Hostname: page-component-76fb5796d-x4r87 Total loading time: 0 Render date: 2024-04-25T18:07:13.332Z Has data issue: false hasContentIssue false
  • English
  • Français

A comparison of radiation effects in crystalline ABO4-type phosphates and silicates

Published online by Cambridge University Press:  05 July 2018

A. Meldrum ,
L. A. Boatner  and
R. C. Ewing
A. Meldrum*
Affiliation:
Solid State Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
L. A. Boatner
Affiliation:
Solid State Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
R. C. Ewing
Affiliation:
The University of Michigan, Dept. of NE&RS, Ann Arbor, MI 49108, USA
*
*E-mail: ameldrum@gpu.srv.ualberta.ca
Get access Rights & Permissions [Opens in a new window]

Abstract

The effects of ion irradiation in the ABO4-type compounds were compared by performing experiments on four materials that include the most common crystal structures (monazite vs. zircon) and chemical compositions (phosphates vs. silicates) for these phases. Pure synthetic single crystals of ZrSiO4, monoclinic ThSiO4, LaPO4 and ScPO4 were irradiated using 800 keV Kr+ ions. Radiation damage accumulation was monitored as a function of temperature in situ in a transmission electron microscope. The activation energies for recrystallization during irradiation were calculated to be 3.1–3.3 eV for the orthosilicates but only 1.0–1.5 eV for the isostructural orthophosphates. For the ion-beam-irradiated samples, the critical temperature, above which the recrystallization processes are faster than damage accumulation and amorphization cannot be induced, is >700°C for ZrSiO4 but it is only 35°C for LaPO4. At temperatures above 600°C, zircon decomposed during irradiation into its component oxides (i.e. crystalline ZrO2 plus amorphous SiO2). The data are evaluated with respect to the proposed use of the orthophosphates and orthosilicates as host materials for the stabilization and disposal of high-level nuclear waste. The results show that zircon with 10 wt.% Pu would have to be maintained at temperatures in excess of 300°C in order to prevent it from becoming completely amorphous. In contrast, a similar analysis for the orthophosphates implies that monazite-based waste forms would not become amorphous or undergo a phase decomposition.

Keywords

zirconmonazitemetamictizationamorphizationradiation effectsplutoniumwaste form
Type
Research Article
Information
Mineralogical Magazine , Volume 64 , Issue 2 , April 2000 , pp. 185 - 194
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2000

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

Footnotes

†

Present address: Department of Physics, The University of Alberta, Edmonton, Alberta, Canada T6G 2J1

References

Boatner, L.A. (1978) Letter to the US Department of Energy, Of. ce of Basic Energy Sciences, Division of Materials Science on 28 April detailing the possible uses of monazite as an alternative to borosilicate glass. Google Scholar
Boatner, L.A. and Sales, B.C. (1988) Monazite. Pp. 495–564 in: Radioactive Waste Forms for the Future (Lutze, W. and Ewing, R.C., editors). Elsevier, Amsterdam.Google Scholar
Boatner, L.A., Beall, G.W., Abraham, M.M., Finch, C.B., Huray, P.G. and Rappaz, M. (1980) Monazite and other lanthanide orthophosphates as alternate actinide waste forms. Pp. 289–96 in: Scientific Basis for Nuclear Waste Management, 2. (Northrup, C.J., editor). Plenum Press, New York.CrossRefGoogle Scholar
Boatner, L.A., Abraham, M.M. and Rappaz, M. (1981) The characterization of nuclear waste forms by EPR spectroscopy. Pp. 181–8 in: Scientific Basis for Nuclear Waste Management, 3 (Moore, J.G., editor). Plenum Press, New York.CrossRefGoogle Scholar
Burakov, B.E., Anderson, E.B., Rovsha, V.S., Ushakov, S.V., Ewing, R.C., Lutze, W. and Weber, W.J. (1996) Synthesis of zircon for immobilization of actinides. Pp. 33–40 in: Scientific Basis for Nuclear Waste Management XIX (Murphy, W.M. and Knecht, D.A., editors). Materials Research Society, Pittsburgh, PA.Google Scholar
Ewing, R.C., Haaker, R.F. and Lutze, W. (1982) Leachability of zircon as a function of alpha dose. Mater. Res. Soc. Symp. Proc., 11, 389–96.CrossRefGoogle Scholar
Ewing, R.C., Lutze, W. and Weber, W.J. (1995) Zircon: a host phase for the disposal of weapons plutonium. J. Mater. Res., 10, 243–6.CrossRefGoogle Scholar
Ewing, R.C., Weber, W.J. and Lutze, W. (1996) Waste forms for the disposal of weapons plutonium. Pp. 65–83 in: Disposal of Ex-Weapons Plutonium as Waste (Merz, E.R. and Walter, C.E., editors). NATO ASI Series, Kluwer Academic Publishers, Dordrecht, The Netherlands.CrossRefGoogle Scholar
Gramaccioli, C.M. and Segalstad, T.V. (1978) A uranium- and thorium-rich monazite from a southalpine pegmatite at Piona, Italy. Amer. Mineral., 63, 757–61.Google Scholar
Hazen, R.M. and Finger, L.W. (1979) Crystal structure and compressibility of zircon at high pressure. Amer. Mineral., 64, 196–201.Google Scholar
Helean, K., Lutze, W. and Ewing, R.C. (1999) The dissolution rate of chemically durable materials: zircon. Pp. 297–304 in: Environmental Issues and Waste Management Technologies IV (Marra, J.C. and Chandler, G.T., editors). American Ceramic Society, Westerville, OH.Google Scholar
McCarthy, G.J., Pepin, J.G. and Davis, D.D. (1980) Crystal chemistry and phase relations in the synthetic minerals of ceramic ware forms: I. Fluorite and monazite structures. Pp. 297–306 in: Scientific Basis for Nuclear Waste Management, 2 (Northrup, C.J., editor). Plenum Press, New York.CrossRefGoogle Scholar
Meldrum, A., Boatner, L.A. and Ewing, R.C. (1997 a) Electron irradiation-induced nucleation and growth in amorphous orthophosphates and zircon. J. Mater. Res., 12, 1816–27.CrossRefGoogle Scholar
Meldrum, A., Boatner, L.A., Wang, L.M. and Ewing, R.C. (1997 b) Displacive irradiation effects in the monazite- and zircon-structure orthophosphates (La- LuPO4). Phys. Rev., B56, 13805–14.Google Scholar
Meldrum, A., Zinkle, S.J., Boatner, L.A. and Ewing, R.C. (1998 a) A transient liquid-like state in the displacement cascades of zircon, hafnon and thorite. Nature, 395, 56–8.CrossRefGoogle Scholar
Meldrum, A., Boatner, L.A., Weber, W.J. and Ewing, R.C. (1998 b) Radiation damage in zircon and monazite. Geochim. Cosmochim. Acta, 62, 2509–20.CrossRefGoogle Scholar
Meldrum, A., Zinkle, S.J., Boatner, L.A. and Ewing, R.C. (1999 a) Amorphization, recrystallization and phase decomposition in the ABO4 orthosilicates. Phys. Rev. B, 59, 3981–92.CrossRefGoogle Scholar
Meldrum, A., Boatner, L.A., Zinkle, S.J., Wang, S.X., Wang, L.M. and Ewing, R.C. (1999 b) Effects of dose rate and temperature on the crystalline-to-metamict transformation in the ABO4 orthosilicates. Canad. Mineral., 37, 207–22.Google Scholar
Miller, M.L. and Ewing, R.C. (1992) Image simulation of partially amorphous materials. Ultramicroscopy, 48, 203–37.CrossRefGoogle Scholar
Milligan, W.O., Mullica, D.F., Beall, G.W. and Boatner, L.A. (1982) Structural investigations of YPO4, ScPO4, and LuPO4 . Inorg. Chim. Acta, 60, 39–43.CrossRefGoogle Scholar
Milligan, W.O., Mullica, D.F., Beall, G.W. and Boatner, L.A. (1983) Structures of ErPO4, TmPO4 and YbPO4 . Acta Crystallogr., C39, 23–34.Google Scholar
Mullica, D.F., Milligan, W.O., Grossie, D.A., Beall, G.W. and Boatner, L.A. (1984) Ninefold coordination in LaPO4: Pentagonal interpenetrating tetrahedral polyhedron. Inorg. Chim. Acta, 95, 231–6.CrossRefGoogle Scholar
Mullica, D.F., Grossie, D.A. and Boatner, L.A. (1985) Structural refinements of praseodymium and neodymium orthophosphate. J. Sol. State Chem., 58, 71–7.CrossRefGoogle Scholar
Reynolds, R.W., Boatner, L.A., Finch, C.B., Châtelain, A. and Abraham, M.M. (1972) EPR investigations of Er3+, Yb2+ and Gd3+ in zircon-structure silicates. J. Chem. Phys., 56, 5607–25.CrossRefGoogle Scholar
Robinson, M.T. (1983) Computer simulation of collision cascades in monazite. Phys. Rev. B, 27, 5347–59.CrossRefGoogle Scholar
Speer, J.A. (1982) Zircon. Pp. 67–112 in: Orthosilicates (Ribbe, P.H., editor). Reviews in Mineralogy, 5. Mineralogical Society of America, Washington D.C. CrossRefGoogle Scholar
Taylor, M. and Ewing, R.C. (1978) The crystal structure of the ThSiO4 polymorphs: huttonite and thorite. Acta Crystallogr., B34, 1074–9.CrossRefGoogle Scholar
Tole, M.P. (1985) The kinetics of dissolution of zircon. Geochim. Cosmochim. Acta, 49, 453–8.CrossRefGoogle Scholar
Wang, L.M. (1998) Application of advanced electron microscopy techniques to the studies of radiation effects in ceramic materials. Nucl. Instr. Meth. Phys. Res., B141, 312–25.CrossRefGoogle Scholar
Vance, E.R. and Anderson, B.W. (1972) Study of metamict Ceylon zircons. Mineral. Mag., 38, 605.CrossRefGoogle Scholar
Virk, H.S. (1995) Single activation energy model of radiation damage in solid state nucelar track detectors. Radiation Effects and Defects in Solids, 133, 87–95.CrossRefGoogle Scholar
Weber, W.J. (1990) Radiation-induced defects and amorphization in zircon. J. Mater. Res., 5, 2687–97.CrossRefGoogle Scholar
Weber, W.J. (2000) Models and mechanisms of irradiation-induced amorphization in ceramics. Nucl. Instr. Meth. Phys Rev.(in press).Google Scholar
Weber, W.J., Ewing, R.C. and Wang, L.M. (1994) The radiation-induced crystalline-to-amorphous transition in zircon. J. Mater. Res., 9, 688–98.CrossRefGoogle Scholar
Weber, W.J., Ewing, R.C. and Lutze, W. (1996) Performance assessment of zircon as a waste form for excess weapons plutonium under deep borehole burial conditions. Mater. Res. Soc. Symp. Proc., 412, 25–32.CrossRefGoogle Scholar
Weber, W.J., Ewing, R.C., Catlow, C.R.A., Diaz de la Rubia, T., Hobbs, L.W., Kinoshita, C., Matzke, Hj., Motta, A.T., Nastasi, M.A., Salje, E.H.K., Vance, E.R. and Zinkle, S.J. (1998) Radiation effects in crystalline ceramics for the immobilization of high-level nuclear waste and plutonium. J. Mater. Res., 13, 1434–84.CrossRefGoogle Scholar
Zinkle, S.J. and Kinoshita, C. (1997) Defect production in ceramics. J. Nucl. Mater., 251 200–17.CrossRefGoogle Scholar