± 0.97 19.12 ± 1.09 337.97 ± 6.15 76.82 0.573 36.39 258.60 44.63 0.208 0.271 0.156 6 6.59 ± 0.54 6.39 ± 0.63 198.00 ± 5.80 30.97 0.240 15.16 109.28 18.59 0.084 0.101 0.065 Unit Bq/Kg Bq/Kg Bq/Kg Bq/Kg Bq/Kg nGy h 1 mSv y 1 mSv y 1 mSv y 1

Table 9 Pearson correlation coefficients (r) for activity concentrations and elevations parameters, shore sediment samples.

Ra-226, Bqkg 1 Th-232, Bqkg 1 K-40, Bqkg 1 Elevation, m (above mean sea level)

Ra-226, Bqkg 1 1 Th-232, Bqkg 1 0.980 1 K-40, Bqkg 1 0.643 0.755 1 Elevation, m (above mean sea level) 0.316 0.244 0.333 1

Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006 A.A. Arafat et al. / Journal of Radiation Research and Applied Sciences xxx (2016) 1e14 13 natural resources (water, soil and shore sediments) in Marsa Alam- Al-Gamal, S. A., & Nada, A. A. (2000). In Isotopic dynamics of groundwater resources Shalateen area, Red Sea coast, Egypt. The present work provides in Halayib and Shelatin district, red sea, Al-Azhar Univ. Engin. Jurn. Proceeding of Al-Azhar 6 Intern.Conf (pp. 15e25). information dealing with activity concentration, distribution and Avwiri, G. O., Osimobi, J. C., & Agbalagba, E. O. (2012). Evaluation of radiation hazard associated hazards of Ra-226 (U-238) series, Th-232 series, K-40 indices and excess lifetime cancer risk due to natural radioactivity in soil profile and Cs-137 radionuclides in these resources. Such information of Udi and Ezeagu local government areas of Enugu state, Nigeria. Compre- hensive Journal of Environmental and Earth Science, 1(1), 1e10. should be known before executing the economic projects related to Azab, M. A. (2009). In Flood hazard between Marsa Alam-Ras Banas, red sea, Egypt: the development process in the area. This work is based on field Fourth environmental conference, Faculty of Science (pp. 17e35). Zagazig and laboratory measurements. The field work included some University. Baha El Din, S. M. (2001). Important bird areas in Africa and associated islands e measurements dealing with water resources (pH, TDS and Egypt. available online: http://www.birdlife.org. groundwater wells dimensions). From the area under investigation, Beretka, J., & Mathew, P. J. (1995). Natural radioactivity of Australian building ma- 30 water samples (15 groundwater, 7 sea water, 4 desalinized water terials, industrial wastes and byproducts. Health Physics, 48,87e95. Bowen, H. J. M. (1979). Environmental chemistry of the elements. London, UK: Aca- and 4 wastewater samples), 33 soil and 6 shore sediments samples demic Press, 333 pp. were collected in 2015 from the main wadis (valleys) and coastal Bui, E. N., Mazullo, J., & Wilding, L. P. (1990). Using quartz grain size and shape plain. The samples were analyzed for Ra-226 (U-238) series, Th-232 analysis to distinguish between aeolian and fluvial deposits in the Dallol Bosso e series, K-40 and Cs-137 radionuclides using Hyper-Pure Germa- of Niger (West Africa). Earth Surface Processes and Landforms, 14,157 166. Chau, D. C., Dulinski, M., Jodlowski, P., Nowak, J., Rozanski, K., Sleziak, M., et al. nium (HPGe) detector. The results indicated that the activity con- (2011). Natural radioactivity in groundwater e a review. Isotopes in Environ- centrations of Cs-137 radionuclide in all samples are under the mental and Health Studies, 47(No. 4), 415e437. fi detection limit of the used analytical procedures. Compton, R. R. (1962). Manual of eld geology. (New York): John Wiley and Sons, Inc, 378p. Within Marsa Alam-Shalateen area, the activity concentrations Currie, L. A. (1968). Limits for qualitative detection and quantitative determination. in water resources (groundwater, sea water, desalinization water Application to radiochemistry. Analytical Chemistry, 40(No. 4), 586e593. and wastewater) varied widely. The Th-232 activity was under the EGSMA (Egyptian Geological Survey and Mining Authority. (1991). Basement rocks of Marsa Alam Quadrangle, Egypt, sheet No. NG 36 H1, Scale 1: 100,000. Cairo, detection limit in the major part of the water samples. The Ra-226 Egypt: Ministry of Industry and Technology, EGSMA. 1 1 activity ranged from <0.7 to 7.6 Bq L and from <0.7 to 6.31 Bq L EGSMA (Egyptian Geological Survey and Mining Authority). (1997). Geologic map of for groundwater and sea water samples, respectively. The fresh Hamata Quadrangle Egypt, sheet No. NG 36 G, Scale 1: 250,000. Cairo, Egypt: EGSMA. water of the desalinization plants and wastewaters from them were El Mamoney, M. H., & Khater, A. E. M. (2004). Environmental characterization and clear of Ra-226, except the wastewaters of Marsa Alam plant 2 and radio-ecological impacts of non-nuclear industries on the Red Sea coast. Journal Marsa Homeira show 6.87 and 10.66 Bq L 1 respectively. The K-40 of Environmental Radioactivity, 73, 151e168. < 1 < 1 < EL Saharty, A. A., & Dar, M. A. (2008). The concentration levels of some isotopic ranged from 3 to 32.84 Bq L , from 3 to 38.17 Bq L , from 3to radionuclides in the coastal sediments of the Red Sea, Egypt. 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Please cite this article in press as: Arafat, A. A., et al., Distribution of natural radionuclides and assessment of the associated hazards in the environment of Marsa Alam-Shalateen area, Red Sea coast, Egypt, Journal of Radiation Research and Applied Sciences (2016), http:// dx.doi.org/10.1016/j.jrras.2016.11.006