Radon exhalation of cementitious materials made with coal fly ash: Part 2--testing hardened cement-fly ash pastes

Increased interest in measuring radionuclides and radon concentrations in fly ash (FA), cement and other components of building products is due to the concern about health hazards of naturally occurring radioactive materials (NORM). The paper focuses on studying the influence of FA on radon exhalation rate (radon flux) from cementitious materials. In the previous part of the paper the state of the art was presented, and the experiments for testing raw materials, Portland cement and coal fly ash, were described. Since the cement and FA have the most critical role in the radon release process relative to other concrete constituents (sand and gravel), and their contribution is dominant in the overall radium content of concrete, tests were carried out on cement paste specimens with different FA contents, 0-60% by weight of the binder (cement+FA). It is found that the dosage of FA in cement paste has a limited influence on radon exhalation rate, if the hardened material is relatively dense. The radon flux of cement-FA pastes is lower than that of pure cement paste: it is about approximately 3 mBq m(-2) s(-1) for cement-FA pastes with FA content as high as 960 kg m(-3).     

Radon exhalation of cementitious materials made with coal fly ash: Part 1--scientific background and testing of the cement and fly ash emanation

Increased interest in measuring radionuclides and radon concentrations in fly ash, cement and other components of building products is due to the concern of health hazards of naturally occurring radioactive materials (NORM). The current work focuses on studying the influence of fly ash (FA) on radon-exhalation rate (radon flux) from cementitious materials. The tests were carried out on cement paste specimens with different FA contents. The first part of the paper presents the scientific background and describes the experiments, which we designed for testing the radon emanation of the raw materials used in the preparation of the cement-FA pastes. It is found that despite the higher (226)Ra content in FA (more than 3 times, compared with Portland cement) the radon emanation is significantly lower in FA (7.65% for cement vs. 0.52% only for FA).     

Factors controlling measurements of radon mass exhalation rate

Radon mass exhalation rate of soil samples was measured using an exhalation chamber of 10 dm(3) volume and a Lucas cell. The results show that mass of sample, grain size and water content influence the radon mass exhalation rate. For soil of (226)Ra activity concentration about 2500 Bq kg(-1) and samples within the range from 0.20 kg to 0.50 kg, the radon mass exhalation rate values are higher than those for samples of other masses. The observed radon exhalation rate is an inverse function of the average grain size. At the water content about 6% by weight, the radon mass exhalation rate reaches maximum, then it decreases with both increasing and decreasing of the water content in the sample.     

Estimation of radon exhalation rate, natural radioactivity and radiation doses in fly ash samples from Durgapur thermal power plant, West Bengal, India

Coal and its by products often contain significant amounts of radionuclides, including uranium which is the ultimate source of the radioactive gas radon. Burning of coal and the subsequent emission to the atmosphere cause the re-distribution of toxic trace elements in the environment. Due to considerable economic and environmental importance and diverse uses, the collected fly ash has become a subject of worldwide interest in recent years. In the present study, radon exhalation rate and the activity concentration of (238)U, (232)Th and (40)K radionuclides in fly ash samples from Durgapur thermal power plant (WB) have been measured by "Sealed Can technique" using LR-115 type II detectors and a low level NaI (Tl) based gamma ray spectrometer, respectively. Radon exhalation rate varied from 360.0 to 470.0 mBq m(-2)h(-1) with an average value of 406.8 mBq m(-2)h(-1). Activity concentrations of (238)U ranged from 84.8 to 126.4 Bq kg(-1) with an average value of 99.3Bqkg(-1), (232)Th ranged from 98.1 to 140.5 Bq kg(-1) with an average value of 112.9 Bq kg(-1) and (40)K ranged from 267.1 to 364.9 Bq kg(-1) with an average value of 308.9 Bq kg(-1). Radium equivalent activity obtained from activity concentrations is found to vary from 256.5 to 352.8 Bq kg(-1) with an average value of 282.5 Bq kg(-1). Absorbed gamma dose rates due to the presence of (238)U, (232)Th and (40)K in fly ash samples vary in the range 115.3-158.5 nGy h(-1) with an average value of 126.4 nGy h(-1). While the external annual effective dose rate varies from 0.14 to 0.19 mSv y(-1) with an average value of 0.15 mSv y(-1), effective dose equivalent estimated from exhalation rate varies from 42.5 to 55.2 microSv y(-1) with an average value of 47.8 microSv y(-1). Values of external hazard index H(ex) for the fly ash samples studied in this work range from 0.69 to 0.96 with a mean value of 0.77.     

High natural radiation exposure in radon spa areas: a detailed field investigation in Niska Banja (Balkan region)

The measurement campaigns have been done in the rural community of Niska Banja, a spa town located in southern Serbia, to evaluate population exposure to natural radioactivity. After a screening survey in 200 houses, annual radon and thoron concentrations were measured in 34 houses, and in 2004 a detailed investigation was carried out at six houses with elevated indoor radon concentrations. The paper presents the results of these detailed measurements. The complementary techniques were applied to determine radon and thoron concentrations in indoor air, in soil gas, radon exhalation from soil, soil permeability, and indoor and outdoor gamma doses. Soil and water samples were collected and analysed in the laboratory. Indoor radon and thoron concentrations were found to be more than 1kBqm(-3) and 200Bqm(-3), respectively. Extremely high concentrations of soil-gas radon (>2000kBqm(-3)) and radon exhalation rates (1.5mBqm(-2)s(-1)) were observed. These results will be utilised to set up the methodology for a more systematic investigation.     

Radon exhalation from granites used in Saudi Arabia

Measurements of radon exhalation for a total of 50 selected samples of construction materials used in Saudi Arabia were taken using a radon gas analyzer. These materials included sand, aggregate, cement, gypsum, hydrated lime, ceramics and granite. It was found that the granite samples were the main source of radon emanations. A total of 32 local and imported granite samples were tested. It was found that the radon exhalation rates per unit area from these granite samples varied from not detectable to 10.6 Bq m-2 h-1 with an average of 1.3 Bq m-2 h-1. The linear correlation coefficient between emanated radon and radium content was 0.92. The normalized radon exhalation rates from 2.0 cm thick granite samples varied from not detectable to 0.068 (Bq m-2 h-1)/(Bq kg-1) with an average of 0.030 (Bq m-2 h-1)/(Bq kg-1). The average radon emanation of the granite samples was found to be 21% of the total radium concentration. Therefore, granite can be a source of indoor radon as well as external gamma-radiation from the uranium decay series.     

Concentration of 226Ra in Hungarian bottled mineral water

Concentration of the radionuclide 226Ra was determined in almost every type of bottled mineral water commercially available in Hungary. Determination of the radon coming from the radium dissolved in the water was used for activity measurement. As the results show, the 226Ra concentrations exceed the level of 100 mBq l(-1) in six cases out of the 28 types of mineral water investigated. In one case 3 Bq l(-1) was measured, which provides 0.3 mSv year(-1) committed effective dose for adults in the case of a consumption rate of 1 l day(-1). In soft drinks produced from mineral water a concentration of 2.6 Bq l(-1) was determined, which means 1.4 mSv year(-1) effective dose in the age group 12-17 years in the case of permanent daily drinking of 1 l of these beverages.     

Radon (222Rn) level variations on a regional scale: influence of the basement trace element (U, Th) geochemistry on radon exhalation rates

The approach proposed in this study provides insight into the influence of the basement geochemistry on the spatial distribution of radon (222Rn) levels both at the soil/atmosphere interface and in the atmosphere. We combine different types of in situ radon measurements and a geochemical classification of the lithologies, based on 1/50,000 geological maps, and on their trace element (U, Th) contents. The advantages of this approach are validated by a survey of a stable basement area of Hercynian age, located in South Brittany (western France) and characterized by metamorphic rocks and granitoids displaying a wide range of uranium contents. The radon source-term of the lithologies, their uranium content, is most likely to be the primary parameter which controls the radon concentrations in the outdoor environment. Indeed, the highest radon levels (> or = 100 Bq m-3 in the atmosphere, > or = 100 mBq m-2 s-1 at the surface of the soil) are mostly observed on lithologies whose mean uranium content can exceed 8 ppm and which correspond to peraluminous leucogranites or metagranitoids derived from uraniferous granitoids.     

Radon level in dwellings and its correlation with uranium and radium content in some areas of Himachal Pradesh,India

LR- 115 plastic track detectors have been used to measure indoor radon level in some dwellings of Una district, Himachal Pradesh, India. The annual average radon concentration in dwellings in most of the villages falls in the range of the action level recommended by the International Commission on Radiological Protection. The radon values in some of the dwellings exceed the action level and may be unsafe from the health hazard point of view. The indoor radon values are in general higher in winter than in summer. Uranium, radium and radon exhalation studies have also been carried out in soil samples collected from these areas. A good correlation is obtained between uranium concentration in the soil and indoor radon in dwellings. The soil radon exhalation rate also correlates with the uranium concentration in soil.     

Spatial and time variations of radon-222 concentration in the atmosphere of a dead-end horizontal tunnel

The concentration of radon-222 has been monitored since 1995 in the atmosphere of a 2 m transverse dimension, 128 m long, dead-end horizontal tunnel located in the French Alps, at an altitude of 1600 m. Most of the time, the radon concentration is stable, with an average value ranging from 200 Bq m(-3) near the entrance to about 1000 Bq m(-3) in the most confined section, with an equilibrium factor between radon and its short-lived decay products varying from 0.61 to 0.78. However, radon bursts are repeatedly observed, with amplitudes reaching up to 36 x 10(3) Bq m(-3) and durations varying from one to several weeks, with similar spatial variations along the tunnel as the background concentration. These spatial variations are qualitatively interpreted in terms of natural ventilation. Comparing the radon background concentration with the measured radon exhalation flux at the wall yields an estimate of 8+/-2 x 10(-6) s(-1) (0.03+/-0.007 h(-1)) for the ventilation rate. The hypothesis that the bursts could be due to transient changes in ventilation can be ruled out. Thus, the bursts are the results of transient increased radon exhalation at the walls, that could be due to meteorological effects or possibly combined hydrological and mechanical forcing associated with the water level variations of the nearby Roselend reservoir lake. Such studies are of interest for radiation protection in poorly ventilated underground settings, and, ultimately, for a better understanding of radon exhalation associated with tectonic or volcanic processes.     

Study of a predictive methodology for quantification and mapping of the radon-222 exhalation rate

We propose a new methodology for predicting areas with a strong potential for radon (222Rn) exhalation at the soil surface. This methodology is based on the Rn exhalation rate quantification, starting from a precise characterisation of the main local geological and pedological parameters that control the radon source and its transport to the soil/atmosphere interface. It combines a cross mapping analysis of these parameters into a geographic information system with a model of the Rn vertical transport by diffusion in the soil. The rock and soil chemical and physical properties define the entry parameters of this code (named TRACHGEO) which calculates the radon flux density at the surface. This methodology is validated from in situ measurements of radon levels at the soil/atmosphere interface and in dwellings. We apply this approach to an area located in western France and characterised by a basement displaying a heterogeneous radon source potential, as previously demonstrated by lelsch et al. (J. Environ. Radioactivity 53(1) (2001) 75). The new results obtained show that spatial heterogeneity of pedological characteristics in addition to basement geochemistry--must be taken into account to improve the mapping resolution. The TRACHGEO forecasts explain the Rn exhalation variability on a larger scale and in general correlate well with in situ observations. Moreover, the radon-prone sectors identified by this approach generally correspond to the location of the dwellings showing the highest radon concentrations.     

Natural radioactivity measurements in building materials in Southern Lebanon

Using gamma-spectroscopy and CR-39 detector, concentration C of naturally occurring radioactive nuclides (226)Ra, (222)Rn, (214)Bi, (228)Ac, (212)Pb, (212)Bi and (40)K, has been measured in sand, cement, gravel, gypsum, and paint, which are used as building materials in Lebanon. Sand samples were collected from 10 different sandbank locations in the southern part of the country. Gravel samples of different types and forms were collected from several quarries. White and gray cement fabricated by Shaka Co. were obtained. gamma-spectroscopy measurements in sand gave Ra concentration ranging from 4.2+/-0.4 to 60.8+/-2.2 Bq kg(-1) and Ra concentration equivalents from 8.8+/-1.0 to 74.3+/-9.2 Bq kg(-1). The highest Ra concentration was in gray and white cement having the values 73.2+/-3.0 and 76.3+/-3.0 Bq kg(-1), respectively. Gravel results showed Ra concentration between 20.2+/-1.0 and 31.7+/-1.4 Bq kg(-1) with an average of 27.5+/-1.3 Bq kg(-1). Radon concentration in paint was determined by CR-39 detector. In sand, the average (222)Rn concentration ranged between 291+/-69 and 1774+/-339 Bq m(-3) among the sandbanks with a total average value of 704+/-139 Bq m(-3). For gravel, the range was found to be from 52+/-9 to 3077+/-370 Bq m(-3) with an average value of 608+/-85 Bq m(-3). Aerial and mass exhalation rates of (222)Rn were also calculated and found to be between 44+/-7 and 2226+/-267 mBq m(-2)h(-1), and between 0.40+/-0.07 and 20.0+/-0.3 mBq kg(-1)h(-1), respectively.     

Radiological characteristics and investigation of the radioactive equilibrium in the ashes produced in lignite-fired power plants

Coal- and lignite-fired power plants produce significant amounts of ashes, which are quite often being used as additives in cement and other building materials. In many cases, coal and lignite present high concentrations of naturally occurring radionuclides, such as 238U, 226Ra, 210Pb, 232Th and 40K. During the combustion process, the produced ashes are enriched in the above radionuclides. The different enrichment of the various radionuclides within a radioactive series, such as that of 238U, results in the disturbance of radioactive secular equilibrium. An extensive research project for the determination of the natural radioactivity of lignite and ashes from Greek lignite-fired power plants is in progress in the Nuclear Engineering Department of the National Technical University of Athens (NED-NTUA) since 1983. This paper presents detailed results for the natural radioactivity, the secular radioactive equilibrium disturbance and the radon exhalation rate of the fly-ash collected at the different stages along the emission control system of a lignite-fired power plant as well as of the bottom-ash. From the results obtained so far, it may be concluded that 226Ra radioactivity of fly-ash in some cases exceeds 1 kBq kg(-1), which is much higher than the mean 226Ra radioactivity of surface soils in Greece (25 Bq kg(-1)). Furthermore, the radioactivity of 210Pb in fly-ash may reach 4 kBq kg(-1). These results are interpreted in relation to the physical properties of the investigated nuclides, the temperature in the flue-gas pathway, as well as the fly-ash grain size distribution. It is concluded that towards the coldest parts of the emission control system of the power plant, the radioactivity of some natural nuclides is gradually enhanced, secular radioactive equilibrium is significantly disturbed and the radon exhalation rate tends to increase.     

222Rn and 210Pb in the Arctic summer air

As part of an extensive air chemistry programme, during summer 1980, on board the Swedish ice-breaker ‘Ymer’, levels of ²²²Rn (radon) and its long-lived daughters ²¹⁰Pb and ²¹⁰Po were measured. The radon was trapped on charcoal and the long-lived daugther products sampled on filters on a daily basis. In addition, short-lived progenies were followed continuously on the filters in order to achieve a time resolution of about one hour. The concentrations of radon and ²¹⁰Pb in the Arctic summer air north of latitude 75° N averaged 75 ± 21 (1 sd) and 0·075 ± 0·028 mBqm⁻³, r respectively. During a two week period of persistent polar winds, the mean radon concentration was 19 ±5 mBq m⁻³. During such ‘Arctic background’ conditions, radon exhalation from the sea may contribute significantly to the measured radon-in-air concentration. It is shown that steady-state equilibrium models, applied to an air mass over the sea, overstimate the aerosol residence-time calculated from activity ratios. Time-dependent calculations indicate a mean aerosol residence time of 4 to 7 d in Arctic air. Good agreement is observed between radon levels and the time since the air mass left larger areas. Both the ²²²Rn and the long-lived daughter measurements are insensitive to contamination from ship and local settlement.     

A study about remedial measures to reduce 222Rn concentration in an experimental building

Radon gas emanating from underground can spread to adjoining closed areas. It can concentrate and reach levels which represent a risk to people's health. It is well known that radon presence in most areas depends mainly on the area's geological features. Indoor radon concentrations further depend on the type of structure, construction materials and the technology used for the building. Therefore, indoor radon monitoring is of primary importance for deciding whether remedial measures are to be adopted for reducing harmful concentrations. This approach has been tried by measuring radon concentration in an experimental building situated in Milan (Italy). This building situated in a geological area that is considered at low radon risk. The results were obtained after analysing radon concentration in indoor rooms, crawl spaces, soil gas and in the atmosphere outside and by measuring before and after adoption of remedial measures. The study shows that improper building design can give rise to higher indoor radon accumulation even in an area of poor radon exhalation. Furthermore, the results enable quantification of the effectiveness of the remedial measures.     

Photon attenuation, natural radioactivity content and radon exhalation rate of building materials

High concentrations of natural radionuclides in building materials can result in high dose rates indoors, from both internal and external exposure. In dose calculations, the main radionuclides of interest are 226Ra, 232Th and 40K. Usually much attention is paid to 226Ra due to 222Rn exhalation and the subsequent internal exposure. Other radionuclides of the uranium series such as 238U and 210Pb, emitting low energy photons are not usually determined and an assumption of radioactive equilibrium is made. The above assumption is seldom checked mainly because of the difficulties in the gamma-spectroscopic analysis of low energy photons. For the determination of radionuclides emitting low-energy photons, in samples like building materials where intense self-absorption of the photons exists, a method for self-absorption correction has been developed. The method needs as input the linear attenuation coefficient mu for the material under analysis. This paper presents: 1. Correlations in the form mu = f(rho,E) developed for the estimation of the linear attenuation coefficient mu (cm(-1)), as a function of the material packing density p (g cm(-3)) and the photon energy E (keV), for building materials as well as other materials of environmental importance. 2. Gamma-spectroscopic analysis techniques used for the determination of 238U, 226Ra, 210Pb, 232Th and 40K in environmental samples, together with the results obtained from the analysis of building materials used in Greece, and industrial by-products used for the production of building materials. Among the techniques used, one is based on the direct determination of 226Ra and 235U from the analysis of the multiplet photopeak at approximarely186 keV. 3. Results from radon exhalation measurements of building materials such as cement and fly-ash and building structures conducted in the radon chambers in our Laboratory. Based on the above results, dosimetric calculations are also reported.     

Radon exhalation from building materials for decorative use

Long-term exposure to radon increases the risk of developing lung cancer. There is considerable public concern about radon exhalation from building materials and the contribution to indoor radon levels. To address this concern, radon exhalation rates were determined for 53 different samples of drywall, tile and granite available on the Canadian market for interior home decoration. The radon exhalation rates ranged from non-detectable to 312 Bq m⁻² d⁻¹. Slate tiles and granite slabs had relatively higher radon exhalation rates than other decorative materials, such as ceramic or porcelain tiles. The average radon exhalation rates were 30 Bq m⁻² d⁻¹ for slate tiles and 42 Bq m⁻² d⁻¹ for granite slabs of various types and origins. Analysis showed that even if an entire floor was covered with a material having a radon exhalation rate of 300 Bq m⁻² d⁻¹, it would contribute only 18 Bq m⁻³ to a tightly sealed house with an air exchange rate of 0.3 per hour. Generally speaking, building materials used in home decoration make no significant contribution to indoor radon for a house with adequate air exchange.     

Groundwater radon measurements in the Mt. Etna area

Radon levels were measured in 119 groundwater samples collected throughout the active volcanic area of Mt. Etna by means of a portable Lucas-type scintillation chamber. The measured activity values range from 1.8 to 52.7 Bq l(-1). About 40% of the samples exceed the maximum contaminant level of 11 Bq l(-1) proposed by the USEPA in 1991. The highest radon levels are measured in the eastern sector of the volcano, which is the seismically most active zone of the volcano. On the contrary the south-western sector, which is both seismically active and a site of intense magmatic degassing, display lower radon levels. This is probably due to the formation of a free gas phase (oversaturation of CO(2)) that strips the radon from the water. Comparison of the data gathered at Mt. Etna with those of other areas indicates that (222)Rn activity in groundwater is positively correlated with both the content of parent elements in the aquifer rocks and the temperature of the geothermal systems that interacts with the sampled aquifers.     

Specific activity and hazards of granite samples collected from the Eastern Desert of Egypt

Fifty granitic rock samples were collected from different plutons in the central part of the Eastern Desert of Egypt and were analyzed for specific concentrations of (238)U, (232)Th and (40)K radionuclei. The measurements were carried out using a high performance and stability Nomad Plus spectroscopy system attached to a 1.7 keV (FWHM) HPGe detector. The spectra were analyzed using the direct gamma counting comparison method as well as the traditional absolute efficiency curve method. The highest average value of (238)U concentration (1184 Bq kg(-1)) was observed at EI Misikat region whereas the highest average values of (40)K and (232)Th concentration (2301.8 and 162.5 Bq kg(-1) respectively), were detected at Gabal Homret Waggat area. The radium equivalent activity (Ra(eq)), the absorbed dose rate (D), the external hazard index (H(ex)) and the annual gonadal dose equivalent were also calculated and compared to the international recommended values. Radon exhalation rate from the rock samples were measured using the activated charcoal canister method. The average value of radon exhalation varies from 0.052 to 0.69 Bq m(-2) h(-1) and depends on the specific concentration of uranium.     

Detection and analysis of xenon isotopes for the comprehensive nuclear-test-ban treaty international monitoring system

The use of the xenon isotopes for detection of nuclear explosions is of great interest for monitoring compliance with the comprehensive nuclear-test-ban treaty (CTBT). Recently, the automated radioxenon sampler-analyzer (ARSA) was tested at the Institute for Atmospheric Radioactivity (IAR) in Freiburg, Germany to ascertain its use for the CTBT by comparing its results to laboratory-based analyses, determining its detection sensitivity and analyzing its results in light of historical xenon isotope levels and known reactor operations in the area. Xe-133 was detected nearly every day throughout the test at activity concentrations ranging between approximately 0.1 mBq/m3 to as high as 120 mBq/m3. Xe-133m and 135Xe were also detected occasionally during the test at concentrations of less than 1 to a few mBq/m3.