Hostname: page-component-586b7cd67f-vdxz6 Total loading time: 0 Render date: 2024-11-26T05:01:23.714Z Has data issue: false hasContentIssue false
  • English
  • Français

Advanced Experimental Technique for Radiation Damage Effects in Nuclear Waste Forms: Neutron Total Scattering Analysis

Published online by Cambridge University Press:  19 February 2018

Maik Lang ,
Eric C. O’Quinn ,
Jacob Shamblin  and
Jörg Neuefeind
Maik Lang*
Affiliation:
Department of Nuclear Engineering, University of Tennessee, Knoxville, TN, USA
Eric C. O’Quinn
Affiliation:
Department of Nuclear Engineering, University of Tennessee, Knoxville, TN, USA
Jacob Shamblin
Affiliation:
Department of Nuclear Engineering, University of Tennessee, Knoxville, TN, USA Department of Physics and Astronomy, University of Tennessee, Knoxville, TN, USA
Jörg Neuefeind
Affiliation:
Chemical and Engineering Materials Division, Spallation Neutron Source, Oak Ridge National Laboratory, Oak Ridge, TN, USA
*
*(Email: [email protected])
Get access

Abstract

For the past 30 years, the development of durable materials for radionuclide immobilization has been driven by efforts to dispose of wastes generated by the nuclear fuel cycle [National Research Council, ‘Waste Forms Technology and Performance: Final Report’, the National Academies Press, Washington D.C., 2011]. Many materials have been developed, but there still exist large gaps in the knowledge of fundamental modes of waste form degradation in repository environments. An important aspect of waste form science is the behavior of the materials under intense irradiation from decaying actinides and fission products. This irradiation induces a wide range of defects and disorder, the details of which depend on the specific waste form material. At the present time, it is not fully explained how radiation effects will influence the performance of nuclear waste forms and their long-term retention of fission products and actinides under operational conditions. The complex defect behavior and radiation damage must be understood over a range of length scales, from the initial atomic-scale defect structure to the long-range observable material modification. This is particularly challenging and requires advanced characterization techniques. This contribution describes how pair distribution function (PDF) analysis obtained from neutron total scattering experiments can be applied in the research field of waste form science to uniquely characterize radiation effects in a wide range of materials, including crystalline complex oxides and waste glasses. Neutron scattering strength does not have an explicit Z-dependence; this allows access to many low-Z elements, such as oxygen, that cannot be accurately studied with X-rays. In many cases, this can permit a detailed analysis of both cation (often high-Z) and anion (often low-Z) defect behavior. In contrast to traditional crystallography, which relies on long-range order, PDF analysis probes the local defect structure, including changes in site occupation, coordination, and bond distance. This is particularly important when characterizing aperiodic waste glasses with no long-range order at all. In contrast to X-ray characterization which requires very little sample mass (∼0.1 mg), neutron characterization (even at state-of-the-art spallation facilities) requires relatively large sample mass (∼50 - 100 mg). Obtaining this quantity is challenging for studies of irradiated materials, but by tailoring our experimental approach to use high-energy ions (GeV) with very high penetration depth, we are able to produce the required mass.

Keywords

nuclear materialsneutron scatteringwaste management
Type
Articles
Information
MRS Advances , Volume 3 , Issue 31: Energy and Sustainability , 2018 , pp. 1735 - 1747
Copyright
Copyright © Materials Research Society 2018 

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.)

References

REFERENCES

Weber, W.J. and Ewing, R.C., Science, 289, 2051–2052 (2000)Google Scholar
Ewing, R.C., Weber, W.J., and Lian, J., J. Appl. Phys. 95, 5949–5971 (2004)Google Scholar
Subramanian, M.A., Aravamudan, G., and Rao, G.V.S., Prog. Solid State Chem. 15, 55–143 (1983)Google Scholar
Sickafus, K.E., Minervini, L., Grimes, R.W., Valdez, J.A., Ishimaru, M., Li, F., McClellan, K.J., and Hartmann, T., Science 289, 748–751 (2009)Google Scholar
Sickafus, K.E., Grimes, R.W., Valdez, J.A., Cleave, A., Tang, M., Ishimaru, M., Corish, S.M., Stanek, C.R., and Uberuaga, B.P., Nature Materials 6, 217–223 (2007)Google Scholar
Naguib, H.M. and Kelly, R., Radiat. Eff. 25, 1–12 (1975)Google Scholar
Trachenko, K., Pruneda, J.M., Artacho, E., and Dove, M.T., Phys. Rev. B 71, 184104 (2005)Google Scholar
Lian, J., Helean, K.B., Kennedy, B.J., Wang, L.M., Navrotsky, A., and Ewing, R.C., J. Phys. Chem. B 110, 2343–2350 (2006)Google Scholar
Sattonnay, G., Sellami, N., Thome, L., Legros, C., Grygiel, C., Monnet, I., Jagielski, J., Jozwik-Biala, I., and Simon, P., Acta Mater. 61, 6492–6505 (2013)Google Scholar
Tracy, C.L., Shamblin, J., Park, S., Zhang, F.X., Trautmann, C., Lang, M., and Ewing, R.C., Phys. Rev. B 94, 064102 (2016)Google Scholar
Shamblin, J., Tracy, C.L., Ewing, R.C., Zhang, F.X., Li, W.X., Trautmann, C., and Lang, M., Acta Materialia 117, 207–215 (2016)Google Scholar
Kaoumi, D., Weber, W.J., Hattar, K., and Ribis, J., Journal of Materials Research Focus Issue 30(9), (2015)Google Scholar
Zhang, F.X., Lang, M., Liu, Z.X., and Ewing, R.C., Phys. Rev. Lett. 105, 15503 (2010)Google Scholar
Egami, T. and Billinge, S.J.L., Underneath the Bragg-Peaks: Structural Analysis of Complex Materials, 1st ed. (Elsevier Science B.V., Amsterdam, 2002)Google Scholar
Zhang, J.M., Lang, M., Toulemonde, M., Devanathan, R., Ewing, R.C., and Weber, W.J., J. Mater. Res. 25, 1344 (2010)Google Scholar
Lang, M., Zhang, F.X., Ewing, R.C., Lian, J., Trautmann, C., and Wang, Z.W., J. Mater. Res. 24, 1322–1334 (2009)Google Scholar
Chung, C.K., Shamblin, J., O’Quinn, E., Shelyug, A., Gussev, I., Lang, M., and Navrotsky, A., Acta Mater. (in press) 2018Google Scholar
Neuefeind, J., Feygenson, M., Carruth, J., Hoffmann, R., and Chipley, K.K., Nucl. Instrum. Meth. Physic Res. B 287, 68–75 (2012)Google Scholar
Rodríguez-Carvajal, J., Abstracts of the Satellite Meeting on Powder Diffraction of the XV Congress of the IUCr, (Toulouse, 1990) p. 127Google Scholar
Larson, A.C. and Von Dreele, R.B., Los Alamos National Laboratory Report LAUR 748, 86–748 (2004)Google Scholar
Petkov, V., Materials Today, 11, 28–38 (2008)Google Scholar
Farrow, C.L., Juhas, P., Liu, J.W., Bryndin, D., Bozin, E.S., Bloch, J., Proffen, T., and Billinge, S.J.L., J. Phys. Condens. Matter 19, (2007)Google Scholar
Tucker, M.G., Dove, M.T., Keen, D.A., Trachenko, K., J. Phys.: Condens. Matter 17, 67–75 (2005)Google Scholar
Ziegler, J.F., Ziegler, M.D., and Biersack, J.P., Nucl. Instrum. Methods Phys. Res. B 268, 1818–1823 (2010)Google Scholar
Lang, M., Tracy, C.L., Palomares, R.I., Zhang, F.X., Severin, D., Bender, M., Trautmann, C., Park, C., Prakapenka, V.P., Skuratov, V.A., and Ewing, R.C., Mater. Res. 30(9), 1366–1379 (2015)Google Scholar
Shamblin, J., Feygenson, M., Neuefeind, J., Tracy, C.L., Zhang, F., Finkeldei, S., Bosbach, D., Zhou, H., Ewing, R.C., and Lang, M., Nat. Mater. 15, 507–512 (2016)Google Scholar
O’Quinn, E.C., Shamblin, J., Perlov, B., Ewing, R.C., Neuefeind, J., Feygenson, M., Gussev, I., and Lang, M., J. Am. Chem. Soc. 139, 10395–10402 (2017).Google Scholar
Gibbons, J.F., Proc. IEEE 60, 1062–1096 (1972)Google Scholar
Lang, M., Lian, J., Zhang, J.M., Zhang, F.X., Weber, W.J., Trautmann, C., and Ewing, R.C., Phys. Rev. B 79(22), 1–9 (2009)Google Scholar
Shamblin, J., Tracy, C.L., Palomares, R.I., O’Quinn, E.C., Ewing, R.C., Neuefeind, J., Feygenson, M., Behrens, J., Trautmann, C., and Lang, M., Acta Mater. 144, 60–67 (2018)Google Scholar
Charpentier, T., Martel, L., Mir, A.H., Somers, J., Jegou, C., and Peuget, S., Scientific Reports 6, (2016)Google Scholar
Peuget, S., Mendoza, C., Maugeri, E.A., Delaye, J.M., Caraballo, R., Charpentier, T., Tribet, M., Bouty, O., and Jegou, C., Procedia Materials Science 7, 252 – 261 (2014)Google Scholar
Peuget, S., in preparation.Google Scholar