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 hardening concrete: monitoring cement hydration and prediction of radon concentration in construction site

The unique properties of radon as a noble gas are used for monitoring cement hydration and microstructural transformations in cementitious system. It is found that the radon concentration curve for hydrating cement paste enclosed in the chamber increases from zero (more accurately - background) concentrations, similar to unhydrated cement. However, radon concentrations developed within 3 days in the test chamber containing cement paste were approximately 20 times higher than those of unhydrated cement. This fact proves the importance of microstructural transformations taking place in the process of cement hydration, in comparison with cement grain, which is a time-stable material. It is concluded that monitoring cement hydration by means of radon exhalation method makes it possible to distinguish between three main stages, which are readily seen in the time dependence of radon concentration: stage I (dormant period), stage II (setting and intensive microstructural transformations) and stage III (densification of the structure and drying). The information presented improves our understanding of the main physical mechanisms resulting in the characteristic behavior of radon exhalation in the course of cement hydration. The maximum value of radon exhalation rate observed, when cement sets, can reach 0.6 mBq kg(-1) s(-1) and sometimes exceeds 1.0 mBq kg(-1) s(-1). These values exceed significantly to those known before for cementitious materials. At the same time, the minimum ventilation rate accepted in the design practice (0.5 h(-1)), guarantees that the concentrations in most of the cases will not exceed the action level and that they are not of any radiological concern for construction workers employed in concreting in closed spaces.     

Radon exhalation from uranium mill tailings: experimental validation of a 1-D model

TRACI, a model based on the physical mechanisms governing the migration of radon in unsaturated soils, has been developed to evaluate the radon flux density at the surface of uranium mill tailings. To check the validity of the TRACI model and the effectiveness of cover layers, an in situ study was launched in 1997 with the French uranium mining company, COGEMA. The study consisted of continuous measurements of moisture content, suction, radon concentration at various depths inside a UMT cover, and flux density at its surface. An initial analysis has shown that radon concentration and flux density, as calculated with a steady-state diffusion model using monthly averaged moisture contents, are in good agreement with measured monthly averaged concentrations and flux densities.     

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.     

Radon exhalation from phosphogypsum building boards: symmetry constraints, impermeable boundary conditions and numerical simulation of a test case

Comprehensive understanding of (222)Rn exhalation from phosphogypsum-bearing building material and its accumulation in indoor air is likely to rely on numerical simulation, particularly if transient effects, three-dimensional domains and convection are to be included and investigated. Yet, experimental data and analytical results are helpful (if not crucial) as far as validation is concerned. Having in mind computational code simplicity and in the light of a recent experimental and theoretical report on (222)Rn release from phosphogypsum boards for housing panels, this paper presents and discusses an alternative testing set-up and the corresponding boundary conditions, namely one side of the panel bounded by impermeable wall. Although this is a new facility to be tested, the resultant steady-state one-dimensional diffusion-dominant analytical solution is shown to match the counterpart deduced in the aforementioned previous report, despite it relaxes the constraint of symmetry about the phosphogypsum board centerline, which is inferred in that prior experimental scenario. In addition, numerical results are conducted for a diffusion-dominant two-dimensional time-varying test case concerning (222)Rn accumulation in a closed chamber having an exhaling phosphogypsum board tightly placed at one wall.     

Revegetating fly ash landfills with Prosopis juliflora L.: impact of different amendments and Rhizobium inoculation

A revegetation trial was conducted to evaluate the feasibility of growing a legume species, Prosopis juliflora L., on fly ash ameliorated with combination of various organic amendments, blue-green algal biofertilizer and Rhizobium inoculation. Significant enhancements in plant biomass, photosynthetic pigments, protein content and in vivo nitrate reductase activity were found in the plants grown on ameliorated fly ash in comparison to the plants growing in unamended fly ash or garden soil. Higher growth was obtained in fly ash amended with blue-green algae (BGA) than farmyard manure or press mud (PM), a waste from sugar-processing industry, due to the greater contribution of plant nutrients, supply of fixed nitrogen and increased availability of phosphorus. Nodulation was suppressed in different amendments of fly ash with soil in a concentration-duration-dependent manner, but not with other amendments. Plants accumulated higher amounts of Fe, Mn, Cu, Zn and Cr in various fly ash amendments than in garden soil. Further, inoculation of the plant with a fly ash tolerant Rhizobium strain conferred tolerance for the plant to grow under fly ash stress conditions with more translocation of metals to the above ground parts. The results showed the potential of P. juliflora to grow in plantations on fly ash landfills and to reduce the metal contents of fly ash by bioaccumulation in its tissues.     

Assessment of the natural radioactivity and radiological hazards in Turkish cement and its raw materials

The natural radioactivity due to presence of (226)Ra, (232)Th and (40)K radionuclides in raw materials, intermediate products (clinker) and end products (22 different cement types) was measured using a gamma-ray spectrometry with HPGe detector. The specific radioactivity of (226)Ra, (232)Th and (40)K in the analyzed cement samples ranged from 12.5+/-0.3 to 162.5+/-1.7Bqkg(-1) with a mean of 40.5+/-26.7Bqkg(-1), 6.7+/-0.3 to 124.9+/-2.5Bqkg(-1) with a mean of 26.1+/-18.9Bqkg(-1) and 64.4+/-2.3 to 679.3+/-18.2Bqkg(-1) with a mean of 267.1+/-102.4Bqkg(-1), respectively. The radium equivalent activity (Ra(eq)), the gamma-index, the emanation coefficient, the (222)Rn mass exhalation rate and the indoor absorbed dose rate were estimated for the radiation hazard of the natural radioactivity in all samples. The calculated Ra(eq) values of cement samples (37.2+/-8.7-331.1+/-15.5Bqkg(-1) with a mean of 98.3+/-53.8) are lower than the limit of 370Bqkg(-1) set for building materials. The Ra(eq) values were compared with the corresponding values for cement of different countries. The mean indoor absorbed dose rate is slightly higher than the population-weighted average of 84nGyh(-1).     

Radon and thoron monitoring in the environment of Kumaun Himalayas: survey and outcomes

Monitoring of radon, thoron and their daughter products was carried out in houses of Kumaun Himalaya, India using LR-115 plastic track detectors. The measurements were made in residential houses from June 1999 to May 2000 at a height of 2.5 m from ground level using a twin chamber radon dosimeter. The twin chamber radon dosimeter can record the values of radon, thoron and their decay products separately. Maximum and minimum indoor radon and thoron concentrations were evaluated and activity concentrations of radon and thoron daughters were estimated. The resulting dose rates due to radon, thoron and their decay products varied from 0.04 to 1.89 microSv/h. A detailed analysis of the distribution of radon, thoron and their decay products inside the house is also reported. The observed dose rates inside the houses of Kumaun Himalaya were found to be lower than the ICRP recommended value of 200 Bq/m3 and thus are within safe limits.     

Recovery and recycling of post-consumer waste materials. Part 1. Generalities and target wastes (paper,cardboard and aluminium cans)

Recycling of post-consumer waste materials is gaining increased interest due to public awareness, legislative promotion and imposition, economic benefits and appropriate technologies being available. The present paper does not deal with municipal solid waste as such, but only with the recyclable constituents. The paper does not aim at presenting recycling process details and/or fundamental research results, but reviews the major recyclables with their reuse potential, recycling technologies used, problems, solutions and potential areas of future research and development. These target recyclables include paper and cardboard, aluminium cans, glass beverage bottles, scrap metal and steel cans, scrap tyres, batteries and household hazardous waste. The present paper sets the overall picture and deals with paper, cardboard and aluminium cans only. A second part of the paper assesses the other target recyclables. The assessment of the waste availability, the existing and currently developed recovery and recycling technologies, and the economically rewarding markets while recycling, stress the technical, economic and environmental importance of this waste management sector. The activities associated with the recovery and recycling of post-consumer wastes require a strong sustainable engineering input at all phases of the treatment, from input quality control, to the selection of the most appropriate technology and the delivery of the recyclables as readily reusable feedstock.     

Inferring coastal processes from regional-scale mapping of Radon and salinity: examples from the Great Barrier Reef, Australia

The radon isotope ²²²Rn and salinity in coastal surface water were mapped on regional scales, to improve the understanding of coastal processes and their spatial variability. Radon was measured with a surface-towed, continuously recording multi-detector setup on a moving vessel. Numerous processes and locations of land-ocean interaction along the Central Great Barrier Reef coastline were identified and interpreted based on the data collected. These included riverine fluxes, terrestrially-derived fresh submarine groundwater discharge (SGD) and the tidal pumping of seawater through mangrove forests. Based on variations in the relationship of the tracers radon and salinity, some aspects of regional freshwater inputs to the coastal zone and to estuaries could be assessed. Concurrent mapping of radon and salinity allowed an efficient qualitative assessment of land-ocean interaction on various spatial and temporal scales, indicating that such surveys on coastal scales can be a useful tool to obtain an overview of SGD locations and processes.     

Design, operation, and performance testing of the Cameo no. 1 unit fabric filter

A carborundum fabric filter was retrofitted to the Cameo No. 1 unit in 1978. Cameo Station, owned and operated by Public Service Company of Colorado, is near Grand Junction, Colorado, and No. 1 unit (22 MW) was first placed in service in 1958. The purchase contract for the fabric filter was written on July 2, 1976, but due to problems in obtaining an emission permit from the state of Colorado, actual construction did not begin until February, 1978. The fabric filter, designed with 1.92 gross air-to-cloth ratio and reverse air, was placed in service December 18, 1978. This paper covers the design aspects, construction features, startup procedures, and acceptance testing.     

The radium legacy: Contaminated land and the committed effective dose from the ingestion of radium contaminated materials

The manufacture and use of radium in the early to mid-20th century within industrial, medicinal and recreational products have resulted in a large number of contaminated sites across a number of countries with notable examples in the USA and Europe. These sites, represent a significant number of unregulated sources of potential radiological exposure that have collectively and hitherto not been well characterised. In 2007, the Radioactive Contaminated Land (RCL) Regulations came into force in the UK, providing the statutory guidance for regulators to classify and deal with RCL. Here we report on results derived from digestion experiments to estimate committed effective dose, a key aspect of the RCL Regulations, from the ingestion of radium contaminated sources that can be found in the environment. This case study includes particles, clinker and artefacts that arise from past military activities on a site that was once an airfield at Dalgety Bay on the Firth of Forth, UK. Since 2011 the number of radium contaminated finds has increased by one order of magnitude on the foreshore areas of Dalgety Bay. The increase in finds may in large part be attributed to a change in monitoring practice. A subsample of sixty sources was selected, on the basis of their activity and dimensions, and subjected to digestion in simulated stomach and lower intestine solutions. The study demonstrated that more radium-226 (²²⁶Ra) and lead-210 (²¹⁰Pb; driven by Polonium solubility) are dissolved from sources in artificial ‘stomach’ solutions compared with ‘lower intestine’ solutions. The combined ‘gut’ solubility for ²²⁶Ra and apparent ²¹⁰Pb varied from less than 1% to up to 35% ICRP 72 conversion factors were used to convert the activities measured in solution to committed effective dose. A little over 10% of the sources tested dissolved sufficient radioactivity to result in 100 mSv committed effective dose to an infant. Using the solubility of 35% as a worst case, minimum source activities necessary to deliver 100 mSv to the full age range of users of the foreshore were estimated. All the estimated activities have been detected and recovered through routine monitoring.     

Occurrence and behaviour of radionuclides in the Moselle River—Part I: Entry of natural and artificial radionuclides

Various sources contribute to the radioactive contamination of the Moselle River, among which the French NPP Cattenom with four units of 1300 M We represents the most important. Appropriate operational precautions were taken in order to monitor the nuclide transfer on different pathways under normal and accidental conditions and the effectiveness of these measures has been tested using natural (²¹⁴Pb/²¹⁴Bi, ⁷Be, ⁴⁰K) and artificial radionuclides. (³H, ⁵⁸Co, ⁶⁰Co, ¹³¹I, ¹³⁷Cs) as tracers. Measurements of suspended matter have revealed that the inputs of natural nuclides exceed the discharges of the NPP Cattenom. In 1992 the annual loads of ⁷Be and ⁴⁰K in suspended matter at Palzem amounted to 21 and 130 GBq year⁻¹, whereas the emission rates of ⁶⁰Co and ¹³⁷Cs were about 2.6 and 1.0 GBq year⁻¹. The total nuclide load of ¹³⁷Cs at Palzem reached 6.2 GBq year⁻¹, which is about six times the quantity emitted by the NPP Cattenom in the same year. This excess is due to the accident at Chernobyl and to a lesser extent to prior atmospheric weapons tests.     

Association between background exposure to organochlorine pesticides and the risk of cognitive impairment: A prospective study that accounts for weight change

BackgroundBackground exposure to organochlorine (OC) pesticides was recently linked to cognitive impairment and dementia in cross-sectional and case–control studies. This prospective study was performed to evaluate if OC pesticides at baseline are associated with the future risk of cognitive impairment in elderly, with particular focus on weight change.MethodsPlasma concentrations of 3 OC pesticides (p,p′-DDE, trans-nonachlor, and hexachlorobenzene) were measured among 989 men and women aged 70 years in the Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS). Cognitive impairment was validated by reviewing medical records. During the ten year follow-up, cognitive impairment was developed in 75 subjects. When weight change from age 70 to 75 was considered in analyses, elderly with incident cases before age 75 were excluded to keep the prospective perspective, leaving 795 study subjects and 44 incident cases.ResultsThe summary measure of 3 OC pesticides predicted the development of cognitive impairment after adjusting for covariates, including weight change. Compared to subjects with OC pesticides < 25th percentile, adjusted hazard ratios (HRs) in those with 25th–<75th and ≥ 75th percentiles were 3.5 (95% confidence interval: 1.5–8.5) and 3.2 (1.1–7.6), respectively (P_trend = 0.04). Among 506 subjects who maintained or gained body weight, adjusted HRs were 6.9 and 11.6 (1.4–92.6) among the elderly in the 25th–<75th and ≥ 75th percentiles compared to < 25th percentile (P_trend < 0.01).ConclusionsThis prospective study demonstrates that background exposure to OC pesticides are linked to the risk of developing cognitive impairment in elderly. The role of the chronic exposure to low dose OC pesticides in the development of dementia should be further evaluated in other populations.     

Sea to land transfer of anthropogenic radionuclides to the North Wales coast, Part II: aerial modelling and radiological assessment

Modelling calculations have been performed to predict the radiological impact of the sea to land transfer pathway to members of the public in North Wales from 1952 to 2004. The radionuclides of interest were (99)Tc, (137)Cs, (239,240)Pu and (241)Am and the exposure routes considered were food consumption, external and inhalation. The consumption of locally grown terrestrial food in the early to mid 1980s was the most significant source of exposure to all of the groups considered, with (239,240)Pu being the radionuclide contributing most to the dose. A maximum dose of 1.46muSvy(-1) was calculated for adult members of the critical consumption group in 1985, with doses for 2004 reducing to 0.59muSvy(-1). Despite the conservative approach of the dose calculations, the dose rate values are very low, less than 0.15% of the annual limit of 1000muSvy(-1) for the UK public from controlled radiation sources (excluding medical).     

Toxicokinetics of dioxins and other organochlorine compounds in Japanese people: Association with hepatic CYP1A2 expression levels

Concentrations of persistent organochlorine compounds (OCs) including polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and polychlorinated biphenyls (PCBs) in the liver and adipose tissue of Japanese cadavers were measured, and their toxicokinetics were examined in association with hepatic cytochrome P450 (CYP) 1A protein expression levels. Total 2,3,7,8-tetrachlorodibenzo-p-dioxin toxic equivalents (TEQs) were 66 ± 74 and 65 ± 57 pg/g lipid weight (mean ± S.D.) in the liver and adipose tissue, respectively. Total PCBs (sum of 62 congeners targeted), p,p′-dichlorodiphenyl-dichloroethylene (p,p′-DDE) and β-hexachlorocyclohexane (β-HCH) were detected at concentrations over 1 μg/g lipid in both tissues of some specimens. For most of the dioxin-like congeners, total PCBs, p,p′-DDE, oxychlordane, α- and β-HCH, hexachlorobenzene (HCB), and tris(4-chlorophenyl)methane (TCPMe), age-dependent increases in concentrations were found in the adipose tissue of males. No such age-dependent trend was observed in the liver, suggesting that there are different mechanisms underlying the hepatic concentrations of OCs. Immunoblot analyses indicated detectable expression of hepatic CYP1A2 protein, whereas no CYP1A1 protein was detected. The CYP1A2 expression levels were positively correlated with concentrations (on wet weight basis) of 2,3,4,7,8-P₅CDF, the dominant TEQ-contributed congeners in the liver, indicating the induction of this CYP. Hepatic CYP1A2 protein levels were strongly correlated with the liver to adipose concentration (L/A) ratios of PCDD/F congeners with more than 5 chlorine atoms. Together with higher concentrations of the congeners in the liver than in the adipose tissue, the observation on L/A ratios of highly chlorinated PCDD/Fs suggests that induced hepatic CYP1A2 protein is involved in their sequestration in this human population, as observed in model animals (rodents). Nonetheless, the magnitude of hepatic sequestration (L/A ratio) of PCDD/Fs in this human population was lower than in other mammals and birds, reported previously. This study emphasizes the fact that toxicokinetics of some OCs can be affected at least partly by CYP1A2 protein levels in humans. For the extrapolation of their toxicokinetics from model animals to humans, knowledge on the induction and sequestration potencies of CYP1A is necessary.     

Sea to land transfer of anthropogenic radionuclides to the North Wales coast, Part I: external gamma radiation and radionuclide concentrations in intertidal sediments, soil and air

Previous projects specifically aimed at performing radiological assessments in the vicinity of North Wales, investigating the presence and transfer of radionuclides from sea to land, were in 1986 and 1989. Since then, changes have occurred in the radioactive discharges from the British Nuclear Group Sellafield site. Annual discharges of (137)Cs, (238)Pu, (239,340)Pu and (241)Am have decreased markedly whereas, up until recent years, discharges of (99)Tc have increased. It is therefore desirable to quantify current transfer processes of radionuclides in the North Wales region and thus provide an update on 15-year-old studies. A field campaign was conducted collecting soil samples from 10 inland transects and air particulates on air filters from three High Volume Air Samplers, along the northern coast of Wales at Amlwch, Bangor Pier and Flint. Complementary field data relating to external gamma dose rates were collected at the soil sites. The field data generated for (137)Cs, (238)Pu, (239,340)Pu and (241)Am were consistent with what had been reported 15 years previously. Therefore, there has been no increase in the supply of these Sellafield-derived radionuclides to the terrestrial environment of the North Wales coast. The (99)Tc data in sediments were consistent with reported values within annual monitoring programmes, however, a relatively high activity concentration was measured in one sediment sample. This site was further investigated to determine the reason why such a high value was found. At present there is no clear evidence as to why this elevated concentration should be present, but the role of seaweed and its capacity in accumulating (99)Tc and transferring it to sediment is of interest. The analysis of the field samples for (99)Tc, (137)Cs, (238)Pu, (239,240)Pu and (241)Am has provided a data set that can be used for the modelling of the transfer of anthropogenic radionuclides from sea to land and its subsequent radiological implications and is reported in an accompanying paper.