Hostname: page-component-76fb5796d-zzh7m Total loading time: 0 Render date: 2024-04-25T16:25:27.838Z Has data issue: false hasContentIssue false

Identification and characterization of radioactive ‘hot’ particles in Chernobyl fallout-contaminated soils: the application of two novel approaches

Published online by Cambridge University Press:  05 July 2018

J. A. Entwistle
Affiliation:
Division of Geography and Environmental Management, Northumbria University, Lipman Building, Newcastle upon Tyne, Tyne and Wear NE1 8ST, UK
A. G. Flowers
Affiliation:
School of Life Sciences, Kingston University, Penrhyn Road, Kingston upon Thames, Surrey KT1 2EE, UK
G. Nageldinger
Affiliation:
School of Life Sciences, Kingston University, Penrhyn Road, Kingston upon Thames, Surrey KT1 2EE, UK
J. C. Greenwood
Affiliation:
NERC ICP Facility, Kingston University, Penrhyn Road, Kingston upon Thames, Surrey KT1 2EE, UK

Abstract

The Chernobyl accident in 1986 resulted in the widespread identification of the post-accident presence of radioactive (or ‘hot’) particles across large areas of Eastern and Central Europe. Such particles arise from direct deposition and also from condensation and interactions on particle surfaces during and following the deposition of soluble fallout. Identification of the presence and nature of hot particles is necessary in order to determine the long-term ecological impact of radioactive fallout. This paper describes several techniques for the identification and characterization of hot particles in soil samples from Belarus. In addition to new results from the use of gamma spectrometry, we include two novel instrumentation approaches that have been developed and applied to Chernobyl fallout-contaminated soils. The first, ‘differential’ autoradiography, utilizes a photographic film sandwich to characterize the nature of the ionizing radiation emitted from samples. In this paper we show that differential autoradiography can not only identify hot particle presence in soil, but can also determine the dominant radionuclide in that particle. The second approach, sector field ICP-MS (ICP-SFMS), can provide rapid, high-precision determination of the actinides, including the transuranic actinides, that characteristically occur in hot particles originating from weapons fallout or fuel matrices. Here, ICP-SFMS is shown to yield sufficiently low detection limits for plutonium isotopes (with the exception of 238Pu) to enable us to confirm negligible presence of plutonium in areas outside the Chernobyl exclusion zone, but with high levels of fission-product contamination.

Type
Research Article
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2003

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

Adams, C.E., Farlow, N.H. and Shell, W.R. (1960) The composition structures and origins of radioactive fallout particles. Geochemica et Cosmochemica Acta, 18, 4256.CrossRefGoogle Scholar
Alloway, B.J. (1995) Heavy Metals in Soils, 2nd edition. Blackie, London.CrossRefGoogle Scholar
Begichev, S.N., Borovi, A.A., Burlakov, E.V., Gagrinsky, A.Ju., Demin, V.F., Khodakovsky, I.L. and Khrulev, A.A. (1989) Radioactive releases due to the Chernobyl accident. Presented at the International Seminar on Fission Product Transport Processes in Reactor Accidents, 2226 May, 1989, Dubrovnik, Yugoslavia.Google Scholar
Begichev, S.N., Borovoj, A.A., Burlakov, E.B., Gararinsky, A.J., Denim, V.F., Khrulev, A.A. and Khodakovsky, I.L. (1990) Radioactive releases due to the Chernobyl accident. Pp. 717734 in: Fission Product Transport Processes in Reactor Accidents (Rogers, J.T., editor). Hemisphere Publishing, USA.Google Scholar
Belli, M. and Tikhomirov, F., editors (1996) Experimental Collaboration Project Number 5. European Community, Brussels.Google Scholar
Bienvenu, P.G., Brochard, E.A. and Excoffier, E.A. (1998) Determination of long-lived beta emitters in nuclear waste by inductively coupled plasma-mass spectrometry. Pp. 5163 in: Applications of Inductively Coupled Plasma-Mass Spectrometry to Radionuclide Determination (Morrow, R.W. and Crain, J.S, editors). ASTM, Pennsylvania, USACrossRefGoogle Scholar
Bogatov, S., Borovoj, A., Dubasov, Yu. and Lomonosov, V. (1990) Forms and characteristics of hot particles of fuel at the Chernobyl NPP accident. Atomnaya Energiya, 69, 3640.Google Scholar
Bolsunovsky, A.Ya. and Tcherkezian, V.O. (2001) Hot particles of the Yenisei River flood plain, Russia. Journal of Environmental Radioactivity, 57, 167174.CrossRefGoogle ScholarPubMed
Bondarenko, O.A., Salmon, P.L., Henshaw, D.L., Fews, A.P. and Ross, A.N. (1996) Alpha-particle spectroscopy with Tastrak (CR-39) type plastic, and its application to the measurement of hot particles. Nuclear Instruments and Methods in Physics Research A, 369, 582587.CrossRefGoogle Scholar
Boulya, S.F., Erdmann, N., Funk, H., Kievets, K., Lomonosova, E.M., Mansel, A., Trautmann, N., Yaroshevich, O.I. and Zhuk, I.V. (1997) Determination of isotopic composition of Pu in hot particles of the Chernobyl area. Radiation Measurements, 28, 349352.CrossRefGoogle Scholar
Boulyga, S.F., Testa, C., Desideri, D. and Becker, S.J. (2001) Optimisation and application of ICP-MS and alpha-spectrometry for determination of isotopic ratios of depleted uranium and plutonium in samples collected in Kosovo. Journal of Analytical Atomic Spectrometry, 16, 12831289.CrossRefGoogle Scholar
Broda, R., Kubica, B., Szeglowski, Z. and Zuber, K. (1989) Alpha emitters in Chernobyl hot particles. Radiochimica Acta, 48, 8996.CrossRefGoogle Scholar
Bunzl, K. (1997) Probability for detecting hot particles in environmental samples by sample splitting. Analyst, 122, 653656.CrossRefGoogle ScholarPubMed
Bunzl, K. (1998) Detection of radioactive hot particles in environmental samples by repeated mixing. Applied Radiation Isotopes, 49, 16251631.CrossRefGoogle Scholar
Charles, M.W. (1991) The hot particle problem. Radiation Protection Dosimetry, 39, 3947.CrossRefGoogle Scholar
Chevchuka, V.E. and Gurachevsky, V.L. (2001) 15 Years After the Chernobyl Accident. State Committee on Post-Chernobyl Problems, Republic of Belarus, Minsk.Google Scholar
Edvarson, K., Low, K. and Sisefsky, J. (1959) Fractionation phenomena in nuclear weapons debris. Nature, 184, 17711774.CrossRefGoogle Scholar
Hoygle, Z. and Maly, M. (2000) Sources, vertical distribution, and migration rates of 239,240Pu, 238Pu, and 137Cs in grassland soil in three localities of central Bohemia. Journal of Environmental Radioactivity, 47, 135147.Google Scholar
Jakubowski, N., Moens, L. and Vanhaecke, F. (1998) Sector field mass spectrometers in ICP-MS. Spectrochimica Acta, 53, 17391763.CrossRefGoogle Scholar
Kirchner, G. and Noack, C.C. (1988) Core history and nuclide inventory of the Chernobyl core at the time of the accident. Nuclear Safety, 29, 15.Google Scholar
Koide, M., Bertine, K.K., Chow, T.J. and Goldberg, E.D. (1985) The Pu-240 Pu-239 ratio, a potential geochronometer. Earth and Planetary Science Letters, 72, 18CrossRefGoogle Scholar
Krouglov, S.V., Filipas, A.S., Alexakhin, R.M. and Arkhipov, M.N.P. (1997) Long-term study on the transfer of 137Cs and 90Sr from Chernobyl- contaminated soils to grain crops. Journal of Environmental Radioactivity, 34, 267286.CrossRefGoogle Scholar
Larsen, I.L., Lee, S.Y., Boston, H.L. and Stetar, E.A., (1992) Discovery of a 137Cs hot particle in municipal wastewater treatment sludge. Health Physics, 62, 235238.CrossRefGoogle ScholarPubMed
Longworth, G., Carpenter, B., Bull, R., Toole, J. and Nichols, A. (1998) The Radiochemical Manual. AEA Technology Plc, Oxford, UK.Google Scholar
Mamuro, T., Fujita, A. and Matsunami T. (1965) Microscopic examination of highly radioactive fallout particles from the first Chinese nuclear test explosion. Health Physics, 11, 10971101.Google ScholarPubMed
Mandjoukov, I.G., Burin, K., Mandjoukova, B., Vapirev, E.I. and Tsacheva, T. (1992) Spectrometry and visualization of ‘standard’ hot particles from the Chernobyl accident. Radiation Protection Dosimetry, 40, 235244.CrossRefGoogle Scholar
Morrow, R.W. and Crain, J.S., editors (1998) Applications of Inductively Coupled Plasma-Mass Spectrometry to Radionuclide Determinations. ASTM, USA.CrossRefGoogle Scholar
Nageldinger, G. (1998) Characterisation of Chernobyl fallout in Belarus soil. Ph.D. thesis, Kingston University, Surrey, UK.Google Scholar
Nageldinger, G., Flowers, A., Schwerdt, C. and Kelz, R. (1998a)) Autoradiographic film evaluated with desktop scanner. Nuclear Instruments and Methods in Physics Research A, 416, 516524.CrossRefGoogle Scholar
Nageldinger, G., Flowers, A., Henry, B. and Postaul, J. (1998b)) Hot particle detection using uncertainties in activity measurements of soil. Health Physics, 74, 472477.CrossRefGoogle Scholar
Nageldinger, G., Flowers, A. and Entwistle, A. (1999) A new mechanism for hot particle development in soil following ionic contamination with radiocesium. Health Physics, 75, 646647.CrossRefGoogle Scholar
Organisation for Economic Cooperation and Development (OECD) (1995) The Radiological and Health Impact of Chernobyl. OECD Nuclear Energy Agency, USA.Google Scholar
Osuch, S., Dabrowska, M., Jaracz, P., Kaczanowski, J., Van Khoi, L., Mirowski, S., Piasecki, E., Szeflinska, Z., Tropilo, J. and Wilhelmi, Z. (1989) Isotopic composition of high-activity particles released in the Chernobyl accident. Health Physics, 57, 707716.CrossRefGoogle ScholarPubMed
Philipsborn, H. and Steinhaeusler, F. (1988) Hot particles from the Chernobyl fallout. Proceedings of an International Workshop held in Theuern , 2829 October, 1987.Google Scholar
Pollanen, R. and Torvonen, H. (1994a) Skin doses from large uranium fuel particles — application to the Chernobyl accident. Radiation Protection Dosimetry, 54, 127132.Google Scholar
Pollanen, R. and Toivonen, H. (1994b) Transport of large uranium fuel particles released from a nuclear power plant in a severe accident. Journal of Radiological Protection, 14, 5565.CrossRefGoogle Scholar
Pollanen, R., Valkama, I. and Toivonen, H. (1997) Transport of radioactive particles from the Chernobyl accident. Atmospheric Environment, 31, 35753590.CrossRefGoogle Scholar
Powers, D.A., Kress, T.S. and Jankowski, M.W. (1987) The Chernobyl source term. Nuclear Safety, 28, 1028.Google Scholar
Rodushkin, I., Linahl, P., Holm, E. and Roos, P. (1999) Determination of plutonium concentrations and isotope ratios in environmental samples with a double-focusing sector field ICP-MS. Nuclear Instruments and Methods in Physics Research A, 423, 472479.CrossRefGoogle Scholar
Salbu, B. (2000) Source-related characteristics of radioactive particles: a review. Radiation Protection Dosimetry, 92, 4954.CrossRefGoogle Scholar
Sandalls, F.J., Segal, M.G. and Victorova, N. (1993) Hot particles from Chernobyl: a review. Journal of Environmental Radioactivity , 18, 522.CrossRefGoogle Scholar
Sanzharova, N.I., Fensenko, S.V., Kotik, V.A. and Spiridonov, S.I. (1996) Behaviour of radionuclides in meadows and efficiency of countermeasures. Radiation Protection Dosimetry, 64, 4348.CrossRefGoogle Scholar
Sich, A.R. (1993) The Chernobyl accident revisited: source term analysis and reconstruction of events during the active phase. Ph.D. thesis, Massachusetts Institute of Technology, USA.Google Scholar
Taylor, R.N., Warneke, T., Milton, A., Croudace, I.W., Warick, P.E. and Nesbitt, R.W. (2001) Plutonium isotope ratio analysis at femtogram to nanogram levels by multicollector ICP—MS. Journal of Analytical Atomic Spectrometry, 16, 279284.CrossRefGoogle Scholar
Tcherkezian, V., Shkinev, V., Khitro, L. and Kolesov, G. (1994) Experimental approach to Chernobyl hot particles. Journal of Environmental Radioactivity, 22, 127139.CrossRefGoogle Scholar
Truscott, J.B., Jones, P., Fairman, B.E. and Evans, E.H. (2001) Determination of actinide elements at femtogram per gram levels in environmental samples by on-line solid phase extraction and sector field inductively coupled plasma-mass spectrometry. Analytica Chimica Acta, 433, 245253.CrossRefGoogle Scholar
UNSCEAR (1982) Ionising Radiation and Biological Effects. United Nations, New York, USA.Google Scholar
U.S. Environmental Protection Agency (1997) Establishment of cleanup levels for CERCLA sites with radioactive contamination. OSWER 9200, United States Environmental Protection Agency, Washington D.C.Google Scholar
Victorova, N.V. and Garger, E.K. (1990) Investigations of the deposition and spread of radioactive aerosol particles in the Chernobyl zone based on biological monitoring. Pp. 223236 in: Proceedings Report EUR 13574. Commission of the European Communities, Luxembourg.Google Scholar
Wood, J.L., Benke, R.R., Rohrer, S.M. and Kearfott, K.J. (1999) A comparison of minimum detectable and proposed maximum allowable soil concentration clean-up levels for selected radionuclides. Health Physics, 76, 413417.CrossRefGoogle Scholar
Zheltonozhsky, V., Muck, K. and Bondarkov, M. (2001) Classification of hot particles from the Chernobyl accident and nuclear weapons detonations by non- destructive methods. Journal of Environmental Radioactivity, 57, 151166.CrossRefGoogle ScholarPubMed