Natural radionuclides in major aquifer systems of the Paraná sedimentary basin, Brazil

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Abstract

This paper describes the natural radioactivity of groundwater occurring in sedimentary (Bauru and Guarani) and fractured rock (Serra Geral) aquifer systems in the Paraná sedimentary basin, South America that is extensively used for drinking purposes, among others. The measurements of gross alpha and gross beta radioactivity as well the activity concentration of the natural dissolved radionuclides 40K, 238U, 234U, 226Ra, 222Rn, 210Po and 210Pb were held in 80 tubular wells drilled in 21 municipalities located at São Paulo State and its border with Mato Grosso do Sul State in Brazil. Most of the gross alpha radioactivity data were below 1 mBq/L, whereas values exceeding the gross beta radioactivity detection limit of 30 mBq/L were found. The radioelement solubility in the studied systems varied according to the sequence radon>radium>other radionuclides and the higher porosity of sandstones relatively to basalts and diabases could justify the enhanced presence of dissolved radon in the porous aquifer. The implications of the data obtained in terms of standards established for defining the drinking water quality have also been discussed. The population-weighted average activity concentration for these radionuclides was compared to the guideline value of 0.1 mSv/yr for the total effective dose and discussed in terms of the choice of the dose conversion factors.

Highlights

► Integration of distinct radiometric data acquired in groundwaters. ► Radiation dose in important hydrological resources in South America. ► Contribution of 226Ra for the more accentuated radiation dose in aquifers. ► Dose factors for Rn and generation of values exceeding the maximum of 0.1 mSv/yr.

Introduction

Estimates of the volumes of various kinds of water on, above, and under the surface of the earth reveal that fresh water makes up only 2.5% of all the water on earth, with groundwater comprising 99% of the earth's available fresh water (Delleur, 1999). Groundwater can be found in all three classes of rocks, i.e. igneous, sedimentary and metamorphic. In fractured rock aquifers, groundwater is stored in the fractures, joints, bedding planes and cavities of the rock mass; water availability is largely dependent on the nature of the fractures and their interconnection. However, sedimentary aquifers, also called unconsolidated aquifers, generally contain the greatest amounts of water due to their greater porosity. For instance, sandstones typically exhibit porosity between 5% and 30%, in contrast to the values of 0–10% often reported for the fractured crystalline rocks (Delleur, 1999). Therefore, sedimentary basins are an important source of groundwater worldwide, where many of them contain extensive multi-layered aquifer systems consisting of permeable sediments laid down at various times in the past.

In recent years, there has been growing public concern about the problems of groundwater quantity and quality as many aquifers are affected by adverse water quality and issues of the hydrological resources are faced with these challenges as a result of the actions or inactions of the responsible entities. Even in the well-known aquifers there are increasing concerns about pollution from diffuse source inputs and an ever-increasing need to balance resources spent on the groundwater management as compared with other priority regions. In managing it, increasing use is being made of information generated from hydrochemical studies held for understanding the release of constituents to the liquid phase due to water–rock interactions.

Potential health hazards from natural radionuclides in consuming water have been considered worldwide, with many countries adopting the guideline activity concentration for drinking water quality recommended by WHO (2008). In general, the recommendations apply to routine operational conditions of water supply systems, however, special attention must be given when groundwaters are utilized for public water supplies.

40K is the only radioactive isotope of potassium and is released to water bodies as a consequence of water/soil–rock interactions (Davis, 1963). Thorium has been considered a highly insoluble element in water due to its presence in minerals of difficult dissolution (Langmuir and Herman, 1980). Uranium tends to be mobile under conditions present at the earth's surface; its concentration generally ranges from 0.1 to 10 μg L−1 in rivers, lakes and groundwaters (Fritz and Fontes, 1980, Ivanovich and Harmon, 1992). WHO (2008) defined guidance levels in drinking water for 238U and daughters like 234U, 230Th, 226Ra, 222Rn, 210Pb, and 210Po, whose activity concentration evaluation involves sophisticated and time-consuming procedures and are generally performed if the gross alpha and beta measurements have exceeded 0.5 and 1 Bq/L, respectively.

Sandstone aquifers have been recognized of importance on the generation of enhanced radioactivity levels worldwide mainly due to 222Rn and radium isotopes 226Ra and 228Ra (Vengosh et al., 2009). Such rock types are widely spread in Paraná sedimentary basin, South America; however, igneous basic intruse rocks also outcrop in large surface area. This paper performs a comparative study of the radiation dose provided by sedimentary/fractured rock aquifers in Paraná basin, taking into account gross alpha/beta measurements and activity concentration data of radionuclides belonging to the 238U decay series.

Section snippets

Research region

Fig. 1 shows the location of the studied region which is situated between parallels 20–24° southern latitude and meridians 47–52° western longitude. It is inserted within Paraná basin whose surface area corresponds to 1.6×106 km2 and comprises southern Brazil (1×106 km2 in the states of Mato Grosso, Mato Grosso do Sul, Goiás, Minas Gerais, São Paulo, Paraná, Santa Catarina and Rio Grande do Sul), eastern Paraguay (0.1×106 km2), NW Uruguay (0.1×106 km2) and the northeastern extreme corner of

Sampling and analytical methods

Three aquifer systems have been focused in this paper, i.e. two sedimentary aquifers (Bauru and Guarani aquifers) and one fractured rock aquifer (Serra Geral aquifer). Groundwater and rock samples have been analyzed. The groundwater sampling was performed in 21 localities of São Paulo and Mato do Grosso Sul States in Brazil, whereas the rock samples were provided from outcrops in roads at São Paulo State. The groundwater samples (80) for physical and chemical analyses were collected along the

Temperature, conductivity, sodium and gross alpha/beta readings

The occurrence of water at elevated temperatures (above 40 °C) was identified in deep tubular wells drilled in Guarani aquifer as a consequence of the great depths reached by the aquifer system (almost 2 km) and thick confining basaltic cover (Table 2). An excellent linear relationship (r=0.93) between temperature and geostatic pressure in Guarani aquifer has been reported (Bonotto, 2006), confirming the results obtained elsewhere (Teissedre and Barner, 1981, Silva, 1983) that relates the

Population-weighted average activity concentrations

WHO (2008) established guidance levels for several radionuclides in drinking water, assuming that 730 L is the annual ingested volume of water. The following guidance levels for the activity concentration in drinking water have been proposed: 238U=10 Bq/L; 234U=1 Bq/L; 226Ra=1 Bq/L; 210Pb and 210Po=0.1 Bq/L. The recommended reference dose level of the committed dose equal to 0.1 mSv from 1 year's consumption of drinking water has been accepted by most WHO Member States, the European Commission, FAO

Concluding remarks

Groundwaters of Bauru, Serra Geral and Guarani aquifers in the Paraná sedimentary basin, South America, have been analyzed in terms of the gross alpha/beta activity and natural radioactivity due to 40K and nuclides belonging to the 238U decay series. Most of the gross alpha readings were below 1 mBq/L, whereas the gross beta activity concentration was normally distributed (mean value=0.24 Bq/L). The radionuclides release to the liquid phase varied according to the aquifer type, existing a direct

Acknowledgements

FAPESP (Foundation Supporting Research in São Paulo State) and CNPq (National Council for Scientific and Technologic Development) in Brazil are greatly thanked for financial support of this investigation.

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