Ra–Po–Pb isotope systematics in waters of Sambhar Salt Lake,Rajasthan (India): geochemical characterization and particulate reactivity

The Sambhar Salt Lake hydrological system, including river waters, groundwaters, evaporating pans and sub-surface brines, has been analyzed for the salt content (TDS) and naturally occurring radionuclides (²¹⁰Po, ²¹⁰Pb and ^226,228Ra). The abundance of these radionuclides and their activity ratios show a wide variation in different hydrological regimes, which helps to geochemically characterize the lake system. A significantly lower Ra to total dissolved solids (TDS) ratio in the brines (by two to three orders of magnitude), when compared to the groundwaters and river waters, suggests removal of dissolved Ra by co-precipitation with Ca–Mg minerals at an early stage of the brine evolution. The concentration of Ra in evaporating lake/pan waters saturates at a value of about 35 Bq L⁻¹ over the salinity range of 100–370 g L⁻¹; attributable to its equilibration with the clay minerals. The two distinct regimes, saline lake system (lake water, evaporating pans and sub-surface brines) and groundwaters have been identified based on their differences in the distribution of ^226,228Ra isotopes. This observation points to the conclusion that the groundwaters and the lake brines are not intimately coupled in terms of their origin and evolution. The abundances of ²¹⁰Po and ²¹⁰Pb along with their activity ratios (²¹⁰Po/²¹⁰Pb) are markedly different among the surface lake waters/evaporating pans, sub-surface lake brines and groundwaters. These differences are explained in terms of different geochemical behaviour of these nuclides in presence of algae and organic matter present in these water regimes.     

Indoor air quality: Radon—Report on a WHO working group

The WHO Regional Office for Europe organized a working group in Dubrovnik, Yugoslavia, on 26–30 August 1985, which discussed radon as a pollutant affecting indoor air quality. Much of the natural background radiation to which the general public is exposed comes from the decay of ²²⁶Ra which produces radon gas and other products. Because radium is a trace element in most rock and soil, indoor concentrations of radon can come from a wide variety of substances, such as building materials and the soil under building foundations. Tap water taken from wells or underground springs may be an additional source. Radon daughter concentrations are considerably higher indoors than outdoors and are of the order of 2–5 Bq m⁻³ equilibrium equivalent radon (EER) concentration. It has been estimated that current exposure to radon gas could account for as much as 5–15% of all lung cancer deaths. It was recommended that, in general, buildings with concentrations of more than 100 Bq m⁻³ EER, as an annual average, should be considered for remedial action to lower such concentrations if simple measures are possible.     

Natural radioactive nuclides in some Tunisian thermo-mineral springs

Radioactivity in some Tunisian thermo-mineral springs (11 hot mineral springs and one cold spring) has been determined for the first time in Tunisia using radiochemical separation procedures. The obtained results show that 238U activity concentrations vary between 1.5 and about 43 mBq/l. The measured activities of 234U and 226Ra range from 1.1 to about 82.2 mBq/l and 34-3,900 mBq/l. respectively. The radioactive disequilibria in these waters are in excess of concentration of 234U compared to that of 238U. The 226Ra/234U activity ratios are high and in the range of 9.0-691.0). U, Th and Ra activities are similar to those published for other non-polluted regions of the world. Radioactivity in the only cold mineral water from A?n Oktor is very low, and thus health hazards due to the consumption of this water are not expected.     

Radionuclide and chemical concentrations in mineral waters at Saratoga Springs, New York

A project to characterize the radionuclide and chemical components in natural spring waters in the vicinity of Saratoga Springs, New York (USA) has been completed. As a result of the measured radionuclide and chemical content, eight springs were labeled as mineral waters, whereas three springs contained very low concentrations of these components. The mineral waters were highly enriched in alkaline and alkaline-earth elements, as well as chloride ions. Three isotopes of radium ((224)Ra, (226)Ra, (228)Ra) were detected in the mineral waters and reached concentrations of 1, 20, and 2 Bq/L, respectively. Overall, the (226)Ra isotope constituted about 80% of the total radioactivity measured in the water samples. Dissolved uranium concentrations in the mineral waters were very low (mean approximately 50 mBq/L).     

Determination and comparison of uranium and radium isotopes activities and activity ratios in samples from some natural water sources in Morocco.

Radiochemical results (238U, 226Ra and 228Ra activities; 234U/238U, 228Ra/226Ra and 226Ra/238U activity ratios) are reported for 42 natural water samples collected from wells, hot mineral springs, rivers, tap water, lakes and irrigation water in 15 Moroccan locations. Results show that 238U activity varies between 4.5 and about 309 mBq l(-1) in wells, 0.6 and 8.5 mBq l(-1) in hot springs, 9.7 and 28 mBq l(-1) in rivers, 2.5 and 16 mBq l(-1) in tap waters and between 6 and 24 mBq l(-1) in lakes. The 234U/238U activity ratio varies in the range 0.87-3.35 in all analyzed water samples except for hot springs where it reaches values higher than 7. Unlike well water, mineral water samples present low 238U activities and high 234U/238U activity ratios and 226Ra activities. The highest activity of radium in mineral water is 150 times higher than the highest activity of 226 Ra found in well water. 226Ra/238U activity ratios are in the ranges 0.07-1.14 in wells, 0.04-0.38 in rivers, 0.04-2.48 in lakes, and 1.79-2115 in springs. The calculated equivalent doses to all the measured activities are inferior to the maximum contaminant levels recommended by the International Commission of Radioprotection and they do not present any risk for public health in Morocco.     

Estimating the dynamics of groundwater input into the coastal zone via continuous radon-222 measurements

Submarine groundwater discharge (SGD) into the coastal zone has received increased attention in the last few years as it is now recognized that this process represents an important pathway for material transport. Assessing these material fluxes is difficult, as there is no simple means to gauge the water flux. To meet this challenge, we have explored the use of a continuous radon monitor to measure radon concentrations in coastal zone waters over time periods from hours to days. Changes in the radon inventories over time can be converted to fluxes after one makes allowances for tidal effects, losses to the atmosphere, and mixing with offshore waters. If one assumes that advective flow of radon-enriched groundwater (pore waters) represent the main input of 222Rn in the coastal zone, the calculated radon fluxes may be converted to water fluxes by dividing by the estimated or measured 222Rn pore water activity. We have also used short-lived radium isotopes (223Ra and 224Ra) to assess mixing between near-shore and offshore waters in the manner pioneered by. During an experiment in the coastal Gulf of Mexico, we showed that the mixing loss derived from the 223Ra gradient agreed very favorably to the estimated range based on the calculated radon fluxes. This allowed an independent constraint on the mixing loss of radon-an important parameter in the mass balance approach. Groundwater discharge was also estimated independently by the radium isotopic approach and was within a factor of two of that determined by the continuous radon measurements and an automated seepage meter deployed at the same site.     

Contamination of settling ponds and rivers as a result of discharge of radium-bearing waters from Polish coal mines

Saline waters from underground coal mines in Poland often contain natural radioactive isotopes, mainly 226Ra from the uranium decay series and 228Ra from the thorium series. Approximately 40% of the total amount of radium remains underground as radioactive deposits, but 225 MBq of 226Ra and 400 MBq of 228Ra are released daily into the rivers along with the other mine effluents from all Polish coal mines. Technical measures such as inducing the precipitation of radium in gobs, decreasing the amount of meteoric inflow water into underground workings, etc. have been undertaken in several coal mines, and as a result of these measures, the total amount of radium released to the surface waters has diminished by about 60% during the last 5-6 years. Mine water can have a severe impact on the natural environment, mainly due to its salinity. However, associated high levels of radium concentration in river waters, bottom sediments and vegetation have also been observed. Sometimes radium concentrations in rivers exceed 0.7 kBq/m3, which is the permitted level for waste waters under Polish law. The extensive investigations described here were carried out for all coal mines and on this basis the total radium balance in the effluents has been calculated. Measurements in the vicinity of mine settling ponds and in rivers have given us an opportunity to study radium behaviour in river waters and to assess the degree of contamination. Solid waste materials with enhanced natural radioactivity have been produced in huge amounts in the power and coal industries in Poland. As a result of the combustion of coal in power plants, low-radioactive waste materials are produced, with 226Ra concentration seldom exceeding a few hundreds of Bq/kg. A different situation is observed in coal mines, where, as a result of precipitation of radium from radium-bearing waters, highly radioactive deposits are formed. Sometimes the radioactivity of such materials is extremely high; precipitates from coal mines may have radium concentrations of 400,000 Bq/kg--equivalent to 3% uranium ore. Usually, such deposition takes place underground, but sometimes co-precipitation of radium with barium takes place on the surface, in settling ponds and in rivers. Therefore management of solid waste with technologically enhanced natural radioactivity (TENR) is a very important subject.     

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).     

Radiological hazards of TENORM in the wasted petroleum pipes

Disposal petroleum pipes containing sludge and scale as a technically enhanced natural occurring radioactive material (TENORM) leads to internal and external radiation hazards and then a significant radiation dose to the workers. In order to contribute to a future waste management policy related to the presence of TENORM in the disposal sites of wasted petroleum pipes, scale and sludge as TENORM wastes are collected form these disposal pipes for radiometric analysis. These pipes are imported from onshore oilfields at south Sinai governorate, Egypt. The highest mean ²²⁶Ra and ²²⁸Ra concentrations of 519 and 50 kBq/kg respectively, were measured in scale samples. Sludge lies within the normal range of radium concentration. The average absorbed dose caused by the exposure to the wasted pipes equal to 4.09 μGy h⁻¹ from sludge and 262 μGy h⁻¹ from scale. This is much higher than the acceptable level of 0.059 μGy h⁻¹. Due to radon inhalation, important radon related parameters are calculated which advantage in internal dose calculation. Fairly good correlation between real radium content and radon exhalation rate for sludge samples is obtained. The hazards from sludge come from its high emanation power for radon which equal to 3.83%. The obtained results demonstrate the need of screening oil residues for their radionuclide content in order to decide about their final disposal.     

Soil radium, soil gas radon and indoor radon empirical relationships to assist in post-closure impact assessment related to near-surface radioactive waste disposal

Least squares (LS), Theil’s (TS) and weighted total least squares (WTLS) regression analysis methods are used to develop empirical relationships between radium in the ground, radon in soil and radon in dwellings to assist in the post-closure assessment of indoor radon related to near-surface radioactive waste disposal at the Low Level Waste Repository in England. The data sets used are (i) estimated ²²⁶Ra in the <2 mm fraction of topsoils (eRa226) derived from equivalent uranium (eU) from airborne gamma spectrometry data, (ii) eRa226 derived from measurements of uranium in soil geochemical samples, (iii) soil gas radon and (iv) indoor radon data. For models comparing indoor radon and (i) eRa226 derived from airborne eU data and (ii) soil gas radon data, some of the geological groupings have significant slopes. For these groupings there is reasonable agreement in slope and intercept between the three regression analysis methods (LS, TS and WTLS). Relationships between radon in dwellings and radium in the ground or radon in soil differ depending on the characteristics of the underlying geological units, with more permeable units having steeper slopes and higher indoor radon concentrations for a given radium or soil gas radon concentration in the ground. The regression models comparing indoor radon with soil gas radon have intercepts close to 5 Bq m⁻³ whilst the intercepts for those comparing indoor radon with eRa226 from airborne eU vary from about 20 Bq m⁻³ for a moderately permeable geological unit to about 40 Bq m⁻³ for highly permeable limestone, implying unrealistically high contributions to indoor radon from sources other than the ground. An intercept value of 5 Bq m⁻³ is assumed as an appropriate mean value for the UK for sources of indoor radon other than radon from the ground, based on examination of UK data. Comparison with published data used to derive an average indoor radon: soil ²²⁶Ra ratio shows that whereas the published data are generally clustered with no obvious correlation, the data from this study have substantially different relationships depending largely on the permeability of the underlying geology. Models for the relatively impermeable geological units plot parallel to the average indoor radon: soil ²²⁶Ra model but with lower indoor radon: soil ²²⁶Ra ratios, whilst the models for the permeable geological units plot parallel to the average indoor radon: soil ²²⁶Ra model but with higher than average indoor radon: soil ²²⁶Ra ratios.     

Simulation of pollution buffering capacity of wetlands fringing the Lake Victoria

Lake Victoria has undergone substantial and most negative changes, especially over the last 30 years. One of the driving factors is nutrient enrichment from human activities in the catchment, which is causing eutrophication. This has been associated with, among others, the rapid proliferation of water hyacinth, alga blooms, and with general disruption of the lake ecosystem. Most of pollution to the lake flow via the natural wetlands. In order to understand how wetlands function within the Lake Victoria ecosystem a wetland model has been developed. The main objective of the model is to establish and simulate the buffering processes and capacity of individual wetlands (that is, their ability to absorb sediments, nutrients and pollutants) within the Lake Victoria basin. It was found that in both seasonal and permanent swamp there is a net export of organic matter produced in the wetlands. Most of the inorganic phosphorous were retained in the wetlands (60% to 90% removal) while there was a negative retention of nitrates probably due to the export of organic matter which associate very much with nitrates.     

Source of radium in a well-water-augmented Florida lake

A study of the lake waters of Saddleback Lake, Florida was undertaken with the goal of determining the source of elevated radium activities in the lake. Four radium isotopes, (226)Ra, (228)Ra, (223)Ra and (224)Ra, were measured and activities of all the four radium isotopes were substantially greater in the well water used to augment the lake as compared to the lake waters. In the surface water, radium activities were highest close to the well used for augmentation in the initial sampling. Activities initially decreased with time after augmentation from the well ceased. The (223)Ra/(226)Ra activity ratio decreased during the first month of sampling and closely followed an exponential decay curve based on the (223)Ra decay constant. Trends in the activities and the (223)Ra/(226)Ra activity ratios support the conclusion that the well used to augment the lake was the dominant source of (223)Ra and (226)Ra to Saddleback Lake during this study. The (224)Ra/(226)Ra activity ratio did not follow the expected trend of exponential decay based on the (224)Ra decay constant. While the augmentation well supplied some (224)Ra, these results suggest that there must be an additional source of (224)Ra to the lake. The most likely additional source of (224)Ra appears to be the ingrowth of (224)Ra on the sediment within the lake from (228)Ra (via (228)Th).     

Systematic radium survey in spring waters of Slovenia

Radium (226Ra) concentration in 115 Slovenian springs ranged from 7.8 to 43.1 Bq m(-3), well below the current Slovenian limit of 1000 Bq m(-3) for drinking water. It showed two distributions, one grouped at around 24 Bq m(-3) and the other at around 37 Bq m(-3). Contrary to expectation, the level of radium does not always relate to the aquifer type. Only at aquifers and springs composed of acid, intermediate and basic igneous and metamorphic rocks, did radium concentration exceed 36 Bq m(-3) and was below this value at the majority of aquifers composed of carbonate and other sedimentary rocks.     

Radionuclides in hot mineral spring waters in Jordan

Hot mineral springs in Jordan are very attractive to people who seek physical healing but they are unaware of natural radioactive elements that may be contained in the hot mineral water. The activities of the natural radioactive isotopes were measured and the concentrations of the parents of their natural radioactive series were calculated. The measured radionuclides were 234Th, 226Ra, 214Pb, 214Bi, 228Ac, 228Th, 212Pb, 212Bi and 208Tl. In addition the activities of 235U and 40K were measured. The activities ranged from 0.14 to 34.8 Bq/l, while the concentrations of parent uranium and thorium isotopes ranged from 3.0 x 10(-3) to 0.59 mg/l. The results were compared with those for drinking water.     

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.     

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.     

Radon concentration in soil gas around local disjunctive tectonic zones in the Krakow area

The purpose of this study was to investigate radon in the vicinity of geologic fault zones within the Krakow region of Poland, and to determine the influence of such formations on enhanced radon concentrations in soil. Radon ((222)Rn and (220)Rn) concentration measurements in soil gas (using ionization chamber AlphaGUARD PQ2000 PRO and diffusion chambers with CR-39 detectors), as well as radioactive natural isotopes of radium, thorium and potassium in soil samples (using gamma ray spectrometry with NaI(Tl) and HPGe detectors), were performed. Site selection was based on a geological map of Krakow. Geophysical methods (ground penetrating radar and shallow acoustic seismic) were applied to recognize the geological structure of the area and to locate the predicted courses of faults. Elevated levels of radon and thoron in soil gas were found in the study area when compared with those observed in an earlier survey covering Krakow agglomeration. For (222)Rn, the arithmetic mean of registered concentration values was 39 kBq/m(3) (median: 35.5 kBq/m(3)). For (220)Rn, the arithmetic mean was 10.8 kBq/m(3) and median 11.8 kBq/m(3).     

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.     

Association of organic matter, iron and inorganic phosphorus in lake waters

Gel permeation chromatography was used to fractionate ³²PO₄³⁻ labelled components by molecular size in filtered, destabilized lake foam, concentrated lake water, and lake sediment extracts. Evidence is presented for the abiotic formation of organic matter iron inorganic P complexes in lake foam, water and sediments. ³²PO₄^staggered was found to excahnge with low molecular weight, dissolved P fraction, probably an organic matter -Fe- inorganic P complex, but not with a high molecular weight, non-inorganic dissolved reactive P pool, hypothesized to be similar to the dimer. Our experiments suggest that inorganic P binding by high molecular weight organic matter may play a significant role in the P cycle. If the bound P is unavailable to algae and bacteria, the complexes could explain Rigler's (1968) hypothesis that the molybdenum blue technique may overestimate the free orthophosphate concentration by 10–100 times.     

A simple bubbling system for measuring radon (222Rn) gas concentrations in water samples based on the high solubility of radon in olive oil

Based on the different levels of solubility of radon gas in organic solvents and water, a bubbling system has been developed to transfer radon gas, dissolving naturally in water samples, to an organic solvent, i.e. olive oil, which is known to be a good solvent of radon gas. The system features the application of a fixed volume of bubbling air by introducing a fixed volume of water into a flask mounted above the system, to displace an identical volume of air from an air cylinder. Thus a gravitational flow of water is provided without the need for pumping. Then, the flushing air (radon-enriched air) is directed through a vial containing olive oil, to achieve deposition of the radon gas by another bubbling process. Following this, the vial (containing olive oil) is measured by direct use of gamma ray spectrometry, without the need of any chemical or physical processing of the samples. Using a standard solution of 226Ra/222Rn, a lowest measurable concentration (LMC) of radon in water samples of 9.4 Bq L(-1) has been achieved (below the maximum contaminant level of 11 Bq L(-1)).