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Determination of 234U/238U isotope ratios in environmental waters by quadrupole ICP-MS after U stripping from alpha-spectrometry counting sources
Authors:José Luis Mas  Renli Ma  Cameron McLeod  Jesús González-Labajo  Alan Cox  Paul Watson
Affiliation:(1) Departamento de Física Aplicada I, Universidad de Sevilla, Escuela Universitaria Politécnica, Virgen de Africa, 7, 21071 Sevilla, Spain;(2) School of Applied Sciences, Northumbria University, A313 Ellison Building, Newcastle upon Tyne, NE1 8ST, UK;(3) Department of Analytical Chemistry, University of Sheffield, Dainton Building, Brookhill, Sheffield, S3 7HF, UK;(4) Elemental Scientific, Inc., 2440 Cunning Street, Omaha, NE 68131, USA
Abstract:The 234U/238U isotope ratio has been widely used as a tracer for geochemical processes in underground aquifers. Quadrupole-based inductively coupled plasma mass spectrometry (ICP-MS) equipped with a high-efficiency nebulizer and a membrane desolvator was employed for the determination of 234U/238U isotope ratios in natural water samples. The instrumental limit of detection for 234U was at the low pg L−1 level with very low sample consumption. Measurement precision (234U/238U) was 3–5% for bottled mineral water with elevated uranium concentration (>1 μg L−1). For the analysis of groundwater samples from the Almonte-Marisma underground aquifer (Huelva, Spain), uranium was stripped from stainless steel planchets that had previously been used as radiometric counting sources for alpha-particle spectrometry. Potential spectral interferences from other metals introduced during the dissolution were investigated. Matrix-matched blank solutions were needed to subtract the background on 234U due to the formation of platinum argides, and to allow for mass bias correction and background correction. The Pt appears to be an impurity present in the stainless steel, either as a minor component by itself or after extraction from the anode and a subsequent uranium electrodeposition. The 234U/238U isotope ratio data were in very good agreement with those of alpha spectrometry, while precision was improved by a factor of up to 10 and counting time was reduced down to ~20 min (10 replicate measurements).
Keywords:Mass spectrometry/ICP-MS  Water  Radiochemical methods  Isotope ratio
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