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Self-Irradiation of Monazite Ceramics: Contrasting Behavior of PuPO4 and (La,Pu)PO4 Doped with Pu-238

Published online by Cambridge University Press:  17 March 2011

Boris E. Burakov ,
Maria A. Yagovkina ,
Vladimir M. Garbuzov ,
Alexander A. Kitsay  and
Vladimir A. Zirlin
Boris E. Burakov
Affiliation:
Laboratory of Applied Mineralogy and Radiogeochemistry, the V.G. Khlopin Radium Institute, 28, 2-nd Murinskiy ave., St. Petersburg, 194021, Russia, e-mail:, burakov@peterlink.ru
Maria A. Yagovkina
Affiliation:
Laboratory of Applied Mineralogy and Radiogeochemistry, the V.G. Khlopin Radium Institute, 28, 2-nd Murinskiy ave., St. Petersburg, 194021, Russia, e-mail:, burakov@peterlink.ru
Vladimir M. Garbuzov
Affiliation:
Laboratory of Applied Mineralogy and Radiogeochemistry, the V.G. Khlopin Radium Institute, 28, 2-nd Murinskiy ave., St. Petersburg, 194021, Russia, e-mail:, burakov@peterlink.ru
Alexander A. Kitsay
Affiliation:
Laboratory of Applied Mineralogy and Radiogeochemistry, the V.G. Khlopin Radium Institute, 28, 2-nd Murinskiy ave., St. Petersburg, 194021, Russia, e-mail:, burakov@peterlink.ru
Vladimir A. Zirlin
Affiliation:
Laboratory of Applied Mineralogy and Radiogeochemistry, the V.G. Khlopin Radium Institute, 28, 2-nd Murinskiy ave., St. Petersburg, 194021, Russia, e-mail:, burakov@peterlink.ru
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Abstract

To investigate the behavior of monazite during accelerated radiation damage, which simulates effects of long term storage, 238Pu-doped polycrystalline samples of (La,Pu)PO4 and PuPO4 were synthesized for the first time ever and studied using powder X-ray diffraction (XRD) analysis and optical microscopy. The starting precursor materials were obtained by precipitation of La and (or) Pu from their aqueous nitrate solutions followed by calcination in air at 700°C for 1 hour, cold pressing, and sintering in air at 1200-1250°C for 2 hours. The 238Pu contents in ceramic samples measured using gamma spectrometry were (in wt.% el.): 8.1 for (La,Pu)PO4 and 7.2 for PuPO4. The (La,Pu)PO4 monazite remained crystalline at ambient temperature up to a cumulative dose of 1.19 × 1025 alpha decays/m3. In contrast, the PuPO4 monazite became nearly completely amorphous at a relatively low dose of 4.2 × 1024 alpha decays/m3. Swelling and crack formation due to the alpha decay damage was observed in the PuPO4 ceramic. Also, under self-irradiation this sample completely changed color from initial deep blue to black. The (La,Pu)PO4 monazite was characterized by a similar change in color from initial light blue to gray, however, no swelling or crack formation have so far been observed. The results of this study allow us to conclude that the radiation damage behavior of monazite strictly depends on the chemical composition. The justification of monazite-based ceramics as actinide waste forms requires additional investigation.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 824: Symposium CC – Scientific Basis for Nuclear Waste Management XXVIII , 2004 , CC4.1
Copyright
Copyright © Materials Research Society 2004

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