A 210Pb chronological study in sediments from poços de caldas alkaline massif (PCAM), Brazil.

The Constant Flux and Constant Sedimentation (CF:CS) of supported/excess 210Pb model was successfully used to study sediment profiles from Antas stream, located in the region of Poços de Caldas city, Minas Gerais State, Brazil. Historical changes in the region were tracked from evaluating the sedimentation rate by the 210Pb method. In that site, Osamu Utsumi mine was the first mining-industrial complex for the production of concentrated uranium in Brazil. Four sediment testimonies were sampled along Antas stream in order to determine sedimentation rates using 210Pb as geochronometer. 210Pb and 238U activity concentrations were determined in sediment samples by alpha spectrometry, allowing to find the excess 210Pb present in the sediments. Additionally, the main oxides, organic matter, particles size and water composition were determined in order to assist the results interpretation from radionuclides data. The results allowed find one (profile PKS-4) or two (profiles PKS-1, PKS-2 and PKS-3) sedimentation rates, probably due to changes in the sediments input regime in the region. The sedimentation rates were in the range between 0.26 and 0.94 g/cm2.year, corresponding to the interval of linear sedimentation rate of 0.21 - 0.92 cm/year. The deposition year in the bottom of PKS-4 profile as estimated from the sedimentation rate coincided with the construction year of Bortolan dam (1956). Large touristic interventions carried out at Poços de Caldas city from 1920s coupled to unbridled urbanization, industrialization and demographic growth there in the second half of the twentieth century possibly caused the changes found in the sedimentation rates.

The use of γ-rays analysis by HPGe detector to assess the gross alpha and beta activities in waters.

This paper describes an alternative method for evaluating gross alpha and beta radioactivity in waters by using γ-rays analysis performed with hyper-pure germanium detector (HPGe). Several gamma emissions related to α and ß- decays were used to provide the activity concentration data due to natural radionuclides commonly present in waters like 40K and those belonging to the 238U and 232Th decay series. The most suitable gamma emissions related to ß- decays were 214Bi (1120.29 keV, 238U series) and 208Tl (583.19 keV, 232Th series) as the equation in activity concentration yielded values compatible to those generated by the formula taking into account the detection efficiency. The absence of isolated and intense γ-rays peaks associated to α decays limited the choice to 226Ra (186.21 keV, 238U series) and 224Ra (240.99 keV, 232Th series). In these cases, it was adopted appropriate correction factors involving the absolute intensities and specific activities for avoiding the interferences of other γ-rays energies. The critical level of detection across the 186-1461 keV energy region corresponded to 0.010, 0.023, 0.038, 0.086, and 0.042 Bq/L, respectively, for 226Ra, 224Ra, 208Tl, 214Bi and 40K. It is much lower than the WHO guideline reference value for gross alpha (0.5 Bq/L) and beta (1.0 Bq/L) in waters. The method applicability was checked by the analysis of groundwater samples from different aquifer systems occurring in the Brazilian states of São Paulo, Minas Gerais and Mato Grosso do Sul. The waters exhibit very different chemical composition and the samples with the highest radioactivity levels were those associated with lithotypes possessing enhanced uranium and thorium levels. The technique allowed directly discard the 40K contribution to the gross beta activity as potassium is an essential element for humans.

A comparative evaluation of the CF:CS and CRS models in 210Pb chronological studies applied to hydrographic basins in Brazil.

The Constant Flux: Constant Sedimentation (CF:CS) and Constant Rate of Supply (CRS) of unsupported⧸excess (210)Pb models have been applied to a (210)Pb data set providing of eighteen sediments profiles sampled at four riverine systems occurring in Brazil, South America: Corumbataí River basin (S1=Site 1, São Paulo State), Atibaia River basin (S2=Site 2, São Paulo State), Ribeirão dos Bagres basin (S3=Site 3, São Paulo State) and Amazon River mouth (S4=Site 4, Amapá State). These sites were chosen for a comparative evaluation of the performance of the CF:CS and CRS models due to their pronounced differences on the geographical location, geological context, soil composition, biodiversity, climate, rainfall, and water flow regime, among other variable aspects. However, all sediments cores exhibited a common denominator consisting on a database built from the use of the same techniques for acquiring the sediments major chemical composition (SiO2, Al2O3, Na2O, K2O, CaO, MgO, Fe2O3, MnO, P2O5, TiO2 and LOI-Loss on Ignition) and unsupported/excess (210)Pb activity data. In terms of sedimentation rates, the performance of the CRS model was better than that of the CF:CS model as it yielded values more compatible with those expected from field evidences. Under the chronological point of view, the CRS model always provided ages within the permitted range of the (210)Pb-method in the studied sites, whereas the CF:CS model predicted some values above 150 years. The SiO2 content decreased in accordance with the LOI increase in all cores analyzed and such inverse relationship was also tracked in the SiO2-LOI curves of historical trends. The SiO2-LOI concentration fluctuations in sites S1 and S3 also coincided with some Cu and Cr inputs in the drainage systems.

Towards a Brazilian radon map: consortium radon Brazil.

Recently, the idea of generating radon map of Brazil has emerged. First attempts of coordinating radon surveys--carried out by different groups across the country--and initial discussions on how to proceed on a larger scale were made at the First Brazilian Radon Seminary, Natal, September 2012. Conventionally, it is believed that indoor radon is no major problem in Brazil, because the overall benign climate usually allows high ventilation rates. Nevertheless, scattered measurements have shown that moderately high indoor radon concentrations (up to a few hundred Bq m⁻³) do occur regionally. Brazilian geology is very diverse and there are regions where an elevated geogenic radon potential exists or is expected to exist. Therefore, a Brazilian Radon Survey is expected to be a challenge, although it appears an important issue, given the rising concern of the public about the quality of its environment.

²²²Rn, ²²6Ra and hydrochemistry in the Bauru Aquifer System, São José do Rio Preto (SP), Brazil.

In this paper, the (222)Rn and (226)Ra activity concentration was measured in groundwater samples collected from the Bauru Aquifer System, São José do Rio Preto city, São Paulo State, Brazil. The site has been selected for a detailed radiometric survey due to the large number of tubular wells drilled in the aquifer there, which provide water for ~70% of the local population. Despite the importance of groundwater for the local water-supply system, there is a lack of both (222)Rn and (226)Ra data in the municipality. Establishment of these data is relevant to assure that the water quality from a radiological point of view, is not health threat. São José do Rio Preto city is geologically situated in Bauru Group that is located within the Paraná sedimentary basin. The monitoring program involved the collection of 50 groundwater samples from deep tubular wells during three field campaigns held from 17th to 19th January 2011, from 2nd to 3rd August 2011 and in 30th November 2011. Temperature and pH readings were realized in the field, whereas (222)Rn and (226)Ra analysis were performed at the laboratory using the Alpha Guard-Aquakit analytical protocol, which allowed us to obtain (222)Rn activity concentration ranging from 0.69 to 14.95 Bq/L. These data indicate that the abundances of (222)Rn and (226)Ra in the groundwater system of Bauru Group is below the WHO guideline limit of 100 Bq/L. Chemical analysis has been also realized for major cations and anions in order to better understand the water features in the municipality.

Evaluation of the chromium contamination at Ribeirão dos Bagres, Franca (SP), Brazil, by the ²¹°Pb method.

This paper presents a chronological study focusing the use of ²¹°Pb in four sediment cores collected at Ribeirão dos Bagres in the region of Franca, São Paulo State, Brazil. When evaluating the sedimentation rate by using the ²¹°Pb method, it was possible to monitor historical changes occurring in the concentrations of chromium present in the sediments. In order to do so, several specific parameters were determined in sediments, as chromium concentration, major oxides, organic matter, grain size, and chemical and physical-chemical parameters of waters. The sediments possessed a Cr concentration range of 0.83-26.25mg/kg that is below the world's average of shales. The sedimentation rates obtained from the ²¹°Pb analysis were between 0.07 and 0.77 g cm⁻²year⁻¹, while the linear sedimentation rate was from 0.6 to 3.2 cm/year. The adoption of the CIC (Constant Initial Concentration) ²¹°Pb model allowed characterize older sediments, aged 177 years, and younger sediments, aged 4 years. The organic matter in the sediments was more abundant in the first few centimeters of practically all profiles, and the analysis of oxides showed that silica is the major constituent of the sediments, in which there is predominance of sand and silt. In addition, the analysis of the physical and chemical parameters of waters indicated that they are suitable for navigation and natural harmony landscape.

Radon in groundwater contaminated by dissolved hydrocarbons in Santa Bárbara d'Oeste, São Paulo State, Brazil.

This investigation reported the (222)Rn activity concentration and dissolved hydrocarbon content in groundwater collected in three gas stations where occurred tanks leaks, in Santa Barbara d'Oeste, São Paulo State, Brazil. The results indicated a tendency of correlation between the radon and BTEX, suggesting that the presence of dissolved hydrocarbons increase the radon concentration in water, due to the preferential partition at this phase. The radiometric data are useful for the detection of residual contamination and dissolved hydrocarbon plumes in groundwater, reinforcing the findings of previous studies held elsewhere.

Uranium distribution and radon exhalation from Brazilian dimension stones.

This paper provides evaluations of the radiometric behavior and exhalation patterns of radon gas in decorative and dimension stones explored in the Brazilian states of Minas Gerais and Espírito Santo, given the importance of determining radon gas concentrations in human-inhabited environments. A total of 10 silicate rock types were studied, featuring different petrographic/petrophysical characteristics given by seven magmatic rocks (three of which are granitic pegmatites) and three metamorphic rocks. The study, comprising radiometric data of U and monitoring of (222)Rn gas exhalation, shows a strong correlation between petrographic parameters and the physical properties of rocks. U levels ranged between 2.9 and 37 ppm, revealing a good coherence between the presence and the absence of radioactive element-bearing accessory minerals for each rock type. The rate of radon exhalation from the stones is related to the petrographic/petrophysical features of each material. By comparing the (222)Rn level generated by a rock to the amount effectively emanated by it, the rate of emanated gas proves to be insignificant; also, a rock that produces more Rn will not always emanate more. Simulations performed to estimate the radon levels inside residences or any given indoor environment showed that nine samples attained values below the 4 pCi/L EPA limit, whereas one was above that limit.

Natural radioactivity and radon exhalation rate in Brazilian igneous rocks.

This paper reports the natural radioactivity of Brazilian igneous rocks that are used as dimension stones, following the trend of other studies on the evaluation of the risks to the human health caused by the rocks radioactivity as a consequence of their use as cover indoors. Gamma-ray spectrometry has been utilized to determine the (40)K, (226)Ra and (232)Th activity concentrations in 14 rock types collected at different quarries. The following activity concentration range was found: 12.18-251.90 Bq/kg for (226)Ra, 9.55-347.47 Bq/kg for (232)Th and 407.5-1615.0 Bq/kg for (40)K. Such data were used to estimate Ra(eq), H(ex) and I(γ), which were compared with the threshold limit values recommended in literature. They have been exceeded for Ra(eq) and H(ex) in five samples, where the highest indices corresponded to a rock that suffered a process of ductile-brittle deformation that caused it a microbrecciated shape. The exhalation rate of Rn and daughters has also been determined in slabs consisting of rock pieces ~10 cm-long, 5 cm-wide and 3 cm-thick. It ranged from 0.24 to 3.93 Bq/m(2)/h and exhibited significant correlation with eU (=(226)Ra), as expected. The results indicated that most of the studied rocks did not present risk to human health and may be used indoors, even with low ventilation. On the other hand, igneous rocks that yielded indices above the threshold limit values recommended in literature may be used outdoors without any restriction or indoors with ample ventilation.

Sedimentation rates in Atibaia River basin, São Paulo State, Brazil, using 210Pb as geochronometer.

The constant initial concentration (CIC) of unsupported/excess (210)Pb model was successfully used to assess (210)Pb data of nine sediment cores from Atibaia River basin, São Paulo State, Brazil. The (210)Pb-based apparent sediment mass accumulation rates ranged from 47.7 to 782.4 mg/cm(2)yr, whereas the average linear sedimentation rates between 0.16 and 1.32 cm/yr, which are compatible with the calculated sediment mass fluxes, i.e. a higher sediment mass accumulation rate yielded a higher linear sedimentation rate. The higher long-term based accumulation rate tended to be found in topographically softer regions. This occurs because the sediments are preferentially transported in topographically steeper regions instead of being deposited. Anthropic activities like deforestation possibly interfered with the natural/normal sedimentation processes, which increased in accordance with modifications on the channel drainage. The radionuclide geochronology as described in this paper allows determination of sedimentation rates that are compatible with values estimated elsewhere. The adoption of an appropriate factor generated from previous laboratory experiments resulted in a successful correction for the (222)Rn-loss from the sediments, bringing the estimate of the parent-supported (in-situ produced) (210)Pb to reliable values required by the CIC model.

The natural radioactivity in Guarani aquifer groundwater, Brazil.

The measurements of gross alpha and gross beta radioactivity in groundwater samples from Guarani aquifer in Brazil are reported in this paper together with the activity concentration of the natural dissolved radionuclides (40)K, (238)U, (234)U, (226)Ra, (222)Rn, (210)Po, (210)Pb, (232)Th, (228Th), and (228)Ra. Most of the gross alpha radioactivity values were below the critical level of detection corresponding to 1 mBq/L, however, the whole data set for the gross beta radioactivity and radionuclides (40)K, (238)U, (234)U, (226)Ra, (222)Rn, (210)Po, (210)Pb, and (228)Ra was submitted to a statistical treatment, considering class intervals arranged in geometric progression, because of the great variability of the activity. The analysis indicated lognormal distribution of the data, as usually observed in samples taken from the natural context. An inverse relationship between the gross alpha and gross beta activity has been identified and is related to an increase in the K content in the water. The mobility coefficient has been estimated for (238)U, (226)Ra, (232)Th and (228)Ra in Guarani aquifer and the results indicated that the radioelement solubility in the studied system varies according to the following order: radium>uranium>thorium. The implications of the data obtained in terms of standards established for defining the drinking water quality have also been discussed.

Some possible evolutionary scenarios suggested by 36Cl measurements in Guarani aquifer groundwaters.

The Guarani aquifer underlies 1.2 M km2 in the Paraná sedimentary basin of South America and is an important source of water for industry, agriculture, and domestic supplies. To determine the sustainability of this aquifer we need to understand the dynamics of the groundwater system. This paper describes the first 36Cl measurements on aquifer groundwaters and some measurements on South American rainwaters, thought to be indicative of the recharge water. The results are compared to previous work in the region, including other radioisotope analyses. A simple model is developed, incorporating radioactive decay, allowing scenarios to be developed for mixing different waters at different mixing rates. Thus, mixing scenarios consistent with other hydrogeological and hydrogeochemical data could be assessed. A model that mixes fresh recharging waters with formational waters, that contain elevated chloride levels, but low (in situ) 36Cl levels, can explain most of the results presented here. The expectation that rainwater samples would provide a good end-member for modelling recharge proved problematic, however. As a consequence, it is suggested that either: the recharge waters are not sourced from the same locations as the rains; that the current rainfall and fallout conditions were significantly different in the past; or that the low levels of chloride in rainfall may have allowed some contamination of the samples by old (36Cl-free) chloride during the recharge process.

U-ages in soils and groundwater evidencing wet periods 400-600kyr ago in southeast Brazil.

(238)U and its radiogenic daughter (234)U have been utilized for dating soil formation and groundwater residence time during the last 1.5 million years, in this case based on the U-dissolution/precipitation occurring during modifications of the oxidation-reduction conditions. In this paper, we report a 400-600kyr proxy of wet periods from sediments occurring in a soil profile developed over rocks outcropping at the Paraná sedimentary basin in Brazil, and from groundwater exploited of Guarani aquifer at the same basin. The approaches indicated successful use of the U-modeled ages for suggesting wet periods exceeding the past 116-210kyr from previous studies.

Determination of weathering rate of the Morro do Ferro Th-REEs deposit, Brazil using U-isotope method.

The weathering rate was estimated by changes in (234)U/(238)U activity ratio (AR) and U content of rocks, borehole spoil and surface water samples at the Morro do Ferro Th-REEs deposit. The deposit is situated in the Poços de Caldas alkaline massif, Brazil. The south stream basin investigated in this paper has not been significantly affected by anthropogenic inputs of pollutants as compared to the Corumbataí River basin in São Paulo State, where the method was previously applied. The weathering rate derived utilizing the U-isotopes modeling corresponded to 0.015 mm/yr (67,000 years to weather 1m of rock under the actual climatic conditions). The estimated rate is very reasonable in comparison with the range of 0.015-0.05 mm/yr of land surface lowering within the entire caldera. It is also compatible with a rate of 0.013 mm/yr determined for the Salgado River basin in a semi-arid region in Bahia State, Brazil. The value generated is reliable and increases the potential use of the method for other different areas in Brazil and elsewhere, because it may be used in regions with different climatic conditions and (un)polluted basins.

A combined method for evaluating radon and progeny in waters and its use at Guarani aquifer, São Paulo State, Brazil.

A combined method for evaluating radon (222Rn) and progeny (214Pb and 214Bi) in water was developed by using inexpensive alpha scintillation counting and gamma ray spectrometry through NaI(Tl) scintillation detectors. A groundwater sample collected at the Poços de Caldas alkaline massif in Brazil was submitted to the technique in order to assure its applicability by comparing the volumetric activities by different methods. Similar volumetric activity was determined for 214Pb and 214Bi in the sample analyzed that is compatible with the expected condition of radioactive equilibrium between these nuclides. The combined method was successfully used to analyze groundwater samples from Guarani aquifer in São Paulo State, Brazil, and the results of the measurements indicated that 214Pb and 214Bi provide useful information concerning the evaluation of the drinking water quality in terms of radiological aspects. This is because they are directly identified in the water samples, without the need of requiring the assumption of the establishment of the transient equilibrium condition with its parent 222Rn.

Doses from 222Rn, 226Ra, and 228Ra in groundwater from Guarani aquifer, South America.

Groundwater samples were analysed for 222Rn, 226Ra, and 228Ra in Guarani aquifer spreading around 1 million km2 within four countries in South America, and it was found that their activity concentrations are lognormally distributed. Population-weighted average activity concentration for these radionuclides allowed to estimate a value either slightly higher (0.13 mSv/year) than 0.1 mSv for the total effective dose or two times higher (0.21 mSv/year) than this limit, depending on the choice of the dose conversion factor. Such calculation adds useful information for the appropriate management of this transboundary aquifer that is socially and economically very important to about 15 million inhabitants living in Brazil, Argentina, Uruguay and Paraguay.

Radon in groundwaters from Guarany aquifer, South America: environmental and exploration implications.

Groundwater and sandstone samples were analyzed for radon in Guarany aquifer, Paraná sedimentary basin, South America. The dissolved radon ranged between 3 and 3303pCi/l, being lognormally distributed, with a modal value of 1315pCi/l, and a median value of 330pCi/l. 222Rn leakage experiments for sandstones yielded a theoretical value of 1390pCi/l for 222Rn in water, showing that theoretical modeling can reliably be used to interpret laboratory and field data.

A method for evaluating 228Ra in environmental matrices and its use at Poços de Caldas plateau, Brazil.

This work describes a methodology developed for performing the extraction, detection and quantification of 228Ra in waters, suspended solids and sediments. The technique proved to be useful for analyzing samples from the hydrological environment of Morro do Ferro, Poços de Caldas plateau, Brazil. The 228Ra activity in underground waters of 5 boreholes drilled in the area varied from 0.02 up to 14.5 Bq/l, whereas for the surficial waters the variation was from 0.04 to 0.51 Bq/l; for the suspended solids, the values ranged from 1.5 up to 419 Bq/g, whereas it was possible to find a value of 2.04Bq/g for the sediments. These results show the applicability of the method for characterizing different matrices of environmental interest.

A laboratory study of the transfer of 234U and 238U during water-rock interactions in the Carnmenellis granite (Cornwall, England) and implications for the interpretation of field data.

Laboratory time-scale experiments were conducted on gravels from the Carnmenellis granite, Cornwall, England, with the purpose of evaluating the release of natural uranium isotopes to the water phase. The implications of these results for the production of enhanced 234U/235U activity ratios in Cornish groundwaters are discussed. It is suggested that the 234U/238U lab data can be used to interpret activity ratios from Cornwall, even when the observed inverse relationship between dissolved U and 234U/235U in leachates/etchates is taken into account.

The transfer of uranium isotopes 234U and 238U to the waters interacting with carbonates from Mendip Hills area (England).

Laboratory time-scale experiments were conducted on limestone and dolomite gravels from the Mendip Hills area, England, with the purpose of evaluating the release of 238U and 234U to different aqueous solutions. The 234U/238U activity ratio (AR) lab data were reliable to interpret the field data. The obtained values do not indicate a reduction in the amount of dissolved U and an increase in the AR of the remaining dissolved U as commonly observed for groundwater systems close to redox boundaries.