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Effect of cooling profile on crystalline phases, oxidation state, and chemical partitioning of complex glasses

Published online by Cambridge University Press:  04 February 2020

J. Marcial Open the ORCID record for J. Marcial [Opens in a new window] ,
O. K. Neill ,
M. Newville ,
J. V. Crum  and
J. McCloy Open the ORCID record for J. McCloy [Opens in a new window]
J. Marcial*
Affiliation:
School of Mechanical and Materials Engineering, Washington State University, Pullman, WA, USA Materials Science and Engineering Program, Washington State University, Pullman, WA, USA
O. K. Neill
Affiliation:
School of Earth and Environmental Sciences, University of Michigan, Ann Arbor, MI, USA
M. Newville
Affiliation:
CARS, University of Chicago, Chicago, IL, USA
J. V. Crum
Affiliation:
Pacific Northwest National Laboratory, Richland, WA, USA
J. McCloy
Affiliation:
School of Mechanical and Materials Engineering, Washington State University, Pullman, WA, USA Materials Science and Engineering Program, Washington State University, Pullman, WA, USA Pacific Northwest National Laboratory, Richland, WA, USA
*
*Corresponding author: J. Marcial, email: jose.marcial@wsu.edu
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Abstract:

Investigations of the crystallization of aluminosilicate phases within Hanford nuclear waste glasses typically involve subjecting samples to the canister centerline cooling (CCC) schedule. This cooling schedule is representative of the slowest cooling thermal profile which these glasses will experience after the glass is poured into the high level waste (HLW) container. However, few investigations have observed how the crystallization behavior changes by varying the heat treatment schedule. In the present study, three Hanford HLW glasses are subjected to CCC and isothermal heat treatments (IHT) to better understand the evolution of phases and the chemical partitioning due to temperature schedule. Samples were characterized using electron probe microanalysis, X-ray diffraction, micro X-ray fluorescence, and micro X-ray absorption spectroscopy. From IHT, eucryptite and apatite phases were observed which were not observed during CCC. Spatially-resolved measurements demonstrated that the oxidation state of the iron was similar among glass and crystal, and we suggest a mechanism to describe the compositional fluctuations near the crystal-glass interface which influence crystallization.

Keywords

crystallizationglassscanning electron microscopy (SEM)extended x-ray absorption fine structure (EXAFS)x-ray diffraction (XRD)
Type
Articles
Information
MRS Advances , Volume 5 , Issue 11: Energy and Environment , 2020 , pp. 569 - 579
Copyright
Copyright © Materials Research Society 2020

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