Natural radioactivity levels and heavy metals in chemical and organic fertilizers used in Kingdom of Saudi Arabia

The present work deals with identifying and determining the activity levels of natural occuring radionuclides, (226)Ra and (232)Th series, their decay products and (40)K, in chemical and organic fertilizers used in Kingdom of Saudi Arabia. A total of 30 samples: 20 phosphatic fertilizers (single super-phosphate SSP and triple super-phosphate,TSP) and 10 organic fertilizers (cow, sheep and chicken) collected from markets and farms. The gamma-ray spectrometer consists of NaI(Tl) detector and its electronic circuit was used for measuring γ-ray spectra. The ranges of radioactivity levels of (226)Ra, (232)Th and (40)K in chemical fertilizers are 51.5±5.2-106.3±7.5, 5.1±1.6-9.9±3.2. and 462.6±21-607.3±14Bqkg(-1), respectively. The activities of (226)Ra, (232)Th and (40)K in natural fertilizers (cow, sheep and chicken) are lower than the activities in chemical fertilizers. The obtained data are compared with available reported data from other countries in literature. The Ra(eq) in chemical fertilizer ranges from 100.37 to 161.43Bqkg(-1) and in organic fertilizer ranges from 34.07 to 102.19Bqkg(-1), which are lower than the limit of 370Bqkg(-1) adopted from NEA-OECD (1979). The average heavy metal (Pb, Cd, Ni, Co and Cr) contents of the fertilizers marketed in the Kingdom of Saudi Arabia are also determined and within the limits of those used worldwide.     

Natural radioactivity in Algerian building materials.

Samples of natural and manufactured building materials collected from Algiers have been analysed for 226Ra, 232Th and 40K using a high-resolution HPGe gamma-spectrometry system. The specific concentrations for 226Ra, 232Th and 40K, from the selected building materials, ranged from (12-65 Bq kg(-1)), (7-51 B qkg(-1)) and (36-675 Bq kg(-1)), respectively. The measured activity concentrations for these natural radionuclides were compared with the reported data of other countries and with the world average activity of soil. Radium-equivalent activities were calculated for the measured samples to assess the radiation hazards arising from using those materials in the construction of dwellings. All building materials showed Ra(eq) activities lower than the limit set in the OECD report (370 Bq kg(-1)), equivalent to external gamma-dose of 1.5 mSv yr(-1).     

Study of natural radioactivity and the state of radioactive disequilibrium in U-series for rock samples, North Eastern Desert, Egypt.

Twenty rock samples collected from North Eastern Desert in Egypt have been investigated. Natural radionuclide contents have been measured by gamma-ray spectrometry employing a shielded HPGe detector. The activities of (238)U, (232)Th and (40)K have been determined in Bq/kg dry weight. The absorbed dose rate of gamma radiation ranged from 100.48 to 22,140.53 nGy/h. The representative external hazard index values (H(ex)) for the corresponding samples were estimated. In the present work, the state of radioactive disequilibrium in the U-series at Wadi Baligh area was studied. The activity ratios between (226)Ra/(214)Pb and (214)Pb/(214)Bi were measured. The thorium-to-uranium concentration ratios (Clark value) were also estimated.     

Radiological impact assessment to the environment due to waste from disposal of porcelain

The present study aimed to assess the radiological parameters from gamma rays due to the uncontrolled disposal of porcelain waste to the environment. Qualitative and quantitative identification of radionuclides in the investigated samples was carried out by means of a high-purity germanium (HPGe) detector. The average activity concentrations of the local porcelain samples were measured as 208.28?Bq/kg for ²²⁶Ra, 125.73?Bq/kg for ²³⁸U, 84.94?Bq/kg for ²³²Th and 1033.61?Bq/kg for ⁴⁰K, respectively. The imported samples had an average activity of 240.57?Bq/kg for ²²⁶Ra, 135.56?Bq/kg for ²³⁸U, 115.74?Bq/kg for ²³²Th and 1312.49?Bq/kg for ⁴⁰K, respectively. Radiological parameters and the radium equivalent Ra_eq for the investigated samples were calculated. The external and internal hazard indices, representative level index (I_γ), alpha index (I_α), and the exemption level (I_x), were estimated to be higher than the recommended value (unity), while the average activity concentrations for the studied samples were higher than recommended levels. In conclusion, we are concerned that disposal of porcelain in the environment might be a significant hazard.     

Radioactivity levels of recent sediments in the Butrint Lagoon and the adjacent coast of Albania.

Sediment samples have been collected in the Butrint area, located in the south-west Albania to determine the radioactivity levels of (40)K, (137)Cs, (212)Bi, (212)Pb, (214)Bi, (214)Pb, (226)Ra and (228)Ac on the bed of the lagoon and adjacent sea, using direct counting gamma spectroscopy. The concentration of (137)Cs and (40)K varied from 2.8 to 37.5 Bq/kg and from 266 to 675 Bq/kg dry weight (dw), respectively (central values). The average concentrations of (238)U and (232)Th daughter products varied from 8 to 27 Bq/kg and from 13 to 40 Bq/kg dw, respectively. The measured (235)U activity ranged from 0.7 to 2.5 Bq/kg dw. Samples of different sedimentary properties, studied for the radioactivity concentration, revealed an inversely proportional relation between grain size and a linear combination of measured specific activities of (226)Ra, (232)Th ((228)Ac, (212)Bi and (212)Pb), (40)K and (137)Cs.     

Behavior and environmental impacts of radionuclides during the hydrometallurgy of calcareous and argillaceous rocks, southwestern Sinai, Egypt

The hydrometallurgy of radionuclides means getting the radioelements from the rocks into solution by leaching, getting the radionuclides from the solution by extraction process, and then precipitation of the desired elements to obtain concentrate. The follow-up of the radionuclides during these processes is the main target of this work to identify the identity of the original samples, pregnant solutions (leachates), residuals and the concentrate. Six samples were chosen to achieve this work. The leaching process was carried out under the conditions; 20-30% acid (H(2)SO(4)) concentration, 1:3 solid/liquid ratios, 60 min stirring time at room temperature. The activity concentrations of (238)U, (235)U, (234)U, (226)Ra, (214)Pb, (214)Bi, (232)Th and (40)K were measured in the original samples, residuals and U-concentrate (Bq/kg), and leachates (Bq/?). The results indicate that, the radionuclides before (226)Ra in the (238)U decay series are more leachable (released) than those from (226)Ra to (214)Bi in the order; (234)U>(238)U=(235)U > (226)Ra>(214)Pb>(214)Bi. (232)Th and (40)K are immobile under the present conditions. The radiological hazards of natural radioactivity in the original samples, leachates, residuals and U-concentrate were calculated and compared with the internationally recommended values and were found to be much higher than the world average values.     

Correction for radon distribution in solid/liquid and air phases in gamma-ray spectrometry

The effect of radon diffusion and distribution between a (226)Ra matrix and the top air gap inside sample containers for gamma-ray spectrometry was studied. Containers filled at almost 100% or just 70% of total capacity yielded correction factors of about 7% and 20% respectively. Applying these correction factors allowed activity values calculated from (226)Ra or radon decay products to agree within 2%.     

Disequilibrium in naturally occurring radioactive series in some phosphate ores

Eight phosphate ore samples from Egypt and Saudi Arabia were studied by atomic absorption spectrometry for the Bi, Pb, Th and Al concentrations in ppm or ppb or per cent. Also X-ray diffraction spectrometry was applied for determining the mineral and chemical composition of the phosphate ore samples. A gamma spectrometry system, based on HPGe crystal, was applied for determining the concentrations of the radioactive elements in (238)U, (226)Ra and (232)Th series as well as (40)K, in Bq/kg dry weight. Concentrations in ppm were found to be from <10.0 to 20.48, from <7.50 to 27.30 and from <1.0 to 50.0 for Bi, Pb and Th, respectively. Al ranged from <0.05 to 3.13%. Major, minor and trace chemical and mineral compositions were assigned for each sample by XRD spectrometry. Concentrations of the different elements in both radioactive series, (238)U, (226)Ra and (232)Th were compared. Disequilibrium was found in both series.     

云南省部分地区大米和玉米放射性核素水平调查

目的 调查云南省部分地区大米和玉米放射性核素水平,充实云南地区食品放射性水平基线数据,评估其对居民产生的健康风险。方法 依据国家标准《生物样品中放射性核素的γ能谱分析方法》《高纯锗γ能谱分析通用方法》《食品中放射性物质检验总则》《土壤中放射性核素的γ能谱分析方法》,对云南省20个县（区）大米和玉米样品进行放射性核素检测,对检测结果进行处理与分析。结果 大米样品中²³⁸U、²³²Th、²²⁶Ra、⁴⁰K和¹³⁷Cs活度浓度均值分别为（0.416±0.403）、（0.045±0.034）、（0.030±0.013）、（28.4±18.8）和（0.014±0.019）Bq/kg,玉米样品中²³⁸U、²³²Th、²²⁶Ra、⁴⁰K活度浓度均值分别为（0.308±0.230）、（0.035±0.031）、（0.053±0.072）、（56.8±38.6）Bq/kg,¹³⁷Cs的活度浓度低于探测下限。结论 云南省20个县（区）大米和玉米中²³⁸U、²³²Th、²²⁶Ra、⁴⁰K和¹³⁷Cs的放射性水平均在国家标准正常范围内,食入后不会对居民的健康造成影响。     

Natural radioactivity and gamma dose from Sri Lankan clay bricks used in building construction.

The specific radioactivity concentrations of 226Ra, 232Th and 40K have been determined by gamma ray spectrometry with an HPGe detector in clay brick samples from kiln sites located in 17 towns. The average values of the measured activities are 35, 72, and 585 Bq kg(-1), respectively, for the above radionuclides. The average estimated radium equivalent concentration is 183 Bq kg(-1) and is comparable with reported values for many countries in the world. This value and the value obtained from the criteria formula suggest that the use of local clay bricks do not pose a radiological hazard. The calculated average absorbed dose rate in air within buildings was found to be 102 nGy h(-1) while the population weighted indoor annual effective dose was 0.20 mSv.     

Relationship between radioactivity of radium and concentrations of barium and lead in hokutolite

Hokutolite consists of barite (BaSO₄) and anglesite (PbSO₄), and contains significant amounts of radium isotopes as a radioactive mineral. Photon activation and gamma-ray spectrometry were employed to determine Ba, Pb and ²²⁶Ra contents in hokutolite samples and to investigate the correlation between ²²⁶Ra activity and both Ba and Pb content. ²²⁶Ra activity in 30 hokutolite samples were estimated in the range of 40–65 Bq/g and was positively related to Ba content (r=0.859, p<0.001), but independent of Pb content (r=−0.236, p=0.217). Experimental results implied that ²²⁶Ra preferably precipitated with Ba over Pb. The ²²⁶Ra activity in hokutolite from the Peitou Hot Spring was experimentally estimated based on the Ba/Pb ratio and expressed as ²²⁶Ra (Bq/g)=14.67 (Ba/Pb)_molar+14.13.     

Distribution of radium in oil and gas industry wastes from Malaysia.

Radium concentrations in 470 samples of the various types of waste from oil and gas industries were analysed using gamma spectrometers. The results showed that the radium concentration varied within a wide range. The highest mean 226Ra and 228Ra concentrations of 114,300 and 130,120 Bq/kg, respectively, were measured in scales. Overall, 75% of the waste, mostly sludge and extraction residue lies within the normal range of radium concentration in soils of Malaysia. However, some platform sludge can have radium concentration up to 560 Bq/kg.     

Measurement of natural radioactivity levels in Indian foodstuffs by gamma spectrometry

Measurements of natural radioisotopes present in some of the foodstuffs which form the main components of the composite Indian diet are presented. Assessment of daily intake of these natural radionuclides has been made on the basis of the average daily intake of these food-items by the population of Bombay and its environment. The content of ⁴⁰K, ²²⁶Ra and ²²⁸Th radioactivity varies from 45.9 to 649.0 Bq/kg, 0.01 to 1.16 Bq/kg and 0.02 to 1.26 Bq/kg, respectively. The average daily intakes of ⁴⁰K, ²²⁶Ra and ²²⁸Th have been estimated as 105.6, 0.17 and 0.18 Bq d⁻¹, respectively for the period 1970–1982.     

Natural gamma-emiting radionuclides in Pakistani Portland cement.

Studies of the natural gamma-emitting radionuclides in Portland cement manufactured in the North West Frontier Province (NWFP) of Pakistan and the various raw materials which compose the product have been carried out using gamma-spectrometric techniques. For data acquisition a high-purity germanium detector (HPGe) was used. The range of the total specific activity (minimum and maximum values) due to all the three radionuclides (40K, 226Ra and 232Th) were found to be 187.8+/-63.5-573.2+/-73.1 Bq kg(-1) (Portland cement); 54.5+/-16.1-183.9+/-31.4 Bq kg(-1) (limestone); 87.1+/-30.7-297.1+/-64.4 Bq kg(-1) (gypsum); 696.4+/-79.1-1043.9+/-85.0 Bq kg(-1) (slate); and 490.9+/-54.5-570.2+/-59.8 Bq kg(-1) (latrite). The average specific activities due to 40K in Portland cement and all the raw materials were found to be higher when compared with 226Ra and 232Th. Such materials do not pose any excess radiological health problem.     

Spatial and monthly variations of radium isotopes in produced water during oil production.

Spatial and monthly variations of radium isotope concentrations in produced water have been evaluated during oil production. Samples of produced water were collected and analyzed on a monthly basis over a period of 5 months, the samples being derived from 11 main oil production wells at three Syrian oilfields. The highest average 226Ra, 228Ra and 224Ra concentrations in these samples of water were found to be 41, 37.5 and 1.1 Bql(-1), respectively. The data obtained for 226Ra, 228Ra and the 228Ra/226Ra activity ratio were evaluated statistically and displayed using the Box Plot method; clear variations can be observed from one field to another, indicating differences in the geological formation of the reservoir. The 228Ra/226Ra activity ratio variations reflect the variability of the Th/U mass ratio of the geological formation, suggesting two different source rock types. The calculated mean Th/U mass ratio for these two possible types of source rock were 2.4 and 5.78. In addition, the 228Ra/226Ra mean activity ratio was also used to estimate the age of some deposited scales in tubulars; the results were compared with the 224Ra/228Ra activity ratio dating method. Monthly variations of 226Ra and 228Ra activity concentrations and the 228Ra/226Ra activity ratio in produced water were also observed, the major causes for these variations being related to the type of injection water and interwell reactions. Possible relationships between 226Ra and 228Ra activity concentrations, the 228Ra/226Ra activity ratio and physical and chemical properties of produced water were statistically evaluated; no linear correlations were found.     

A source for measurement of the absolute intensities of 226Ra gamma-radiation in equilibrium with decay products.

The design and production techniques of a gamma-ray spectrometric source of 226Ra in equilibrium with its daughter decay products have been developed. The radon emanation coefficient of the source did not exceed 0.1%. The 226Ra activity in the gamma-ray spectrometric source was measured relative to that in an alpha-particle spectrometric source by comparison of the intensities of the main gamma rays using a semiconductor gamma-ray spectrometer. The total uncertainty of the activity measurement results was 0.5% for a coverage factor of k = 2.     

Accounting for 222Rn loss during oven drying for the immediate laboratory gamma-ray spectroscopy of collected soil samples.

Drying soil samples in an oven to remove water alters the 222Rn emanation rate. Measurements of the oven drying 222Rn emanation rate from soil were made with a continuous radon monitor and the degree of 222Rn disequilibrium was quantified by laboratory gamma-ray spectroscopy. This paper presents a disequilibrium correction where the 226Ra activity in oven-dried soil samples is inferred from immediate laboratory gamma-ray spectroscopy of 214Bi before 222Rn and its decay progeny reach secular equilibrium.     

Precise determination of photon emission probabilities for the main X- and gamma-rays of 226Ra in equilibrium with daughters.

Within the context of a joint project between VNIIM (D.I. Mendeleyev Institute for Metrology) and LNHB (Laboratoire National Henri Becquerel), special 226Ra sources were prepared by VNIIM in order to determine as accurately as possible the absolute photon emission probabilities for the main X- and gamma-rays following the decay of 226Ra and daughters. The main purpose of this work was to supplement a previous joint study by Laboratorio Nacional de Metrologia das Radia?oes Ionizantes (LNMRI) and LNHB to determine their relative values. Some specific point sources were produced for alpha-spectrometry measurements that were undertaken at VNIIM and also for gamma-ray spectrometry studies at VNIIM and LNHB. The 226Ra activity for the gamma-spectrometric sources was measured relative to the alpha-spectrometric sources by comparing the counts of the main gamma-rays. The total uncertainty of the activity for these sources was 0.2% (k = 1). Using calibrated germanium detectors, several X- and gamma-ray spectra were analyzed to determine the absolute photon emission probabilities of 226Ra in radioactive equilibrium with daughters. The results are presented and compared to other published values.     

Natural radioactivity levels in granitic plutons and groundwaters in Southeast part of Eskisehir, Turkey.

The present work investigated the radioactivity level of the granitoid plutons and its effect on the groundwaters in the southeast part of Eskisehir. Fourteen granitic samples from the Kaymaz and Sivrihisar plutons and 11 groundwater samples from the near vicinity of the pluton were analyzed. The activity concentrations measured for (238)U and (232)Th ranged from 43.59+/-2 to 651.80+/-24 Bq/kg, and 51.16+/-3 to 351.94+/-13 Bq/kg, respectively. The activity concentrations obtained for (40)K varied from 418.50+/-17 to 1618.03+/-66 Bq/kg. The absorbed dose rates in air outdoors ranged from 87.14 to 531.81 nGy/h. All the results obtained from the Kaymaz pluton are higher than those from the Sivrihisar. The U (ave. 16.6 ppm) and Th (ave. 49.9 ppm) values of the Kaymaz pluton are higher than the average concentrations of the magmatic rocks of granitic composition. These results are consistent with high dose rates of the pluton. The gross-alpha activities in the groundwater samples ranged from 0.009 to 1.64 Bq/l and the gross-beta activities from 0.006 to 0.89 Bq/l. The highest gross-alpha value was found in the sample taken from near the Kaymaz pluton. The concentrations of (222)Rn varied from 0.060 to 0.557 Bq/l.     

Distribution of scales containing NORM in different oilfields equipment.

Evaluation has been made of the distribution of hard scales containing naturally occurring radioactive materials (NORM) in a range of oilfield equipment in Syrian oilfields. One hundred and fifty-two scale samples from oilfield equipment were collected and analysed for radioactivity, elemental and mineralogical compositions. The average 226Ra, 228Ra and 224Ra concentrations in scales were found to be 174, 91 and 67 Bqg(-1), respectively; the highest value of 226Ra was found to be 1520 Bqg(-1). A gradual increase in 226Ra specific activity from down-hole tubulars to surface parts of the installations was observed. The 228Ra/226Ra mean activity ratio was observed to be 0.76, indicating a Th/U mass ratio of about 2.3. This value can be considered a fingerprint for the Th/U mass ratio of the geological formation of the reservoir. Radium isotopic data were also used to estimate the age of the deposited scales using the 224Ra/228Ra activity ratio; the highest average age (5.3 years) was found to be in scales collected from valves. Multiple regressions of the data have shown that 226Ra is more highly correlated with Ba and Sr content in scales (R2=0.92) than Ca. Around 77% of 226Ra was found to be incorporated with anhydrate barium strontium sulphate (R2=0.93), solubility in water being very low to negligible; lower levels of radium isotopes were found in calcite.