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

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 inmore » 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). In conclusion, 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.« less

Authors:
 [1];  [1];  [1]; ORCiD logo [2]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1484144
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
MRS Advances
Additional Journal Information:
Journal Volume: 3; Journal Issue: 31; Journal ID: ISSN 2059-8521
Publisher:
Materials Research Society (MRS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Lang, Maik, O’Quinn, Eric C., Shamblin, Jacob, and Neuefeind, Jörg C. Advanced Experimental Technique for Radiation Damage Effects in Nuclear Waste Forms: Neutron Total Scattering Analysis. United States: N. p., 2018. Web. doi:10.1557/adv.2018.199.
Lang, Maik, O’Quinn, Eric C., Shamblin, Jacob, & Neuefeind, Jörg C. Advanced Experimental Technique for Radiation Damage Effects in Nuclear Waste Forms: Neutron Total Scattering Analysis. United States. doi:10.1557/adv.2018.199.
Lang, Maik, O’Quinn, Eric C., Shamblin, Jacob, and Neuefeind, Jörg C. Mon . "Advanced Experimental Technique for Radiation Damage Effects in Nuclear Waste Forms: Neutron Total Scattering Analysis". United States. doi:10.1557/adv.2018.199. https://www.osti.gov/servlets/purl/1484144.
@article{osti_1484144,
title = {Advanced Experimental Technique for Radiation Damage Effects in Nuclear Waste Forms: Neutron Total Scattering Analysis},
author = {Lang, Maik and O’Quinn, Eric C. and Shamblin, Jacob and Neuefeind, Jörg C.},
abstractNote = {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). In conclusion, 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.},
doi = {10.1557/adv.2018.199},
journal = {MRS Advances},
number = 31,
volume = 3,
place = {United States},
year = {2018},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Figure 1 Figure 1: Representative XRD patterns of Er2Sn2O7 before and after irradiation with 2.2 GeV Au ions to various ion fluences (fluence values in ions/cm2). The initial pattern, before irradiation, corresponds to a pyrochlore structure. Upon increasing irradiation, peaks related to pyrochlore superstructure ordering are attenuated, while peaks related to fluoritemore » substructure are retained. This indicates a transformation from the pyrochlore phase to a phase with a long-range defectfluorite structure.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.