Determination of naturally occurring radioactive materials (NORM) in formation water during oil exploration

The present study is conducted, in order to contribute to a future waste management policy related to the presence of technologically enhanced natural occurring radioactive material (TENORM) in Iran petroleum industry. Samples were collected from offshore oil company for analysis of ²³⁸U, ²³⁵U, and ²³²Th series in produced waters. The activities of samples were determined by high-purity germanium detector, well for lowlevel activity γ-spectrometry. The results have shown that, ²²⁶Ra concentration ranges from 5.26 Bq/L to 27.93 Bq/L. Also the total activity in produced water is in the range of 16–840 Bq/L were mainly due to enhanced levels of dissolved ²²⁶Ra, ²¹⁴Pb, ²¹⁴Bi ions. Also, enhanced dissolution of elements such as radium by increasing of salinity, result in higher concentration of NORM in old oil region. Measured values are above EPA regulation (40 CFR 141055) & aqueous Derived Release Limit (DRL) of Canadian guideline for the management of (NORM). Therefore produced water has to dispose in pits which have to design for decrease the environmental effects. Also according to this study, re-injection of produced water in to abandon well of Iran Offshore Oil Company in Persian Gulf, have preference over discharging to the pits.     

First proficiency test for the determination of NORM in contaminated soil from the oil field

The Atomic Energy Commission of Syria (AECS), in cooperation with the Arabic Atomic Energy Agency (AAEA), has initiated the first proficiency test exercise for the determination of naturally occurring radioactive materials (NORM) in contaminated soil from the oil field. The soil sample was collected from one of the most highly radioactively contaminated lagoons with production water in the Syrian oil fields, which was then prepared, characterised and certified according to a standard procedure. Samples were dispatched to laboratories from eight Arab countries; Kuwait, Egypt, Yemen, Tunisia, Jordan, the Kingdom of Saudi Arabia, Libya and Syria. The results were evaluated using three statistical criteria; z-score, the U _test score and the relative bias. These statistical methods were used to evaluate the performance of each laboratory, in addition to the overall evaluation for each radionuclide. This evaluation has indicated that 57% and 86% of the results passed the criteria set for precision and accuracy applied for this test in relation to ²²⁶Ra and ²²⁸Ra, respectively. These two radionuclides are considered to be the most important radionuclides in the oil industry.     

Direct determination of 226Ra in NORM/TENORM matrices by gamma-spectrometry

Summary The main shortcoming with the procedure to determine ²²⁶Ra in a gamma spectrum of an environmental sample by means of the ²¹⁴Bi and ²¹⁴Pb photopeaks is the likelihood of ²²²Rn leakage from the sample counting vial. An option to make such determination is to disregard the ²²⁶Ra gamma-contributions to the spectrum, other than 186.2 keV (3.5%), subtracting the ²³⁵U contribution to the ²²⁶Ra+²³⁵U peak at 186 keV. The use of this option to determine directly ²²⁶Ra activity concentrations in environmental samples and in NORM/TENORM matrices will be presented and discussed.     

Preconcentration and separation of <Superscript>99</Superscript>Tc in groundwater by using TEVA resin

An effort has been made to optimize the counting time for low-level measurement of naturally occurring radioactive material (NORM) by considering the standard deviation between the activity values of different photopeaks and counting error. It is observed that at lower counting time, relative standard deviation (RSD) varies randomly, but attains a gradual trend with increasing time and also comes closure to the counting error. Therefore minimum counting time for low-level NORM measurement of ²³⁸U and ²³²Th would be the time required to stabilize the RSD values.     

Accurate determination of naturally occurring radionuclides in Philippine coal-fired thermal power plants using inductively coupled plasma mass spectrometry and γ-spectroscopy

There is an increased interest in measuring naturally occurring radioactive materials (NORM) like coal, fly ash considering health hazards caused by naturally occurring radionuclides. This paper presents activity concentration (AC) of ²²⁶Ra, ²²⁸Ra, ²³²Th, ²³⁸U and ⁴⁰K in feed coal, bottom and fly ash samples from Philippines coal-fired thermal power plants using inductively coupled plasma mass spectrometry (ICP-MS) and high-purity germanium gamma spectroscopy (HPGe γ-spectroscopy). Coal, bottom and fly ash samples were digested using a microwave oven with a mixture of HNO₃, HClO₄ and HF. Uranium (²³⁸U) and thorium (²³²Th) ACs were also analyzed from samples using ICP-MS. A good correlation was found for the measurement of U and Th using both techniques (R² = 0.97 and 0.94 respectively). ICP-MS measurements showed the highest AC of ²³²Th and ²³⁸U in fly ash and lowest for feed coal samples. With HPGe γ-spectroscopy measurements, highest AC (in Bq kg^{− 1}) of ²²⁶Ra, ²²⁸Ra, ²²⁸Th and ⁴⁰K, were noticed in fly ash followed by bottom ash and feed coal. ICP-MS method is rapid for the measurement of uranium and thorium in comparison to γ-spectroscopy as secular equilibrium is not required. Activity concentrations of bottom and fly ash samples were found to be within the reported values worldwide and below the International Atomic Energy Agency recommended values for regulatory control.     

Measurement of naturally occurring radioactive materials (NORM) in beach sand minerals using HPGe based gamma-ray spectrometry

This paper discusses the measurement of naturally occurring radioactivity materials (NORM) in beach sand minerals using high resolution gamma spectrometry. In India, the beach sand minerals of economic interest from coastal Kerala, Tamil Nadu and Orissa are enriched with NORM due to the occurrence of monazite deposits and heavy minerals such as zircon, ilmenite, magnetite, garnet, rutile etc. Since many of these ores are rich in ²³²Th and other radio elements, certification of radioactivity levels has become mandatory in recent years. The average activity concentrations of ²²⁶Ra in zircon, rutile and garnet were 3,531, 1,134 and 17 Bq kg^?1, respectively. The average activity concentration of ²³²Th observed in zircon, rutile and garnet were 618, 454 and 64 Bq kg^?1, respectively. Concentration of ²²⁶Ra, ²³²Th, and ⁴⁰K in ilmenite ore ranged from 17.6–444 Bq kg^?1, 80.4–1971 Bq kg^?1 and ≤5.5–25.0 Bq kg^?1, respectively.     

Determination of 226Ra in solid samples of few milligrams after mineralisation and measurement by solid scintillation

A protocol is proposed for the measurement of ²²⁶Ra on 150 mg of solid sample without radiochemistry. To evaluate the performance of this method, standard samples were used and the results were in good agreement with reference values. The detection limit obtained is about 130 Bq kg⁻¹ (dry weight) without mineralised solution concentration by evaporation. A concentration of the solution by 4 and/or an increase of sample mass by 4 in the case of microwave digestion system, allows achieving a detection limit of 30 Bq kg⁻¹ (dry weight) and thus measuring ²²⁶Ra in most soils. This method could also be used for NORM sites on soil and sediment samples.

     

NORM activity concentration in sediment cores from the Peninsular Malaysia East Coast Exclusive Economic Zone

Study for distribution of Naturally Occurring Radioactive Materials (NORM) i.e. ²²⁶Ra, ²²⁸Ra and ⁴⁰K in the east coast of Peninsular Malaysia Exclusive Economic Zone (EEZ) was carried out as part of the national marine environment project. Sixteen marine sediment cores from selected locations within the EEZ were collected for determination of NORM activity concentrations using high-purity germanium (HPGe) gamma spectrometer. From the measurement, the activity concentration of ²²⁶Ra, ²²⁸Ra and ⁴⁰K is ranged from 16 ± 4 Bq/kg to 46 ± 6 Bq/kg (total mean 30), 28 ± 7 Bq/kg to 87 ± 11 Bq/kg (total mean 56) and 171 ± 33 Bq/kg to 690 ± 89 Bq/kg (total mean 420), dry wt., respectively. The activity concentrations of radionuclides in most of the core were quite uniform suggesting that there were thorough vertical mixed of sediment throughout the core. The results obtained were also in good agreement with those previous reported from other countries in the region and therefore can be used to enhance present radioactivity database. The calculated external hazard values were ranged from 0.25 to 0.51 with the mean of 0.38 (less than unity) showed little risk of external hazard to the workers handling the sediments and it was likely low level of the mainland natural gamma-radiation in the east coast of Peninsular Malaysia.     

Activity concentration of226Ra and238U in various soils

The distribution of²²⁶Ra and²³⁸U in various soils has been studied. Supposing that radioactive equilibrium were in existence, the average activities of²²⁶Ra and²³⁸U would show a nearly 11 correlation. As weathering affects radioactive equilibrium in surface soil, radioactive equilibrium was not in existence. Therefore, four kinds of soil were selected from different weathering conditions, viz. river bed soil, paddy field soil, field soil and uncropped soil. The²²⁶Ra/²³⁸U ratio of various soils lies in the range of 1.63 to 2.41. The activity concentrations of²²⁶Ra were greater than²³⁸U in various soils. The ratio²²⁶Ra/²³⁸U can be shown to be a quantitative index of weathering. Phosphatic manure contains²³⁸U and its daughter isotopes in concentrations far exceeding the average abundance in the earth's crust. But the cultivated soils (paddy field soil, field soil) are not affected by fertilizers in Kamisaibara.     

Treatment of an aqueous radioactive waste solution with elevated levels of226Ra and228Ra

Treatment of an aqueous radioactive waste solution to remove radium prior to discharge was conducted at a laboratory scale. The actual solution is mainly composed of combined radium (²²⁶Ra and²²⁸Ra) with high concentrations of manganese, iron and calcium, which are present as chlorides in dilute hydrochloric acid. Direct precipitation by sulfate anions was selected to be the more viable treatment technique. Sulfate anion concentration, free acidity, temperature and aging of the sulfate precipitate in the supernate prior to filtration are factors that were investigated for their effect on the separation efficiency. The data obtained are discussed in detail.     

Analytical methods for the characterization and the leachability evaluation of a solid waste generated in a phosphoric acid production plant

Naturally Occurring Radioactive Materials (NORM) are present in the environment and can be concentrated by technical activities, particularly those involving natural resources. These NORM deposits are highly stable and very insoluble under environmental conditions at the earth's surface. However reducing or oxidant conditions or pH changes may enable a fraction of naturally occurring radionuclides to eventually be released to the environment. In this paper the analytical methods to determine the chemical and radiochemical composition of a solid waste generated in an acid phosphoric production plant was shown. The sample, analysed by gamma spectrometry and radiochemical methods, contained ²¹⁰Pb and ²¹⁰Po and a high activity concentration of uranium isotopes but it shows a very low quantity of ²²⁶Ra. Also a sequential extraction method consisting of five operationally-defined fractions was used to evaluate the leachability of uranium isotopes, ²¹⁰Pb and ²¹⁰Po. The average leaching potential observed in the sample is 97.6% for ²³⁸U, 93.2% for ²¹⁰Pb and 82.4% for ²¹⁰Po. Moreover the results show that ²¹⁰Pb and ²¹⁰Po are leachable under only extreme conditions, whereas uranium is very more soluble.     

Radium accumulation in animal thyroid glands a possible method for uranium and thorium prospecting

A method of prospecting for uranium and thorium is proposed based on uptake of their radioactive daughters²²⁶Ra and²²⁸Ra by plants, the collection of plant material by herbivores, the concentration of the radioactive species by specific animal tissues, and the subsequent gamma-ray analysis of the tissues. This paper is based on work performed under United States Energy Research and Development Administration (formerly U.S.A.E.C.), Contract EY-76-C-06-1830.     

Correlation of natural and artificial radionuclides in soils with pedological,climatological and geographic parameters

Various types of soil samples were collected in the southern part of Brazil, with depth intervals of 5 cm, down to 50 cm, using a specially designed sampler. Pedological analysis of these soils were performed. Nuclear activities of¹³⁷Cs (expressed in Bq m^–2) and radioactive natural element (²²⁶Ra,²²⁸Ra and⁴⁰K) concentrations were determined by low background gamma-ray spectrometry.¹³⁷Cs concentrations were correlated with radioactive natural element concentrations and pedological, climatological and geographic parameters related to the soil samples collected.     

Radium,uranium and thorium concentrations in low specific activity scales and in waters of some oil and gas production plants

Low specific activity scales consisting of alkaline earth metal carbonates and sulfates are often present in some gaseous and liquid hydrocarbon plants; these scales contain a certain concentration of radium, uranium and thorium, which can cause a risk of -irradiation and of internal radiocontamination when they must be mechanically removed. That being stated,²³⁸U,²³²Th and²²⁶Ra were determined in scales, sludges and waters coming from different plants.²³⁸U and²³²Th concentrations were found very low; the isotopes²³⁸U and²³⁴U resulted in radioactive equilibrium, whilst²³²Th and²²⁸Th were not always in equilibrium.²²⁶Ra concentration was higher in scales and sludges than in waters.     

Radium isotopes in suspended matter in an estuarine system in the southwest of Spain

The presence of²²⁶Ra and²²⁴Ra in suspended matter from an estuarine system which surrounds a phosphate fertilizer complex has been investigated. The results have confirmed an important radioactive impact from the industrial complex, since up to 2.5 Bq²²⁶Ra/g suspended matter (dry) has been measured. The influence of tides and seasonal conditions, through changes in salinity, has been found to be relevant. The distribution coefficients for²²⁶Ra between the suspended matter and the river water have been calculated. The values are in agreement by order of magnitude with those found in the literature, but they clearly depend on tidal state and seasonal conditions.     

226Ra and possible water contamination due to phosphate fertilizer production

The raw material used in the production of fetilizers is phosphate ore containing various amounts of naturally radioactive elements. During phosphate ore processing, owing to chemical properties of radium, practically all²²⁶Ra gets incorporated into phosphogypsum and becomes the main source of radioactivity. This study was carried out in a fertilizer factory in central Croatia, which may represent a site of significant environmental contamination due to fertilizer production and phosphogypsum deposition in the area. The purpose of this paper was to determine whether ingestion of drinking water in this area poses a health risk for the inhabitants. The results of our study confirmed the occurrence of²²⁶Ra in elevated concentrations in the samples of trickling waters. However, concurrent analyses of drinking water indicated that the risk of adverse health effects for the population living in the vicinity of a phosphate fertilizer plant is negligible.     

Assessment of 226Ra and 228Ra activity concentration in west coast of India

An investigation on the distribution of ²²⁶Ra and ²²⁸Ra activity concentration in coastal surface sea water from Okha in Gujarat to Ratnagiri in Maharashtra state along the west coast of India was carried out. In-situ pre-concentration technique was used to measure radium isotopes by passing 1,000 L of seawater through MnO₂ impregnated polypropylene filter cartridges at all the locations. ²²⁶Ra was estimated using gamma ray peak of its daughter radionuclides ²¹⁴Bi and ²¹⁴Pb. ²²⁸Ra was estimated from its daughter ²²⁸Ac. In the coastal waters, ²²⁶Ra and ²²⁸Ra activity concentration were observed to be in the range of 1.5–2.9 and 2.5–8.6 Bq m^?3 with a mean of 2.2 and 4.9 Bq m^?3 respectively. The activity of ²²⁸Ra was observed to be more than ²²⁶Ra in all the locations. The variation in spatial distribution of the radium isotopes activity concentration and its ratio with respect to location is discussed in the paper. The radioactive database obtained represents reference values for coastal environment of India.     

The radioactivity of building materials

Summary Radiation exposure of the population can be increased appreciably by the use of building materials containing above-normal levels of naturally occurring radionuclides of terrestrial origin, as high as 1600 Bq^. kg^-1for ⁴⁰K in granites, 700 Bq^. kg^-1for ²²⁶Ra in phosphogypsum and 360 Bq^. kg^-1for ²³²Th in granites. In a 25-year survey including more than two hundreds of different materials were investigated. Of the materials normally used in the building industry, i.e., red clay bricks, cement of Portland Types I and II, concretes, gravels and sand, contain regular levels of the primordial radionuclides. The adsorbed dose rate in indoor air, in general, does not exceed the dose criterion of 80 nGy^. h^-1or 0.3 mSv^. y^-1for the effective dose. Granites and phosphogypsum are the highly radioactive materials for which the absorbed dose rate in indoor air becomes up to five times higher than the dose criterion. It is recommended to avoid the use of those materials without radioactivity control.     

Spatial distribution of radium in coastal marine waters of Tamil Nadu

An investigation on the distribution of radium activity levels in the entire south eastern coast of Tamil Nadu, India, from Chennai to Kanyakumari was carried out. Insitu preconcentration technique was adopted by passing 1,000?L of seawater through MnO₂ impregnated cartridge filters at all the locations. In the coastal waters, ²²⁶Ra and ²²⁸Ra concentration was observed to be in the range of 1 to 1.81 and 3.1 to 7.5?mBq/L, respectively with an average of 1.52 and 4.53?mBq/L. respectively, while the sediment samples showed ²²⁶Ra activity levels from 8.1 to 129.0?Bq/kg and ²²⁸Ra varied from 14.7 to 430.01?Bq/kg. The Kd values for ²²⁶Ra was observed to be from 5.3E03 to 3.5E05?L/kg and for ²²⁸Ra it was in the range of 2.3E03 to 5.9E04. It was observed that the concentration of ²²⁸Ra was more than ²²⁶Ra in all the locations. The spatial distribution of the activity with respect to location is discussed in the paper. The radioactive database obtained, represents reference values for coastal environment of Tamil Nadu.     

Estimation of growth rate of hokutolite from Tamagawa hot-spring,Akita, Japan

The concentrations of radium isotopes and the progenies (²²⁶Ra; ²²⁸Ra and ²²⁸Th) in three hokutolite samples from Tamagawa hot-spring were measured. These isotopes were analyzed by a well-type HPGe γ-ray spectrometer for the 351, 911 and 583 keV γ-ray from ²¹⁴Pb, ²²⁸Ac and ²⁰⁸Tl, respectively, each being in radioactive equilibrium with precursors. Concentration of ²²⁶Ra and ²²⁸Ra were observed to be in the range of 52–85 and 7.1–85 Bq/g, respectively. The activity ratios of ²²⁸Ra/²²⁶Ra and ²²⁸Th/²²⁶Ra provided the estimation of the growth rate (0.09–0.15 mm/y). Estimated ²²⁸Ra/²²⁶Ra activity ratios in hot-spring water from surface of three hokutolite were concordant.