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Glass structure and crystallization in boro-alumino-silicate glasses containing rare earth and transition metal cations: a US-UK collaborative program

Published online by Cambridge University Press:  06 February 2019

John S. McCloy Open the ORCID record for John S. McCloy [Opens in a new window] ,
José Marcial ,
Deepak Patil ,
Muad Saleh Open the ORCID record for Muad Saleh [Opens in a new window] ,
Mostafa Ahmadzadeh ,
Hua Chen ,
Jarrod V. Crum ,
Brian J. Riley ,
Hrishikesh Kamat  and
Antoine Bréhault
...Show all authors
John S. McCloy*
Affiliation:
Washington State University, Pullman, WA, USA Pacific Northwest National Laboratory, Richland, WA, USA
José Marcial
Affiliation:
Washington State University, Pullman, WA, USA
Deepak Patil
Affiliation:
Washington State University, Pullman, WA, USA
Muad Saleh
Affiliation:
Washington State University, Pullman, WA, USA
Mostafa Ahmadzadeh
Affiliation:
Washington State University, Pullman, WA, USA
Hua Chen
Affiliation:
Washington State University, Pullman, WA, USA Inner Mongolia University of Science and Technology, China
Jarrod V. Crum
Affiliation:
Pacific Northwest National Laboratory, Richland, WA, USA
Brian J. Riley
Affiliation:
Washington State University, Pullman, WA, USA Pacific Northwest National Laboratory, Richland, WA, USA
Hrishikesh Kamat
Affiliation:
Rutgers University, New Jersey, USA
Antoine Bréhault
Affiliation:
Rutgers University, New Jersey, USA
Ashutosh Goel
Affiliation:
Rutgers University, New Jersey, USA
Kristian E. Barnsley
Affiliation:
University of Warwick, Coventry, UK
John V. Hanna
Affiliation:
University of Warwick, Coventry, UK
Prashant Rajbhandari
Affiliation:
University of Sheffield, Sheffield, UK
Claire L. Corkhill
Affiliation:
University of Sheffield, Sheffield, UK
Russell J. Hand
Affiliation:
University of Sheffield, Sheffield, UK
Neil C. Hyatt
Affiliation:
University of Sheffield, Sheffield, UK
*
*(Email: [email protected])
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Abstract

Nuclear wastes generated from reprocessing of used nuclear fuel tend to contain a large fraction of rare earth (RE, e.g., Nd3+), transition (TM, e.g., Mo6+, Zr4+), alkali (A, e.g., Cs+), and alkaline earth cations (AE, e.g., Ba2+, Sr2+). Various strategies have been considered for immobilizing such waste streams, varying from nominally crystal-free glass to glass-ceramic to multi-phase ceramic waste forms. For glass and glass-ceramic waste forms, the added glass-forming system is generally alkali-alkaline earth-aluminoborosilicate (i.e., Na-Ca-Al-B-Si oxide). In a US-UK collaborative project, summarized here, we investigated the glass structure and crystallization dependence on compositional changes in simulated nuclear waste glasses and glass-ceramics. Compositions ranged in complexity from five – to – eight oxides. Specifically, the roles of Mo and rare earths are investigated, since a proposed glass-ceramic waste form contains crystalline phases such as powellite [(AE,A,RE)MoO4] and oxyapatite [(RE,AE,A)10Si6O26], and the precipitation of molybdenum phases is known to be affected by the rare earth concentration in the glass. Additionally, the effects of other chemical additions have been systematically investigated, including Zr, Ru, P, and Ti. A series of studies were also undertaken to ascertain the effect of the RE size on glass structure and on partitioning to crystal phases, investigating similarities and differences in glasses containing single RE oxides of Sc, Y, La, Ce, Nd, Sm, Er, Yb, or Lu. Finally, the effect of charge compensation was investigated by considering not only the commonly assessed peralkaline glass but also metaluminous and peraluminous compositions. Glass structure and crystallization studies were conducted by spectroscopic methods (i.e., Raman, X-ray absorption, nuclear magnetic resonance (NMR), optical absorption, photoluminescence, photoluminescence excitation, X-ray photoelectron spectroscopy), microscopy (i.e., scanning electron microscopy, transmission electron microscopy, electron probe microanalysis), scattering (i.e., X-ray and neutron diffraction, small angle measurements), and physical characterization (i.e., differential thermal analysis, liquidus, viscosity, density). This paper will give an overview of the research program and some example unpublished results on glass-ceramic crystallization kinetics, microstructure, and Raman spectra, as well as some examples of the effects of rare earths on the absorption, luminescence, and NMR spectra of starting glasses. The formal collaboration described here has resulted in the generation of a large number of results, some of which are still in the process of being published as separate studies.

Keywords

nuclear materialswaste managementrare-earthsnuclear magnetic resonance (NMR)crystallization
Type
Articles
Information
MRS Advances , Volume 4 , Issue 17-18: Energy-Transfer, Storage and Conversion , 2019 , pp. 1029 - 1043
Copyright
Copyright © Materials Research Society 2019 

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