Phase and chemical stability of simulated waste forms Gd2Zr2-xCexO7(0≤ x≤ 2.0)

Lu Xi-Rui; Dong Fa-Qin; Hu Song; Wang Xiao-Li; Wu Yan-Lin

doi:10.7498/aps.61.152401

Abstract

In order to investigate phase change and chemical stability of pyrochlore Gd2Zr2O7 used for immobilizing Pu(Ⅳ), tetravalent cerium is used as the simulacrums for plutonium with tetravalence, and Gd2Zr2-xCexO7(0≤ x≤ 2.0) series samples are successfully synthesized by high temperature solid reaction and using Gd2O3 and ZrO2 powders as starting materials. The experiments of long-term chemical stability are conducted in synthetic seawater at 40 °C and 70 °C separately. The XRD diffractive data and extraction ratio of as-gained samples are collected by the help of X-ray diffraction (XRD) instrument and inductively coupled plasma mass spectrometry. The results indicate that the phases of compounds change from pyrochlore to fluorite-type phase when the value of x is more than 0.08. Extraction ratios of Gd3+, Zr4+ and Ce4+ in waste forms increase with the increase of immersion time in synthetic seawater. The extraction ratio of waste form at 70 °C is higher than at 40 °C. The highest extraction ratios of Gd3+, Zr4+ and Ce4+ for 42 days are no more than 0.032, 0.003 and 0.032 μg·ml-1 respectively.

Keywords:

Authors and contacts

1.
Institute of Nuclear Science and Technology, SU, Chengdu 610064, China;
2.
National Defense Key Discipline Lab of Nuclear Waste and Environmental Safety, SWUST, Mianyang 621010, China;
3.
Institute of Nuclear Physics and Chemistry, CAEP, Mianyang 621900, China;
4.
Graduate University for Advanced Studies, Hayama 240-0193, Japan
Funds: Project supported by the Key Project of National High Technology Research and Development Program (863Program) of China (Grant No. 2009AA050703), the Young Scientists Fund of National Natural Science Foundation of China (Grant No. 21007052), the Foundation of Key Laboratory of Radiation Physics and Technology (Sichuan University), Ministry of Education of China (Grant No. 2011-03), the Foundation of Key Subject Laboratory of National Defense for Radioactive Waste and Environmental Security (Southwest University of Science and Technology) (Grant No. 11zxnk09), and the Youth Foundation of Southwest University of Science and Technology (Grant No. 11zx3108).

References

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Cited By

[1]	Hatch L P 1953 American Scientist 41 410
[2]	Ringwood A E, Kesson S E, Ware N G, Hibberson W, Major A 1979 Nature 15 278
[3]	Clarke D R 1983 Annual Review of Materials Science 13 191
[4]	Robert L E J 1990 Annual Review of Nuclear and Particle Science 40 79
[5]	Donald I W, Metcalfe B L, Taylor R N J 1997 Journal of Materials Science 32 5851
[6]	Weber W J, Ewing R C, Angell C A, Arnold G W, Cormack A N, Delaye J M, Griscom D L, Hobbs L W, Navrotsky. A, Price D L, Stoneham A M, Weinberg M C 1997a Journal of Materials Research 12 1946
[7]	Weber W J, Ewing R C, Angell C A 1998 Journal of Materials Research 13 1434
[8]	Wang S X, Begg B D, Wang L M, Ewing R C, Weber W J, Govidan Kutty K V 1999 Journal of Materials Research 14 4470
[9]	Weber W J, Ewing R C 2000 Science 289 5487
[10]	Ewing R C, Weber W J, Lian J 2004 Journal of Applied Physics 95 5949
[11]	Lu X R, Cui C L, Zhang D, Chen M J, Yang Y K 2011 Acta Phys. Sin. 60 078901 (in chinese) [卢喜瑞, 崔春龙, 张东, 陈梦君, 杨岩凯 2011 60 078901]

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Vol. 61, Issue 15 - 2012-08-05

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