Isotope tracing of submarine groundwater discharge offshore Ubatuba, Brazil: results of the IAEA–UNESCO SGD project

Results of groundwater and seawater analyses for radioactive (³H, ²²²Rn, ²²³Ra, ²²⁴Ra, ²²⁶Ra, and ²²⁸Ra) and stable (D and ¹⁸O) isotopes are presented together with in situ spatial mapping and time series ²²²Rn measurements in seawater, direct seepage measurements using manual and automated seepage meters, pore water investigations using different tracers and piezometric techniques, and geoelectric surveys probing the coast. This study represents first time that such a new complex arsenal of radioactive and non-radioactive tracer techniques and geophysical methods have been used for simultaneous submarine groundwater discharge (SGD) investigations. Large fluctuations of SGD fluxes were observed at sites situated only a few meters apart (from 0 cm d⁻¹ to 360 cm d⁻¹; the unit represents cm³/cm²/day), as well as during a few hours (from 0 cm d⁻¹ to 110 cm d⁻¹), strongly depending on the tidal fluctuations. The average SGD flux estimated from continuous ²²²Rn measurements is 17 ± 10 cm d⁻¹. Integrated coastal SGD flux estimated for the Ubatuba coast using radium isotopes is about 7 × 10³ m³ d⁻¹ per km of the coast. The isotopic composition (δD and δ¹⁸O) of submarine waters was characterised by significant variability and heavy isotope enrichment, indicating that the contribution of groundwater in submarine waters varied from a small percentage to 20%. However, this contribution with increasing offshore distance became negligible. Automated seepage meters and time series measurements of ²²²Rn activity concentration showed a negative correlation between the SGD rates and tidal stage. This is likely caused by sea level changes as tidal effects induce variations of hydraulic gradients. The geoelectric probing and piezometric measurements contributed to better understanding of the spatial distribution of different water masses present along the coast. The radium isotope data showed scattered distributions with offshore distance, which imply that seawater in a complex coast with many small bays and islands was influenced by local currents and groundwater/seawater mixing. This has also been confirmed by a relatively short residence time of 1–2 weeks for water within 25 km offshore, as obtained by short-lived radium isotopes. The irregular distribution of SGD seen at Ubatuba is a characteristic of fractured rock aquifers, fed by coastal groundwater and recirculated seawater with small admixtures of groundwater, which is of potential environmental concern and has implications on the management of freshwater resources in the region.     

Radium and radium-daughter nuclides in carbonates: a brief overview of strategies for determining chronologies

Radium isotopes have been used extensively to trace the movement of groundwater as well as oceanic water masses, but these radionuclides (and their daughters) are also useful chronometers for the determination of the time scales of other Earth and environmental processes. The purpose of this overview is to present the application of Ra and Ra daughters in the dating of carbonates. We show that the choice of dating method (decay of excess radionuclide or ingrowth of daughter) depends strongly on the parent/daughter activity ratios in the water in which the carbonate was precipitated. Thus freshly precipitated carbonates uniformly show excesses of ²²⁶Ra relative to its parent ²³⁰Th, and ²²⁶Ra decay can provide ages of carbonates over Holocene time scales. In contrast, carbonates are precipitated in waters of greatly varying ²¹⁰Pb/²²⁶Ra. Corals, deep-sea hydrothermal vent clams and the shelled cephalopod Nautilus live in waters with significant dissolved ²¹⁰Pb and all show excesses of ²¹⁰Pb in their carbonate. Bivalve molluscs from nearshore and coastal waters, and carbonates deposited from groundwater environments (e.g. travertines) in which ²¹⁰Pb is efficiently scavenged from solution, show deficiencies of ²¹⁰Pb relative to ²²⁶Ra. In contrast, fish otoliths strongly discriminate against ²¹⁰Pb regardless of the environment in which the fish lives. Deficiencies of ²²⁸Th relative to ²²⁸Ra are common in all carbonates. Useful time ranges for the ²¹⁰Pb/²²⁶Ra and ²²⁸Th/²²⁸Ra chronometers are ∼100 y and ∼10 y, respectively.     

Radium geochemistry in Na-Cl type groundwater in Niigata Prefecture, Japan

Radium isotopes in 23 Na-Cl type groundwater sampled mainly from deep wells in Niigata Prefecture, which is the site of the largest oil- and gas-fields in Japan, were measured along with U isotopes, chemical components and hydrogen and oxygen isotope ratios to elucidate the distribution and behavior of Ra in a brackish environment underground. Also analyzed were U and Th isotopes in 38 rock samples collected from outcrops at 17 locations. Ra-226 concentrations (8.86-1637 mBq kg⁻¹) of groundwater samples roughly correlated with total dissolved solid (TDS) concentrations and other alkaline earth contents. Their ²²⁸Ra/²²⁶Ra activity ratios (0.32-5.2) were similar to or higher than the ²³²Th/²³⁸U activity ratios (0.6-1.7) in the rocks. The most likely transport mechanism of Ra isotopes into groundwater was due to their α-recoil from the solid phase, probably from the water-rock interface where Th isotopes had accumulated, and adsorption/desorption reaction based on the increase in ²²⁶Ra contents with TDS.     

Antlers of Cervus elaphus as biomonitors of ⁹⁰Sr in the environment

Adequate radioprotection of the environment requires the identification of biomonitors sensitive to the variation of its radionuclide content. Due to the chemical similarities between calcium and strontium, calcified tissues of mammals are considered to be good ⁹⁰Sr biomonitors. This work considered Cervus elaphus antlers which, being shed annually, can give information about the importance of radiostrontium contamination in an ecosystem in the time period required for the growth of the antler. The samples were collected at various points of W and SW Spain. The mean value of their ⁹⁰Sr content was (70 ± 43 (S.D.)) Bq/kg d.w., range (16-218) Bq/kg d.w., and the radionuclide was evenly distributed in the different parts of the antler. There was a good correlation between the antlers’ ⁹⁰Sr content and the ⁹⁰Sr deposited in the soil. The antlers’ content of ²²⁶Ra (from the natural uranium series) and the contents of some stable elements (Ca, Mg, Sr, and K) were also determined. The values for these stable elements were practically constant in the analyzed samples, and the concentrations measured decreased in the following order:Ca » Mg > K > Sr » ⁹⁰Sr > ²²⁶Ra     

建筑材料的放射性污染浅析

介绍了建筑材料放射性污染检测、控制的重要性及其危害。经研究表明：几乎所有的建筑材料都存在不同程度的放射性污染，超限量的放射性会对人体造成危害。同时，还介绍了建筑材料放射性定量控制的两个指标及其限量标准，着重阐述了建筑材料放射性的测量原理和典型测量方法，并对几年来的一些测量结果进行了分析，提出了要有选择性地使用建筑材料的观点。     

Use of multitracers for the study of water mixing in the Paraíba do Sul River estuary

Multitracers were used to study water mixing in the Paraíba do Sul River estuary region in August 2007 (dry season) and March 2008 (rainy season) and to evaluate the reach of the river plume in the direction of the open ocean. Two sampling campaigns were carried out, each in a different season. Based on these results, it was possible to conclude that the multitracers used in this study (salinity, Si, Ba and U, as well as the radium isotopes ²²³Ra, ²²⁴Ra, ²²⁶Ra and ²²⁸Ra) presented satisfactory results toward defining the plume reach and determining the residence time and water-mixing processes in the estuary. A strong correlation was observed between tracers and the distance to the coast. During the low river water discharge period, the riverine water took about 10 days to reach open ocean waters (salinity ∼ 35). During the rainy period this value decreased to 6 days. Based on the radium results, it was possible to calculate diffusion coefficients (K_h) of 23 km² d⁻¹ and 38 km² d⁻¹ for ²²⁴Ra and ²²³Ra, respectively, during the dry season (winter). Values of 65 km² d⁻¹ and 68 km² d⁻¹ for ²²³Ra and ²²⁴Ra, respectively, were found for the rainy period (summer).     

新疆大芸中铀,钍,镭,^9^0锶,^1^3^7铯的含量

对新疆中草药大芸中铀、钍、镭、~(90)锶、~(137)铯进行了含量测定,取得数据结果,并与浙江茶叶、宁夏枸杞子中五种核素含量进行了对比,提供有关部分参考。     

Natural radionuclide concentrations in two phosphate ores of east Algeria

Ore is considered as an important source of many elements such as the iron, phosphorus, and uranium. Concerning the natural radionuclides, their concentrations vary from an ore to other depending on the chemical composition of each site.In this work, two phosphate ores found in East of Algeria have been chosen to assess the activity concentration of natural radionuclides represented mainly by three natural radioactive series ²³⁸U, ²³⁵U and ²³²Th, and the primordial radionuclide ⁴⁰K where they were determined using ultra-low background, high-resolution gamma-ray spectroscopy.The measured activity concentrations of radioactive series ranged from 6.2 ± 0.4 to 733 ± 33 Bq.kg⁻¹ for the ²³²Th series, from 249 ± 16 to 547 ± 39 Bq.kg⁻¹ for the ²³⁸U series, around 24.2 ± 2.5 Bq.kg⁻¹ for the ²³⁵U series, and from 1.4 ± 0.2 to 6.7 ± 0.7 Bq.kg⁻¹ for ⁴⁰K.To assess exposure to gamma radiation in the two ores, from specific activities of ²³²Th, ⁴⁰K and ²²⁶Ra, three indexes were determined: Radium equivalent (Ra_eq), external and internal hazard indexes (H_ex and H_in), their values ranged from 831 ± 8 to 1298 ± 14 Bq.kg⁻¹ for Ra_eq, from 2.2 ± 0.4 to 3.5 ± 0.7 Bq.kg⁻¹ for H_ex, and from 4.2 ± 0.7 to 4.5 ± 0.7 Bq.kg⁻¹ for H_in.     

Measuring the radium quartet (Ra, Ra, Ra, Ra) in seawater samples using gamma spectrometry

Radium isotopes are widely used in marine studies (eg. to trace water masses, to quantify mixing processes or to study submarine groundwater discharge). While ²²⁸Ra and ²²⁶Ra are usually measured using gamma spectrometry, short-lived Ra isotopes (²²⁴Ra and ²²³Ra) are usually measured using a Radium Delayed Coincidence Counter (RaDeCC). Here we show that the four radium isotopes can be analyzed using gamma spectrometry. We report ²²⁶Ra, ²²⁸Ra, ²²⁴Ra, ²²³Ra activities measured using low-background gamma spectrometry in standard samples, in water samples collected in the vicinity of our laboratory (La Palme and Vaccarès lagoons, France) but also in seawater samples collected in the plume of the Amazon river, off French Guyana (AMANDES project). The ²²³Ra and ²²⁴Ra activities determined in these samples using gamma spectrometry were compared to the activities determined using RaDeCC. Activities determined using the two techniques are in good agreement. Uncertainties associated with the ²²⁴Ra activities are similar for the two techniques. RaDeCC is more sensitive for the detection of low ²²³Ra activities. Gamma spectrometry thus constitutes an alternate method for the determination of short-lived Ra isotopes.     

Determination of 226Ra and 228Ra in slightly mineralised natural waters

A radiochemical method for simultaneous separation of ²²⁶Ra and ²²⁸Ra from natural waters by precipitating the radionuclides in the form of chromates that have low solubility in weak acetic acid has been described. For analytical purposes the change into soluble state was achieved through high-temperature melting the radium chromates precipitate with sodium and potassium carbonates at certain ratios. The chemical yield for radium-226 amounted to 87.1 ± 1.4% at the efficiency of counting 92.8 ± 0.7%. Calculated in series of 20 parallel determinations, reproducibility of the method was 7%. The chemical yield in separating radium-228 made up 63.8 ± 1.1%.