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Influence of long-term aqueous leaching of irradiated graphite on surface properties and behavior of radionuclides

Published online by Cambridge University Press:  24 January 2020

Andrey A. Shiryaev*
Affiliation:
Institute of physical chemistry and electrochemistry RAS, Leninsky pr. 31, korp. 4, 119071, Moscow, Russia (shiryaev@phyche.ac.ru) Department of Chemistry, Lomonosov Moscow State University, Leninskie gory, 1 bld.3, Moscow, 119991, Russia Institute of geology of ore deposits, petrography, mineralogy and geochemistry RAS, Staromonetny per. 35, 119017, Moscow, Russia
Anna G. Volkova
Affiliation:
Institute of physical chemistry and electrochemistry RAS, Leninsky pr. 31, korp. 4, 119071, Moscow, Russia (shiryaev@phyche.ac.ru)
Stanislav Dvoryak
Affiliation:
Department of Chemistry, Lomonosov Moscow State University, Leninskie gory, 1 bld.3, Moscow, 119991, Russia
Maximillian S. Nickolsky
Affiliation:
Institute of physical chemistry and electrochemistry RAS, Leninsky pr. 31, korp. 4, 119071, Moscow, Russia (shiryaev@phyche.ac.ru) Institute of geology of ore deposits, petrography, mineralogy and geochemistry RAS, Staromonetny per. 35, 119017, Moscow, Russia
Elena V. Zakharova
Affiliation:
Institute of physical chemistry and electrochemistry RAS, Leninsky pr. 31, korp. 4, 119071, Moscow, Russia (shiryaev@phyche.ac.ru)
*
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Abstract

Samples of real irradiated (i-)graphite from bushings of RBMK reactor after several types of decontamination treatments were put in contact with aqueous solutions modelling underground water of Nizhnekansky massif (Russia) equilibrated with bentonite for periods up to 1.5 years. Leach rates of radionuclides and evolution of graphite surface morphology and oxidation state were monitored using nuclear spectroscopy, SEM and XPS. After the experiment, less than one third of surface carbons remains unoxidised. Extensive precipitation of secondary phases (alumosilicates, carbonates) was observed on some samples and is possibly correlated with surface oxidation extent. The leach rates of dose-forming 14C and 36Cl are comparable with the leach rates of radionuclides in glassy waste forms. According to the current study i-graphite could be regarded as a waste form, which is suitable for near-surface disposal.

Type
Articles
Copyright
Copyright © Materials Research Society 2020

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References

Volkova, A.G., Zakharova, E.V., Pavlyuk, A.O., and Shiryaev, A.A., Radionuclides in Irradiated Graphite of Uranium–Graphite Reactors: Liquid Decontamination of Bushings, Radiochemistry, 60(5), 558562 (2018).CrossRefGoogle Scholar
Volkova, A.G., Zakharova, E.V., Rodygina, N.I., Pavlyuk, A.O., and Shiryaev, A.A.Radionuclides in Irradiated Graphite of Uranium–Graphite Reactors: Decontamination by Thermochemical Methods, Radiochemistry, 60(6), 657-663 (2018).CrossRefGoogle Scholar
Dorofeev, А.N., Кomarov, Е.А., Zakharova, Е.V., Volkova, А.G., Мartynov, К.V., Linge, I.I., Ivanov, А.Yu., Utkin, S.S., Pavlyuk, А.О., Kotlyarevskij, S.G.. On reactor graphite disposal, Radioaktivnie othody (Radioactive waste), 2(7), 18-30 (2019). DOI: 10.25283/2587-9707-2019-2-18-30 (in Russian)CrossRefGoogle Scholar
Kochkin, B.T., Malkovskii, V.I., Yudintsev, S.V., Scientific basis of evaluation of safety of geological repositories of long-living radionuclides (Yenissey project). (Moscow, IGEM RAS, 2017) 384 p. (in Russian)Google Scholar
Beamson, G., Briggs D., D.High resolution XPS of organic polymers: The Scienta ESCA 300 database. Chichester: John Wiley & Sons, 1992. 295 p.Google Scholar
Shiryaev, A.A., Volkova, A.G., Zakharova, E.V., Nikolsky, M.S., Averin, A.A., Dolgopolova, E.A., and Yapaskurt, V.O., Radionuclides in Irradiated Graphite of Industrial Uranium–Graphite Reactors: Effect of Irradiation and Thermochemical Treatment on the Graphite Structure, Radiochemistry, 60(6), 664-671 (2018).CrossRefGoogle Scholar
Chernov, A.A.. in: Modern crystallography III. Crystal growth with contributions by Givargizov, E.I., Bagdasarov, K.S., Kuznetsov, V.A., Demianets, L.N., Lobachev, A.N.. (Springer‐Verlag Berlin, Heidelberg, New York, Tokyo 1984) 517 p.CrossRefGoogle Scholar
Vienna, J.D., Ryan, J.V., Gin, S., Inagaki, Y., Current understanding and remaining challenges in modeling long-term degradation of borosilicate nuclear waste glasses. Int.J. Appl. Glass Sci., 4, 283-294 (2013).CrossRefGoogle Scholar
Boukhvalov, D.W., Oxidation of a Graphite Surface: The Role of Water, J. Phys. Chem. C, 118, 2759427598 (2014).CrossRefGoogle Scholar
McDermott, L., Characterization and chemical treatment of irradiated UK graphite waste, PhD Thesis, Univ. of Manchester, 2011.Google Scholar
Nicaise, G.O., Poncet, B., A reverse method for the determination of the radiological inventory of irradiated graphite at reactor scale, Kerntechnik, 81(5), 565-570 (2016).CrossRefGoogle Scholar