M. Srncik

Uranium extraction from aqueous solutions by ionic liquids.

For determining natural levels of (236)U with its environmental abundance of 10(-16)% rather large sample volumes (approximately 30L) are necessary, therefore the conventional radiochemical uranium analysis (pre-concentration and column chromatography) is very time consuming. To speed up the procedure hydrophobic ionic liquids (ILs) were evaluated as a potential extraction agent for uranium from aqueous solutions. High selectivity and efficiency for uranium compared to calcium and magnesium in natural water was achieved with tricaprylmethylammonium thiosalicylate, [A336][TS]. Uranium was stripped successfully from the investigated ILs with 2M HNO(3).

The first use of 236U in the general environment and near a shutdown nuclear power plant

We present a first effort to investigate (236)U in the environment near a shutdown nuclear power plant far away from highly contaminated sites, by using accelerator mass spectrometry. The detection limit of about 1pg (236)U allowed us to identify a minimal increase of the (236)U/(238)U isotopic ratio correlated to a peak of (137)Cs in river sediments downstream of the nuclear power plant, and to detect anthropogenic (236)U also upstream, where it is probably not related to the power plant but to global fallout. The (236)U content shoved variations of the (236)U/(238)U isotopic ratio in relation to the chemical-physical characteristics of the sediments. This demonstrates the potential of (236)U as an environmental tracer, and as an indicator for releases from nuclear facilities.

236U/238U and 240Pu/239Pu isotopic ratios in small (2 L) sea and river water samples.

Accelerator Mass Spectrometry (AMS) and alpha spectrometry were used to determine uranium ((236)U, (238)U, (234)U) and plutonium isotopes ((239)Pu, (240)Pu) in sea and river water samples. Plutonium was separated by Dowex(®) 1 × 8 resin and UTEVA(®) resin was used for uranium purification. The measured (236)U/(238)U isotopic ratios for surface water from the Atlantic Ocean, the Pacific Ocean and the Black Sea were in the order of 10(-9), while values for river water were in the order of 10(-8). These contaminations may be attributed to global fallout. A sample of the reference material IAEA-443, collected from the Irish Sea, showed, in accordance to the reference value, a ratio that was 10(3) times higher due to effluents from the reprocessing plant at Sellafield. These results underline the good suitability of (236)U/(238)U as a tracer for hydrology and oceanography, and show that relatively small water samples are sufficient for the determination of (236)U by AMS, which is not the case for plutonium with present techniques. The plutonium concentrations in our water samples could only be measured with large uncertainties and were in the order of 10(-3) mBq/L (with the exception of the Irish Sea sample).

Depth profile of 236U/238U in soil samples in La Palma, Canary Islands

The vertical distribution of the 236U/238U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the 240Pu/239Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios 236U/238U, 240Pu/239Pu and 236U/239Pu, respectively. The 236U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio 240Pu/239Pu indicated a global fallout signature we assume the same origin as the probable source for 236U. Our measured 236U/239Pu value of around 0.2 is within the expected range for this contamination source.

Determination of U, Pu and Am isotopes in Irish Sea sediment by a combination of AMS and radiometric methods

Samples from a marine sediment core from the Irish Sea (54.416 N, 3.563 W) were analyzed for the isotopic composition of uranium, plutonium and americium by a combination of radiometric methods and AMS. The radiochemical procedure consisted of a Pu separation step by anion exchange, subsequent U separation by extraction chromatography using UTEVA® and finally Am separation with TRU® Resin. Additionally to radiometric determination of these isotopes by alpha spectrometry, the separated samples were also used for the determination of (236)U/(238)U and plutonium isotope ratios by Accelerator Mass Spectrometry (AMS) at the VERA facility.