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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.
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Keywords:
- pyrochlore Gd2Zr2O7 /
- waste forms /
- phase /
- chemical stability
[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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[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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