Synthesis of Actinide-Doped Ceramics: from Laboratory Experiments to Industrial Scale Technology

2003 ◽  
Vol 807 ◽  
Author(s):  
Alexander A. Kitsay ◽  
Vladimir M. Garbuzov ◽  
Boris E. Burakov

ABSTRACTThe experience of the Laboratory of Applied Mineralogy and Radiogeochemistry of the V.G.Khlopin Radium Institute on synthesis of Pu-Am-doped ceramics is summarized. During the last 5 years, dozens of actinide doped polycrystalline samples and single crystals have been successfully synthesized such as zircon, hafnon, cubic zirconia, monazite, Ti-pyrochlore, perovskite and garnet. Actinide loading has been varied as follows:-239Pu - from 5–6 wt.% in zircon (polycrystalline and single crystals), hafnon, garnet and perovskite to 10 wt.% in Ti-pyrochlore and up to 37 wt.% in zirconia;- 238Pu - from 2.5 wt.% in zircon single crystals to 5 wt. % in polycrystalline zircon and 10 wt.% in monazite and cubic zirconia;- 243Am - 20–23 wt.% in cubic zirconia and monazite.The weight of each single ceramic pellet varied from 0.2 to 2.0 grams. Special furnaces developed in KRI for ceramic synthesis allowed obtaining up to 7 ceramic pellets simultaneously during the same experiment. The highest amounts of actinides used under glove-box conditions in the same experiment were: 1.5–2.0 g for 239Pu, 0.6 g for 238Pu and 0.3 g for 243Am. Most experiments on synthesis of ceramics and single crystals doped with 239Pu, 238Pu and 243Am carried out at the KRI did not lead to contamination of internal walls of glove boxes. No release of Pu-Am-aerosols was observed as a result of sintering or melting at 1300–1600°C. These results allowed us to conclude that at the present the KRI has developed the experimental basis for transferring laboratory innovations to the industry of actinide immobilization. It is important that adopting ceramic synthesis methods at industrial scale does not require development of new special equipment.

2008 ◽  
Vol 1107 ◽  
Author(s):  
Boris E. Burakov ◽  
Maria A. Yagovkina ◽  
Maria V. Zamoryanskaya ◽  
Vladimir M. Garbuzov ◽  
Vladimir A. Zirlin ◽  
...  

AbstractTo investigate the resistance of actinide host phases to accelerated radiation damage, which simulates radiation induced effects of long term storage, the following samples doped with plutonium-238 (from 2 to 10 wt. %) have been repeatedly studied using XRD and other methods: cubic zirconia, Zr0.79Gd0.14Pu0.07O1.99; monazite, (La,Pu)PO4; ceramic based on Pu-phosphate of monazite structure, PuPO4; ceramic based on zircon, (Zr,Pu)SiO4, and minor phase tetragonal zirconia, (Zr,Pu)O2; single crystal zircon, (Zr,Pu)SiO4; single crystal monazite, (Eu,Pu)PO4; ceramic based on Ti-pyrochlore, (Ca,Gd,Hf,Pu,U)2Ti2O7. No change of phase composition, matrix swelling, or cracking in cubic zirconia were observed after cumulative dose 2.77×1025 alpha decay/m3. The La-monazite remained crystalline at cumulative dose 1.19×1025 alpha decay/m3, although Pu-phosphate of monazite structure became nearly amorphous at relatively low dose 4.2×1024 alpha decay/m3. Zircon has lost crystalline structures under self-irradiation at dose (1.3-1.5)×1025 alpha decay/m3, however, amorphous zircon characterized with high chemical durability. The Ti-pyrochlore after cumulative dose (1.1-1.3)×1025 alpha decay/m3 became amorphous and lost chemical durability. Radiation damage caused crack formation in zircon single crystals but not in the matrix of polycrystalline zircon. Essential swelling and crack formation as a result of radiation damage were observed in ceramics based on Ti-pyrochlore and Pu-phosphate of monazite structure, but not so far in La-monazite doped with 238Pu.


Author(s):  
B. Burakov ◽  
V. Gribova ◽  
A. Kitsay ◽  
M. Ojovan ◽  
N. C. Hyatt ◽  
...  

Methods for the synthesis of ceramic wasteforms for the immobilization of actinides are common to those for non-radioactive ceramics: hot uniaxial pressing (HUP); hot isostatic pressing (HIP); cold pressing followed by sintering; melting (for some specific ceramics, such as garnet/perovskite composites). Synthesis of ceramics doped with radionuclides is characterized with some important considerations: all the radionuclides should be incorporated into crystalline structure of durable host-phases in the form of solid solutions and no separate phases of radionuclides should be present in the matrix of final ceramic wasteform; all procedures of starting precursor preparation and ceramic synthesis should follow safety requirements of nuclear industry. Synthesis methods that avoid the use of very high temperatures and pressures and are easily accomplished within the environment of a glove-box or hot cell are preferable. Knowledge transfer between the V. G. Khlopin Radium Institute (KRI, Russia) and Immobilisation Science Laboratory (ISL, UK) was facilitated in the framework of a joint project supported by UK Royal Society. In order to introduce methods of precursor preparation and ceramic synthesis we selected well-known procedures readily deployable in radiochemical processing plants. We accounted that training should include main types of ceramic wasteforms which are currently discussed for industrial applications.


1995 ◽  
Vol 72 (1) ◽  
pp. 59-80 ◽  
Author(s):  
B. Ya. Farber ◽  
A. S. Chiarelli ◽  
A. H. Heuer

2000 ◽  
Vol 20 (12) ◽  
pp. 2069-2077 ◽  
Author(s):  
M. Kilo ◽  
G. Borchardt ◽  
B. Lesage ◽  
O. Kaı̈tasov ◽  
S. Weber ◽  
...  

1997 ◽  
Vol 233 (1-2) ◽  
pp. 75-87 ◽  
Author(s):  
D. Baither ◽  
B. Baufeld ◽  
U. Messerschmidt ◽  
M. Bartsch

1998 ◽  
Vol 166 (1) ◽  
pp. 127-153 ◽  
Author(s):  
B. Baufeld ◽  
D. Baither ◽  
M. Bartsch ◽  
U. Messerschmidt

2016 ◽  
Vol 55 (3) ◽  
pp. 031305 ◽  
Author(s):  
Stephan Haringer ◽  
Armando Giannattasio ◽  
Hans Christian Alt ◽  
Roberto Scala

1998 ◽  
Vol 166 (1) ◽  
pp. 115-126 ◽  
Author(s):  
B.Ya. Farber ◽  
B.Ya. Farber ◽  
V. I. Orlov ◽  
V. I. Orlov ◽  
A. H. Heuer

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