Determination of uranium isotopes in environmental samples by alpha-spectrometry

Abstract

A new and accurate method for the determination of uranium isotopes (238U, 234U and 235U) in environmental samples by alpha-spectrometry has been developed. Uranium is preconcentrated from filtered water samples by coprecipitation with iron(III) hydroxide at pH 9-10 using an ammonia solution and the precipitate is dissolved in HNO3 and mineralized with H2O2 and HF; uranium in biological samples is ashed at 600 °C, leached with Na2CO3 solution and mineralised with HNO3, HF and H2O2; uranium in soil samples is fused with Na2CO3 and Na2O2 at 600 °C and leached with HCl, HNO3 and HF. The mineralized or leaching solution in 2M HNO3 is passed through a Microthene-TOPO (tri-octyl-phosphine oxide) column; after washing, uranium is directly eluted into a cell with ammonium oxalate solution, electrodeposited on a stainless steel disk and measured by alpha-spectrometry. The lower limits of detection of the method is 0.37 Bq.kg-1 (soil) and 0.22 mBq.l-1 (water) for 238U and 234U and 0.038 Bq.kg-1 (soil) and 0.022 mBq.l-1 (water) for 235U if 0.5 g of soil and 1 litre of water are analyzed. Five reference materials supplied by the IAEA have been analyzed and reliable results are obtained. Sample analyses show that, the 238U, 234U and 235U concentrations are in the ranges of 0.30-103, 0.49-135 and 0.02-4.82 mBq.l-1 in waters, of 1.01-7.14, 0.85-7.69 and 0.04-0.32 Bq.kg-1 in mosses and lichens, and of 25.6-53.1, 26.4-53.8 and 1.18-2.48 Bq.kg-1 in sediments. The average uranium yields for waters, mosses, lichens and sediments are 74.5±9.0%, 80.5±8.3%, 77.8±4.9% and 89.4±9.7%, respectively.