Abstract
In the search for novel ceramics for use within nuclear fuel–related applications and nuclear waste-form matrices, a major focus has been on the development of radiation-tolerant materials. Of particular interest in this field have been numerous compounds with either pyrochlore or the related fluorite-type structures. In this study, we look to expand the family of compounds with defect fluorite–type structure. We have fabricated three new compounds; Yb2Sn1.125O5.25, Yb2Sn1.25O5.5, and Yb2Sn1.375O5.75. The compound Yb2Sn1.125O5.25 was determined, via x-ray diffraction, to have the long-range defect fluorite structure, Fm-3 m symmetry, with cell parameter a = 5.17233(1). Further to this, Sm2ZrO5 and Yb2TiO5 compounds were also fabricated and crystal structures characterised. The use of transmission electron microscopy has revealed a much more complex crystal structure than that of the relatively high symmetry fluorite, with the presence of structural modulations being detected. The ion-irradiation response of these compounds was tested via bulk specimen irradiation using 15-MeV gold ions with grazing incidence x-ray diffraction characterisation. The results show that both Sm2ZrO5 and Yb2Sn1.25O5.5 are highly tolerant to ion-irradiation exposure whilst Yb2TiO5 is susceptible to amorphisation.
Similar content being viewed by others
References
Uberuaga, B.P., et al.: Opposite correlations between cation disordering and amorphization resistance in spinels versus pyrochlores. Nat. Commun. 6(1), 8750 (2015)
Lumpkin, G.R., et al.: Nature of the chemical bond and prediction of radiation tolerance in pyrochlore and defect fluorite compounds. J. Solid State Chem. 180(4), 1512–1518 (2007)
Sickafus, K.E., et al.: Radiation-induced amorphization resistance and radiation tolerance in structurally related oxides. Nat. Mater. 6(3), 217–223 (2007)
Van Dijk, M., K. De Vries, A.J.S.S.I: Burggraaf, Oxygen ion and mixed conductivity in compounds with the fluorite and pyrochlore structure. 9: 913–919 (1983)
Lian, J., et al: Nanoscale manipulation of pyrochlore: new nanocomposite ionic conductors. 87(14), 145901 (2001)
Subramanian, M., G. Aravamudan, G.S.J.P.i.S.S.C. Rao: Oxide pyrochlores—a review. 15(2), 55–143 (1983)
Andrievskaya, E.: Phase equilibria in the refractory oxide systems of zirconia, hafnia and yttria with rare-earth oxides. J. Eur. Ceram. Soc. 28(12), 2363–2388 (2008)
Aughterson, R. D., G.R.L., Zhang, Z., Avdeev, M., Kong, L: Crystal chemistry and ion-irradiation resistance of Ln2ZrO5 compounds with Ln = Sm, Eu, Gd and Tb. Manuscript submitted for publication (2021)
Risovany, V., Varlashova, E., Suslov, D.: Dysprosium titanate as an absorber material for control rods. J. Nucl. Mater. 281(1), 84–89 (2000)
Aughterson, R.D., N.J. Zaluzec, G.R. Lumpkin, Synthesis and ion-irradiation tolerance of the Dy2TiO5 polymorphs. Acta Materialia, 204, 116518 (2021)
Aughterson, R.D., et al.: The influence of crystal structure on ion-irradiation tolerance in the Sm(x)Yb(2–x)TiO5 series. J. Nucl. Mater. 471, 17–24 (2016)
Aughterson, R.D., et al.: Ion-irradiation resistance of the orthorhombic Ln2TiO5 (Ln = La, Pr, Nd, Sm, Eu, Gd, Tb and Dy) series. J. Nucl. Mat 467(2), 683–691 (2015)
Zhang, J., et al.: Ion-irradiation-induced structural transitions in orthorhombic Ln2TiO5. Acta Mater. 61(11), 4191–4199 (2013)
Tracy, C.L., Liang, M., Zhang, J., Zhang, F., Wang, Z., Ewing, R.C.: Structural response of A2TiO5 (A=La, Nd, Sm, Gd) to swift heavy ion irradiation. Acta Mater. 60(11), 4477–4486 (2012)
Whittle, K.R., et al.: Ion irradiation of novel yttrium/ytterbium-based pyrochlores: The effect of disorder. Acta Mater. 59(20), 7530–7537 (2011)
Whittle, K.R., et al.: Ion-beam irradiation of lanthanum compounds in the systems La2O3–Al2O3 and La2O3–TiO2. J. Solid State Chem. 183(10), 2416–2420 (2010)
Pramudita, J.C., et al: Using in situ synchrotron x-ray diffraction to study lithium-and sodium-ion batteries: a case study with an unconventional battery electrode (Gd2TiO5). J. Mat. Res, 1–9 (2014)
Pan, T.M., Lin, C.W.: High-kappa Dy2TiO5 Electrolyte-Insulator-Semiconductor Urea Biosensors. J. Electrochem. Soc. 158(4), J100–J105 (2011)
Kao, C.H., Chen, H.A., Lin, S.P.: The comparison of the high-k Sm2O3 and Sm2TiO5 dielectrics deposited on the polycrystalline silicon. Electrochem Solid State Lett 14(2), G9–G12 (2011)
Pan, T.M., et al.: A urea biosensor based on pH-sensitive Sm2TiO5 electrolyte-insulator-semiconductor. Anal. Chim. Acta 669(1–2), 68–74 (2010)
Shepelev, Y.F., Petrova, M.A.: Crystal structures of Ln(2)TiO(5) (Ln = Gd, Dy) polymorphs. Inorg. Mater. 44(12), 1354–1361 (2008)
Lau, G.C., et al.: Stuffed rare earth pyrochlore solid solutions. J. Solid State Chem. 179(10), 3126–3135 (2006)
Aughterson, R.D., et al.: The ion-irradiation tolerance of the pyrochlore to fluorite Ho(x)Yb(2–x)TiO5 and Er2TiO5 compounds: a TEM comparative study using both in-situ and bulk ex-situ irradiation approaches. J. Nucl. Mater. 507, 316–326 (2018)
Aughterson, R.D., et al.: The crystal structures and corresponding ion-irradiation response for the Tb(x)Yb(2–x)TiO5 series. Ceram. Int. 44(1), 511–519 (2018)
Lau, G.C., et al.: Long- and short-range order in stuffed titanate pyrochlores. J. Solid State Chem. 181(1), 45–50 (2008)
Withers, R., Thompson, J., Barlow, P.: An electron, and X-ray powder, diffraction study of cubic, fluorite-related phases in various ZrO2 Ln2O3 systems. J. Solid State Chem. 94(1), 89–105 (1991)
Tabira, Y., et al: The strain-driven pyrochlore to “defect fluorite” phase transition in rare earth sesquioxide stabilized cubic zirconias. 159(1), 121–129 (2001)
Kennedy, B.J., Hunter, B.A., Howard, C.J.J.J.o.S.S.C: Structural and bonding trends in tin pyrochlore oxides. 130(1), 58–65 (1997)
Newman, R., Aughterson, R.D., Lumpkin, G.R.: Synthesis and Structure of Novel A2BO5 Compounds Containing A = Y, Yb, Gd, Sm, and La and B = Zr, Ti, and Sn. MRS Advances 3(20), 1117–1122 (2018)
Lian, J., et al: Radiation-induced amorphization of rare-earth titanate pyrochlores. Phys. Rev. B. 68(13), 134107 (2003)
Park, S., et al.: Swift-heavy ion irradiation response and annealing behavior of A2TiO5 (A= Nd, Gd, and Yb). J. Solid State Chem. 258, 108–116 (2018)
Shamblin, J., et al.: Structural response of titanate pyrochlores to swift heavy ion irradiation. Acta Mater. 117, 207–215 (2016)
Wang, S.X., et al.: Radiation stability of gadolinium zirconate: a waste form for plutonium disposition. J. Mater. Res. 14(12), 4470–4473 (1999)
Begg, B., et al.: Heavy-ion irradiation effects in Gd2 (Ti2− xZrx) O7 pyrochlores. J. Nucl. Mater. 289(1–2), 188–193 (2001)
Lian, J., et al.: Ion-beam irradiation of Gd2Sn2O7 and Gd2Hf2O7 pyrochlore: Bond-type effect. J. Mater. Res. 19(5), 1575–1580 (2004)
Lian, J., et al.: Ion beam irradiation in La2Zr2O7–Ce2Zr2O7 pyrochlore. Nucl. Instrum. Methods Phys. Res., Sect. B 218, 236–243 (2004)
Cliff, G., Lorimer, G.W.: The quantitative analysis of thin specimens. J. Microsc. 103(2), 203–207 (1975)
Hunter, B: Rietica - A Visual Rietveld Program. International Union of Crystallography Commission on Powder Diffraction. Newsletter number 20 (Summer) (1998)
Fink, D., et al.: The ANTARES AMS facility at ANSTO. Nucl. Instrum. Methods Phys. Res., Sect. B 223–224, 109–115 (2004)
Ziegler, J. F., Ziegler, J.P.B., M. D., SRIM The Stopping and Range of Ions in Matter. www.SRIM.org (2008)
Lumpkin, G.R., et al.: Ion irradiation of ternary pyrochlore oxides. Chem. Mater. 21(13), 2746–2754 (2009)
Stoller, R.E., et al.: On the use of SRIM for computing radiation damage exposure. Nucl. Instrum. Methods Phys. Res., Sect. B 310, 75–80 (2013)
Aughterson, R.D., et al.: Crystal structures of orthorhombic, hexagonal, and cubic compounds of the Sm(x)Yb(2–x)TiO5 series. J. Solid State Chem. 213, 182–192 (2014)
Rouanet, A.: Zirconium dioxide—Lanthanide oxide systems close to the melting point. Rev. Int. Hautes Temp. Refract 8(2), 161–180 (1971)
Shannon, R.D.: Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Crystallogr. A 32, 751–767 (1976)
Mitchell, M.R., et al: 119 Sn MAS NMR and first-principles calculations for the investigation of disorder in stannate pyrochlores. 13(2), 488–497 (2011)
de los Reyes, M., et al: The pyrochlore to defect fluorite phase transition in Y 2 Sn 2− x Zr x O 7. RSC Advances. 3(15), 5090–5099 (2013)
Le Bail, A.: Whole powder pattern decomposition methods and applications: A retrospection. Powder Diffr. 20(4), 316–326 (2005)
Whittle, K.R., et al.: Lanthanum pyrochlores and the effect of yttrium addition in the systems La2−xYxZr2O7 and La2−xYxHf2O7. J. Solid State Chem. 182(3), 442–450 (2009)
Degen, T., et al: The highscore suite. 29(S2), S13-S18 (2014)
Lian, J., et al.: Effect of structure and thermodynamic stability on the response of lanthanide stannate-pyrochlores to ion beam irradiation. J. Phys. Chem. B 110(5), 2343–2350 (2006)
Tracy, C.L., et al: Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation. Phys. Rev. B. 94(6), 064102 (2016)
Sickafus, K.E., et al.: Radiation tolerance of complex oxides. Science 289(5480), 748–751 (2000)
Naguib, H., Kelly, R.: Criteria for bombardment-induced structural changes in non-metallic solids. Radiat. Eff. 25(1), 1–12 (1975)
Trachenko, K.: Understanding resistance to amorphization by radiation damage. J. Phys. Condensed Matt 16(49), R1491–R1515 (2004)
Wang, S.X., et al.: Ion irradiation of rare-earth- and yttrium-titanate-pyrochlores. Nucl. Instrum. Methods. Phys. Res. Sect. B-Beam Interact. Mat. Atoms 169, 135–140 (2000)
Lumpkin, G., et al: Radiation Tolerance of A2Ti2O7 Compounds at the Cubicmonoclinic Boundary, in Pacific Basin Nuclear Conference (15th : 2006 : Sydney, Australia). 2006, Australian Nuclear Association: Sydney, N.S.W. p. [703]-[709]
Acknowledgements
The authors wish to thank Tim Palmer, NMDC, metallography, ANSTO, for his SEM specimen preparation.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Aughterson, R.D., Newman, R., Ionescu, M. et al. The ion irradiation tolerance of the fluorite RE2MO5 (RE = Sm, and Yb, M = Ti, Zr, and Sn) system. J Aust Ceram Soc 58, 287–298 (2022). https://doi.org/10.1007/s41779-021-00689-9
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s41779-021-00689-9