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Size Distributions of Airborne Radionuclides from the Fukushima Nuclear Accident at Several Places in Europe

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† Nuclear Safety and Radioprotection Institute (IRSN), Laboratory for Continental and Marine Radioecological Studies (LERCM), BP 3 - 13115 St Paul lez Durance CEDEX, France
‡ Austrian Agency for Health and Food Safety (AGES), Wieningerstrasse 8, A-4020 Linz, Austria
§ National Radiation Protection Institute (SURO), Bartoskova 1450/28, 140 00 Prague, Czech Republic
∥ Institute of Applied Radiation Chemistry, Technical University of Lódz, ul. Zeromskiego 116, 90-924 Lódz, Poland
⊥ Environmental Radioactivity Laboratory, Institute of Nuclear & Radiological Sciences, Energy & Safety, N.C.S.R. ″Demokritos″, 15310 Aghia Paraskevi, Attiki, Greece
# Helmholtz Zentrum München (HMGU), Ingolstädter Landstr. 1, 85764 Neuherberg, Germany
Nuclear Safety and Radioprotection Institute (IRSN), Environmental Radioactivity Measurements Laboratory (LMRE), Bâtiment 501, le bois des Rames -91400 Orsay, France
△ Nuclear Safety and Radioprotection Institute (IRSN), Aerosol Physics and Metrology Laboratory (LPMA), BP 68 - 91192 Gif-sur-Yvette CEDEX, France
*Phone: +33-442-199-608; fax: +33-442-199-142; e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2013, 47, 19, 10995–11003
Publication Date (Web):September 3, 2013
https://doi.org/10.1021/es401973c
Copyright © 2013 American Chemical Society
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Abstract

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Segregation and radioactive analysis of aerosols according to their aerodynamic size were performed in France, Austria, the Czech Republic, Poland, Germany, and Greece after the arrival of contaminated air masses following the nuclear accident at the Fukushima Dai-ichi nuclear power plant in March 2011. On the whole and regardless of the location, the highest activity levels correspond either to the finest particle fraction or to the upper size class. Regarding anthropogenic radionuclides, the activity median aerodynamic diameter (AMAD) ranged between 0.25 and 0.71 μm for 137Cs, from 0.17 to 0.69 μm for 134Cs, and from 0.30 to 0.53 μm for 131I, thus in the “accumulation mode” of the ambient aerosol (0.1–1 μm). AMAD obtained for the naturally occurring radionuclides 7Be and 210Pb ranged from 0.20 to 0.53 μm and 0.29 to 0.52 μm, respectively. Regarding spatial variations, AMADs did not show large differences from place to place compared with what was observed concerning bulk airborne levels registered on the European scale. When air masses arrived in Europe, AMADs for 131I were about half those for cesium isotopes. Higher AMAD for cesium probably results from higher AMAD observed at the early stage of the accident in Japan. Lower AMAD for 131I can be explained by the adsorption of gaseous iodine on particles of all sizes met during transport, especially for small particles. Additionally, weathering conditions (rain) encountered during transport and in Europe in March and April contributed to the equilibrium of the gaseous to total 131I ratio. AMAD slightly increased with time for 131I whereas a clear decreasing trend was observed with the AMADs for 137Cs and 134Cs. On average, the associated geometric standard deviation (GSD) appeared to be higher for iodine than for cesium isotopes. These statements also bear out a gaseous 131I transfer on ambient particles of a broad size range during transport. Highest weighted activity levels were found on the 0.49–0.95 μm and on the 0.18–0.36 μm size ranges in France and in Poland, respectively. The contribution from resuspension of old deposited 137Cs was assessed for the coarse particle fractions only for the first sampling week.

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Two tables and one figure. Tables summarize theoretical cut-offs (μm) of equivalent aerodynamic diameter, according to the type of impactor and sampling conditions. The figure corresponds to the map of sampling locations. This material is available free of charge via the Internet at http://pubs.acs.org.

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