Natural radioactivity in Al-Lajjun region Jordan soil by gamma-ray spectroscopy

doi:10.21203/rs.3.rs-3291464/v1

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Natural radioactivity in Al-Lajjun region Jordan soil by gamma-ray spectroscopy

https://doi.org/10.21203/rs.3.rs-3291464/v1

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Activity concentrations of primordial radionuclides in soil samples collected from the Al-Lajjun region were measured using a γ-ray spectrometry system using pure germanium (HPGe) detector in a low background configuration. The mean activity concentrations for ⁴⁰K, ²²⁶Ra, ²³²Th, ²³⁸U, ²³⁵U, and ²⁴¹Am at different locations of Al-Lajjun/Karak/Jordan were found to be in the range of 12–560, 234–6037, 4.3–28.4, 459-54147, 43-3656, 43-3332 Bq/Kg, respectively. The obtained values of some samples are much greater than the world average values except for ⁴⁰K and ²³²Th. Radium equivalent activity, absorbed dose rate, and annual effective dose equivalent were calculated for assessing the assessment of radiological risk. The external hazard value (Hex) is between 0.638 and 16.316. In the present study. ²³⁸U concentration is much higher than the acceptable value reported by UNSCEAR-2000.

Gamma-ray spectrometry

Annual effective dose

External hazard index. Natural radioactivity

238U

226Ra

232Th

40K

High-purity germanium detector (HPGe) was used to measure the activity concentration of gamma-emitting radionuclides in the collected soil samples at different locations in the world. The researchers studied the collected soil samples from different regions, besides rivers, coastal beaches, phosphate, types of cement, medical plants, and so on [1–10]. Similarly, our colloquies in Jordanian universities studied the different regions of Jordan from north to south and from east to west. They studied irrigation water, drinking water, milk products, and dust [11–27].

It is well-recognized that radioactivity is a natural occurrence in the environment. ²³⁸U, ²³²Th, and ⁴⁰K are the most prevalent radioactive elements on Earth that emit gamma rays. The levels of natural ambient radioactivity in the soils of various geological regions vary and rely on the underlying geological conditions. The primary source of natural radioactivity contamination and the main source of radiation exposure to people comes from primordial radionuclides like ⁴⁰K and radioisotopes from the ²³⁸U and ²³²Th series, as well as their byproducts in the surface soil.

The major goals of the current study are to examine the level of radioactive elements like radium, thorium, and potassium in Jordan's Al-Lajjun region to determine the potential health risks and to get the industry ready for the day when nuclear reactors would be used to generate power. In addition, we will concentrate on a location rich in various minerals to discover its various radiation components. To finish a survey of the environmental radioactivity in Jordanian locations, we will look into the Al-Lajjun regions.

2.1. Sampling

In the present study, nine soil samples were collected from different locations in the Al-Lajjun region (Karak Province) on a random basis. Soil samples were properly marked and then sent to the lab to be processed. After collection, samples were crushed into fine powder by using a mortar and pestle. The fine quality of the samples is obtained using a scientific sieve of small mesh size. The mass of each soil sample was measured precisely using a 0.001-gram balance. Each sample is weighted, packed, and sealed in an airtight PVC container. Before experimentation, the samples were collected and saturated for up to 40 days. This amount of time is sufficient to ensure that the parent nuclides are in secular equilibrium with their daughter nuclides.

2.2. Measurement of Natural Radioactivity

The sample activity was counted using a high-purity germanium (HPGe) detector based on a high-resolution gamma spectrometry system. GAMMA-X (GMX) N-type coaxial HPGe detector is made for high-performance gamma spectroscopy in the energy range of 3 keV up to 10 MeV. The GMX detector is a coaxial Germanium (Ge) detector with an ultra-thin entrance window. The entrance window of the detector is a 0.3-µm-thick, ion-implanted contact, extending the lower range of useful energies to around 3 keV. Ion implantation results in a stable contact that will not deteriorate with repeated cycling. Moreover, the N-type HPGe detector is resistant to damage by fast neutrons. The detector is shielded with lead on all sides to reduce the background level of the system. (The detector is manufactured by EG&G, ORTEC, Oak Ridge, USA). Cryogenic cooling is required for germanium semiconductor radiation detectors, so a liquid nitrogen system is used. Before experimenting, the system was calibrated to produce a Gamma spectrum of intensity (number of counts/s) versus energy in MeV. Four sources were used to calibrate the MCA (Multi-Channel Analyzer), 60Co with two energy peaks of 1173.24 keV and 1332.50 keV, 137Cs with an energy peak of 661.67 keV, 133Ba (356.01 keV), and 241Am (59.54 keV). The detector has a resolution of 2.0 keV and a relative efficiency of 20% for the 1.332 MeV gamma energy of ⁶⁰Co. The output of the detector was analyzed using a 4K multichannel analyzer system connected to a PC.

The spectrum for each sample was collected for a counting time of 86400 seconds to reduce statistical errors. The results (gamma-spectra) were analyzed using Genie 2000 spectroscopy software (Canberra, 2004).

2.3 Geological Area of the Samples

The sampling site is exactly at the left abutment of the Al-Lajjun Dam. Al-Lajjun Dam is located in Al-Karak Governorate, on valley Al-Ghobyan, approximately 1 km from the main street of Al-Karak, at the latitude and longitude of 31^o13’55’’N 35^o51’00’’E Fig. 1.

The geology of the Dam site begins with Amman Silicified Limestone (ASL) of Campanian age with 30–55 m thickness, consisting of bedded brown-black chert that is interbedded with limestone, marl, granule phosphatic chert, and 8m of oyster-coquina limestone. Overlain by the Al-Hisa Phosphorite (AHP) formation of Campanian-Maastrichtian with a 40–6 m thickness of interbedded phosphatic chert, granular phosphatic limestone, micritic limestone, and marl, the upper part of the thickness range is 2–15 m composed of phosphatic chert, phosphatic limestone, marly limestone, and marl. At the surface, outcrops the alluvial deposits of Pleistocene–Holocene age. The surficial yellowish uranium mineralization was found mainly within the AHP formations as veins along joints and as encrustation in marly limestone, phosphatic chert, marl, and phosphatic limestone layers of the upper part of AHP as illustrated in Fig. 1. These deposits were outcrops due to the dam excavation works.

Using the identified gamma peaks from the obtained spectra, the activity concentration A for the radionuclides ⁴⁰K, ¹³⁷Cs, ²²⁶Ra, ²³²Th, and ²³⁸U was determined. The concentration of ⁴⁰K activity is calculated directly from its gamma line (1461.8 keV, yield = 10.67%). The radium (²²⁶Ra) activity concentration $\varvec{A}\left({}_{88}{}^{226}\varvec{R}\varvec{a}\right)$ is calculated from the photo peaks of its daughters ²¹⁴Bi (energy line 609.3 keV, yield = 46.3%) and ²¹⁴Pb (energy line 351.9 keV, yield = 37.2%), which are provided by:

$$\varvec{A}\left({}_{88}{}^{226}\varvec{R}\varvec{a}\right)=\left(\frac{{\varvec{A}}_{\varvec{B}\varvec{i}}}{{\varvec{\sigma }}_{\varvec{B}\varvec{i}}^{2}}+\frac{{\varvec{A}}_{\varvec{P}\varvec{b}}}{{\varvec{\sigma }}_{\varvec{P}\varvec{b}}^{2}}\right)/\left(\frac{1}{{\varvec{\sigma }}_{\varvec{B}\varvec{i}}^{2}}+\frac{1}{{\varvec{\sigma }}_{\varvec{P}\varvec{b}}^{2}}\right)$$

where A is the activity concentration and σ is the uncertainty in A. The activity concentration A of ²³²Th is determined from the photo peaks of its daughters: ²²⁸Ac (line energy 911.60 keV, yield = 27.7%), ²⁰⁸Tl (line energy 583.0 keV, yield = 30.9%), and ²¹²Pb (line energy 238.62 keV, yield = 44.6%), as given by:

$$\varvec{A}\left({}_{90}{}^{232}\varvec{T}\varvec{h}\right)=\left(\frac{{\varvec{A}}_{\varvec{A}\varvec{c}}}{{\varvec{\sigma }}_{\varvec{A}\varvec{c}}^{2}}+\frac{{\varvec{A}}_{\varvec{T}\varvec{l}}}{{\varvec{\sigma }}_{\varvec{T}\varvec{l}}^{2}}+\frac{{\varvec{A}}_{\varvec{P}\varvec{b}}}{{\varvec{\sigma }}_{\varvec{P}\varvec{b}}^{2}}\right)/\left(\frac{1}{{\varvec{\sigma }}_{\varvec{A}\varvec{c}}^{2}}+\frac{1}{{\varvec{\sigma }}_{\varvec{T}\varvec{l}}^{2}}+\frac{1}{{\varvec{\sigma }}_{\varvec{P}\varvec{b}}^{2}}\right)$$

When they are in secular equilibrium, the activity concentration of ²³²Th can likewise be estimated from the activity of ²²⁸Ra. Finally, the ²³⁵U activity concentration is calculated using the photo peak line (186.2 keV, yield = 57.2%) that overlaps with the ²²⁶Ra photo peak line (185.7 keV, yield = 3.28%). The activity of ²³⁵U is:

$$\varvec{A}\left({}_{92}{}^{235}\varvec{U}\right)=\varvec{A}\left({}_{88}{}^{226}\varvec{R}\varvec{a} \varvec{a}\varvec{t} 186\varvec{k}\varvec{e}\varvec{V}\right)-\varvec{A}\left({}_{88}{}^{226}\varvec{R}\varvec{a}\right)$$

Figures 3 and 4 show examples of the obtained gamma spectrum for samples 4 and 6. The highest number of counts per second in Fig. 2 is 20000 counts/s, whereas in Fig. 4 it is 2000 counts/s (the activity is one-tenth of the first one). This disparity may be explained by the varying uranium concentrations in some collected samples. Table 1 presents an overview of the obtained findings relating to the various samples. We have one sample from the Aqaba region in the south of Jordan, which gives a normal case, concerning the acceptable range of activity concentration.

The acquired data show that we have high activity concentration levels in numerous samples compared to the global average concentrations. The Aqaba sample demonstrates the typical activity. To ensure the accuracy of the results, we sent the samples to the Jordan Atomic Energy Commission (JAEC) for further examination using RID-SOP-006/Gamma ISO 18589-3 method. Consequently, the results of JAEC support the obtained values. Their results are tabulated in Table 2. Only the sample of Al-Lajjun6 shows ²³⁴Th with A = 36312 ± 500 and ¹³⁷Cs with A = 6.65 ± 3.35 Bq/Kg. The results are compared with previous results obtained from other scholars from different regions in Jordan in Table 3. There is a large activity concentration in some of the studied samples concerning previous studies.

Table 1

The activity concentration A (Bq/kg) of the collected samples of the radionuclides (⁴⁰K, ²²⁶Ra, ²³⁸U, ²³²Th, ²³⁵U)
Sample	A (⁴⁰K)	A (²¹⁴Bi)	A (²¹⁴Pb)	A (²²⁶R)	A (²³⁸U)	A (²³²Th)	A (²³⁵U)	A (²⁴³Am)
Samople0	110 ± 17	309 ± 4	610 ± 8	377 ± 4	3618	-	243 ± 13	3332 ± 370
Aqaba1	54 ± 13	223 ± 4	281 ± 4	250 ± 3	459	4.3 ± 0.7	43 ± 2	-
Al-Lajjun2	39 ± 33	1073 ± 10	1467 ± 11	1250 ± 7	6527	-	472 ± 11	199 ± 8
Al-Lajjun3	24 ± 10	205 ± 3	270 ± 3	234 ± 2	1451	-	102 ± 3	43 ± 2
Al-Lajjun4	-	-	16040 ± 115	-	-	-	2782 ± 54	789 ± 16
Al-Lajjun5	-	5526 ± 13	7502 ± 21	6037 ± 11	54147	-	3656 ± 69	709 ± 13
Al-Lajjun6	560 ± 71	3160 ± 23	4057 ± 21	3653 ± 15	4705	28.4 ± 0.3	463 ± 11
Al-Lajjun8	61 ± 35	1985 ± 12	2770 ± 12	2378 ± 8	16743	-	1161 ± 23
Al-Lajjun9	12 ± 20	1418 ± 7	1818 ± 8	1583 ± 5	4299	-	357 ± 8
Range	12–560	205–3160	270-16040	234–6037	459-54147	4.3–28.4	43-3656	43-3332
World average concentrations	400	-	-	35	-	30	-	-

Table 2. Results of activity concentration obtained by Jordan Atomic Energy Commission A²³⁸U.

Table 3

Activity concentrations in Bq/Kg in different studied regions in Jordan

Element/Region	⁴⁰K	²²⁶Ra(238U)	²³⁵U	²³²Th	²³⁸U	¹³⁷Cs
Zarqa 2016	212.87	211.44		11.10
Russaifa 2014	207.10	265.95		0.895
THE NORTHERN JORDAN RIFT VALLEY 2009	156.0	33	2.2	11.2		3.5
Maan 2014	138.1	57.7,44.9		18.1
The types of cement in 2022	354.70	79.52		30.99
Irbid 2013 Jordan University of Science and Technology	312.39	20.84		24.45	83.88	2.43
Amman Aqaba Highway 2003	560			82	84
urban areas in the southern governorates of Jordan 2018	233	39		23	45
urban areas of the northern highlands of Jordan 2009	291	42.5		26.7	49.9
Jordan Research and Training Reactor 2018	340.3					2.94-25
each governante of Jordan 2019	309	42		23		3.7
Araba Valley, Jordan 2008	94–762			14.3–35	19-38.7
The Aqaba Gulf 2010		626			57–677
Worldwide rang**	140–850	17–60		11–64
Worldwide Median Value*	400	35		30
Present Research	12–560	234–6037	43-3656	4.3–28.4	459-54147	6.65

The external hazard index (Hex) is given by a model proposed by Krieger (1981):

$${H}_{ex}=\left(\text{A}{}^{226}Ra/370\right)+\left(\text{A}{}^{232}Th/259\right)+\left(\text{A}{}^{40}K/4180\right)$$

H _ex must not exceed the limit of unity for the radiation hazard to be negligible. On the other hand, the internal hazard index (Hin) gives the internal exposure to carcinogenic radon and its short-lived progeny and is given by the following formula (Beretka and Mathew,1985):

$${H}_{in}=\left(\text{A}{}^{226}Ra/185\right)+\left(\text{A}{}^{232}Th/259\right)+\left(\text{A}{}^{40}K/4180\right)$$

The values of H_in must also be less than unity to have negligible hazardous effects of radon and its short-lived progeny on the respiratory organs (UNSCEAR, 2000). The gamma absorbed dose rate in the air out the doors, D at 1 m above the ground surface due to specific activity concentrations of ²³⁸U, ²³²Th, and ⁴⁰K is defined as given in Eq. (6), to the effective dose received by adults. However, D values were calculated by the following equation (UNSCEAR-2000):

D(nGy h ^− 1 ) = 0.462A ²³⁸ Ra + 0.604A ²³² Th + 0.0417A ⁴⁰ K (6)

where $\text{A}{}^{238}U$, $\text{A}{}^{232}Th$ and $\text{A}{}^{40}K$ are the activity concentration of ²³⁸U, ²³²Th and ⁴⁰K in Bq/kg, respectively. Exposure Radiation is defined in terms of many parameters. Radium equivalent activity (Raeq) is a widely used hazard index. It is calculated, as given by Eq. (7), assuming that 370 Bq/kg of ²²⁶Ra, 259 Bq/kg of 23kg, and 4810 Bq/kg of ⁴⁰K produce a gamma-ray dose rate (Beretka and Mathew, 1985):

$${Ra}_{eq}\left(\frac{Bq}{kg}\right)=\text{A}{}^{226}Ra+1.43\text{A}{}^{232}Th+0.077\text{A}{}^{40}K$$

where $A{}^{226}Ra$, $A{}^{232}Th$ and $A{}^{40}K$ are the activity concentration of ²²⁶Ra, ²³²Th, and ⁴⁰K in Bq/kg, respectively. Note the total value must be equal to or less than 370.

Annual Effective Dose Equivalent (AEDE) due to the activity of the samples was calculated using Eq. (8) (Emad Farrag 2016)

$$AEDE\left(mSv{y}^{-1}\right)=D\left(nGy{h}^{-1}\right)\times 8760\left(h{y}^{-1}\right)\times 0.2\times 0.7\left(SvG{y}^{-1}\right)\times {10}^{-6}$$

where the value 0.7 SvGy-1 is the conversion coefficient from the absorbed dose in the air to the effective dose received by adults, 8760 is the time in hours in one year, 0.2 represents the outdoor occupancy factor (UNSCEAR-2000), and is the observed dose rate. The calculated values are given in Table 4 :

Table 4

*Hex*, *Hin*, and the annual effective dose equivalent
Sample	Raeq (Bq/Kg)	D (nGy/h)	AEDE (mSv/y)	Hex	Hin
sample 0	385.36	178.64	0.219	1.045	2.063
Aqaba 1	260.18	179.02	0.220	0.705	1.380
Al-Lajjun2	1253.21	579.13	0.710	3.388	6.767
Al-Lajjun3	235.67	109.11	0.134	0.638	1.270
Al-Lajjun 4	-------	------	--------	--------	------
Al-Lajjun5	6036.86	2789.09	3.421	16.316	32.632
Al-Lajjun6	1643.56	1728.19	2.119	10.116	19.989
Al-Lajjun 8	2382.24	1101.18	1.350	6.434	12.866
Al-Lajjun9	1582.91	731.84	0.898	4.281	11.207

In the current study, the concentration levels of naturally occurring radioactive materials (NORMs) of ⁴⁰K, ²²⁶Ra, ²³²Th, ²³⁸U, ²³⁵U, and ²⁴¹Am in the surface soil samples of selected areas in Al-Lajjun/Jordan were investigated. The collected soil samples were analyzed employing gamma-ray spectrometry. The radioactivity concentration of the naturally occurring radionuclides ⁴⁰K, ²²⁶Ra, ²³²Th, ²³⁸U, ²³⁵U, and ²⁴¹Am in the soil samples varied from 12–560, 234–6037, 4.3–28.4, 459-54147, 43-3656, 43-3332 Bq/Kg, respectively. Radium equivalent activity, absorbed dose rate, and annual effective dose equivalent were also calculated for the assessment of radiological risk. The external hazard value (Hex) is between 0.638 and 16.316. In this study, ²³⁸U activity concentration is much higher than the acceptable value reported by UNSCEAR-2000. Some samples show very high average concentrations. The results were confirmed using another method to prove the obtained values. The locations studied have a very high concentration of activity.

Acknowledgments:

We would like to thank Dr. Eshraq Ababneh for her help in performing all the experiments at the Dababneh physics lab, and for her continuous fruiting discussions. Also, we appreciate the help of the Jordan Atomic Energy Commission (JAEC) in reinvestigating the studied samples.

Conflict of interest

We have no conflicts of interest to disclose.

All authors declare that they have no conflicts of interest.

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Natural radioactivity in Al-Lajjun region Jordan soil by gamma-ray spectroscopy

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Abstract

Figures

1. Introduction

2. Experimental Procedure

2.1. Sampling

2.2. Measurement of Natural Radioactivity

2.3 Geological Area of the Samples

3. Results and Data Analysis

4. Conclusions

Declarations

References

Additional Declarations

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