J. M. López-Gutiérrez

Iodine-129: Sample preparation, quality control and analyses of pre-nuclear materials and of natural waters from Lower Saxony, Germany

Sample preparation procedures for AMS measurements of 129I and 127I in environmental materials and some methodological aspects of quality assurance are discussed. Measurements from analyses of some pre-nuclear soil and thyroid gland samples and of a systematic investigation of natural waters in Lower Saxony, Germany, are described. Although the up-to-now lowest 129I/127I ratios in soils and thyroid glands were observed, they are still suspect to contamination since they are significantly higher than the pre-nuclear equilibrium ratio in the marine hydrosphere. A survey on all available 129I/127I isotopic ratios in precipitation shows a dramatic increase until the middle of the 1980s and a stabilization since 1987 at high isotopic ratios of about (3.6–8.3)×10−7. In surface waters, ratios of (57–380)×10−10 are measured while shallow ground waters show with ratios of (1.3–200)×10−10 significantly lower values with a much larger spread. The data for 129I in soils and in precipitation are used to estimate pre-nuclear and modern 129I deposition densities.

On the origin of 129I in rain water near Zürich

129I concentrations in precipitation at Dübendorf/Zürich, Switzerland, have been determined with monthly resolution for almost three years in the mid 1990s. The results confirm that annual mean 129I concentrations in precipitation in central Europe have remained about constant since the late 1980s. Liquid and gaseous emissions from the nuclear fuel reprocessing plants at Sellafield and La Hague are discussed as the only possible sources of 129I in precipitation in central Europe. Based on an upper limit estimate for iodine transferred from the sea to the atmosphere, the gaseous discharges constitute the potentially bigger 129I reservoir for precipitation. Moreover, the time dependence of the annual gaseous 129I releases from Sellafield and La Hague correlates much better with the 129I concentrations in precipitation in central Europe since the late 1980s than does the time dependence of the liquid emissions from these sites. At monthly resolution, the 129I concentrations in the precipitation samples close to Zürich exhibit a large variability. A meteorological transport analysis was carried out for four selected months with particularly low or high observed 129I concentrations. It was found that meteorological transport alone, based upon assimilated wind fields and observed precipitation values, can not directly account for the large month-to-month variability.

Wet and dry deposition of 129I in Seville (Spain) measured by accelerator mass spectrometry.

Iodine-129 (T1/2 = 1.57 x 10(7) yr) concentrations have been determined by accelerator mass spectrometry in rainwater samples taken at Seville (southwestern Spain) in 1996 and 1997. This technique allows a reduction in the detection limits for this radionuclide in comparison to radiometric counting and other mass spectrometric methods such as ICP-MS. Typical 129I concentrations range from 4.7 x 10(7) 129I atoms/l (19.2%) to 4.97 x 10(9) 129I atoms/l (5.9%), while 129I depositions are normally in the order of 10(8)-10(10) atoms/m2d. These values agree well with other results obtained for recent rainwater samples collected in Europe. Apart from these, the relationship between 129I deposition and some atmospheric factors has been analyzed, showing the importance of the precipitation rate and the concentration of suspended matter in it.

Determination of 129I in atmospheric samples by accelerator mass spectrometry

A method for the radiochemical extraction of 129I from atmospheric charcoal filters and its measurement by accelerator mass spectrometry is presented. Either the 129I concentration or the 129I/127I atom ratio can be determined in the sample. With this method, air filters from Seville, in the Southwest of Spain (37.4 degrees N, 6 degrees W) have been analyzed. Sensitivities in the order of 10(4) atoms/m3 for 129I concentrations and 10(-10) for 129I/127I atom ratios are obtained. AMS measurements are performed with the 6 MV tandem accelerator at the ETH-Hönggerberg in Zurich.

129I measurements on the 1MV AMS facility at the Centro Nacional de Aceleradores (CNA, Spain)

The AMS system at CNA has been the first 1MV compact AMS system designed and manufactured by HVE. In this paper we present the experimental set-up for (129)I measurements in this facility. Charge state +3 has been selected at high-energy side and an optimum stripper pressure of 6×10(-3)mbar of argon (mass thickness of about 0.15μgcm(-2)) has been reached to obtain lowest blank values ((129)I/(127)I≅3×10(-13)). The measurements of the reference materials provided by the IAEA have demonstrated the viability of this facility to make routine measurements of (129)I at environmental levels. This blank value obtained is enough for the measurement of most environmental samples and comparable with other reported backgrounds obtained in facilities working at higher energies and higher charge states.

Accelerator mass spectrometry as a powerful tool for the determination of 129I in rainwater

129I is a very long-lived radionuclide (T(1/2) = 15.7 x 10(6) years) that is present in the environment both because of natural and anthropogenic sources. Its environmental interest, for example, as a tracer of geological processes, makes it the research target of a growing scientific community. However, its detection in environmental samples by radiometric methods is very difficult because of its long half-life. In this work, we present the methodology developed for its detection by Accelerator Mass Spectrometry (AMS) in rainwater.

The behaviour of 129I released from nuclear fuel reprocessing factories in the North Atlantic Ocean and transport to the Arctic assessed from numerical modelling

A quantitative evaluation of the fate of (129)I, released from the European reprocessing plants of Sellafield (UK) and La Hague (France), has been made by means of a Lagrangian dispersion model. Transport of radionuclides to the Arctic Ocean has been determined. Thus, 5.1 and 16.6 TBq of (129)I have been introduced in the Arctic from Sellafield and La Hague respectively from 1966 to 2012. These figures represent, respectively, 48% and 55% of the cumulative discharge to that time. Inventories in the North Atlantic, including shelf seas, are 4.4 and 13.8 TBq coming from Sellafield and La Hague respectively. These figures are significantly different from previous estimations based on field data. The distribution of these inventories among several shelf seas and regions has been evaluated as well. Mean ages of tracers have been finally obtained, making use of the age-averaging hypothesis. It has been found that mean ages for Sellafield releases are about 3.5 year larger than for La Hague releases.

129I/127I ratios and 129I concentrations in a recent sea sediment core and in rainwater from Sevilla (Spain) by AMS

In spite of the environmental relevance of 129I, there is still a scarcity of data about its presence in the different natural compartments. In this work, results are presented on the concentration of 129I in rainwater samples taken in Sevilla (southwestern Spain) and in a sediment core taken near the Ringhals coast (Sweden). Typical concentrations of 108 and 109129I at/l are found in rainwater samples, similar to other values in literature. In the case of the sediment core, our results clearly show the impact of anthropogenic sources, with concentrations in the order of 1013129I at./kg and isotopic ratios 129I/127I in the order of 10−8 in the higher layers.

Iodine-129 microdosing for protein and peptide drug development: erythropoietin as a case study

BACKGROUND Microdosing is a technique for studying the behavior of compounds in vivo at 1/100th of the dose of a test substance calculated, based on animal data, to yield a pharmacologic effect. In microdosing, use is made of accelerator MS (AMS). In this study, we investigated whether (129)I-labeling of proteins with subsequent AMS measurements is a suitable method to perform microdose studies with therapeutic proteins. We used erythropoietin (EPO) as a case study. RESULTS In an animal study with (129)I-labeled EPO in Han-Wistar rats, an increase of (129)I-EPO is observed after dose administration. The half-life was found to be 2 and 5.5 h for two different EPOs. These results are in accordance with expected values. CONCLUSION Although further research is required, (129)I-labeling of proteins seems a feasible method for AMS microdose studies with peptide and protein drugs, such as biosimilars.

Influence of releases of 129I and 137Cs from European reprocessing facilities in Fucus vesiculosus and seawater from the Kattegat and Skagerrak areas

(129)I is a very long-lived radionuclide (T1/2=15.7×10(6) years) that is present in the environment because of natural and anthropogenic sources. Compared to the pre-nuclear era, large amounts of (129)I have been released to the marine environment, especially as liquid and gaseous discharges from two European reprocessing facilities located at Sellafield (England) and La Hague (France). The marine environment, i.e., the oceans, is the major source of iodine. Brown seaweed accumulates iodine at high levels up to 1.0% of dry weigh, and therefore they are ideal bioindicators for studying levels of (129)I. In this work, (129)I concentrations have been determined in seaweed Fucus vesiculosus and seawater collected in the Kattegat and Skagerrak areas in July 2007. The resulting data were evaluated in terms of (129)I concentrations and (129)I/(137)Cs ratios. (129)I concentrations were found to be in the order of (44-575)×10(9) atoms g(-1) in seaweed and (5.4-51)×10(9) atoms g(-1) in seawater, with an enhancement in the Skagerrak area in comparison to the Kattegat area. Iodine-129 concentrations in both seaweed and seawater were used to determine the concentration factor of iodine in brown seaweed F. vesiculosus. The high levels of (129)I and (129)I/(137)Cs ratios in the Skagerrak area and their gradually decreasing trend to the Kattegat indicates that the most important contribution to the (129)I inventory in those areas comes from Sellafield and La Hague reprocessing plants.