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Title: Comparison of structure, morphology, and leach characteristics of multi-phase ceramics produced via melt processing and hot isostatic pressing

Abstract

Melt processing of multi-phase ceramic waste forms offers potential advantages over traditional solid-state synthesis methods given both the prevalence of melters currently in use and the ability to reduce the possibility of airborne radionuclide contamination. In this work, multi-phase ceramics with a targeted hollandite composition of Ba1.0Cs0.3Cr1.0Al0.3Fe1.0Ti5.7O16 were fabricated by melt processing at 1675 °C and hot isostatic pressing (HIP) at 1250 and 1300 °C. X-ray diffraction analysis (XRD) confirmed hollandite as the major phase in all specimens. Zirconolite/pyrochlore peaks and weaker perovskite reflections were observed after melt processing, while HIP samples displayed prominent perovskite peaks and low-intensity zirconolite reflections. Melt processing produced specimens with large (>50 μm) well-defined hollandite grains, while HIP yielded samples with a more fine-grained morphology. Elemental analysis showed “islands” rich in Cs and Ti across the surface of the 1300 °C HIP sample, suggesting partial melting and partitioning of Cs into multiple phases. Photoemission data revealed multiple Cs 3d spin-orbit pairs for the HIP samples, with the lower binding energy doublets likely corresponding to Cs located in more leachable phases. Among all specimens examined, the melt-processed sample exhibited the lowest fractional release rates for Rb and Cs. However, the retention of Sr and Mo wasmore » greater in the HIP specimens.« less

Authors:
 [1];  [2]; ORCiD logo [2];  [3];  [1]
  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
  2. Clemson Univ., SC (United States)
  3. Australian Nuclear Science and Technology Organisation (ANSTO), Lucas Heights, NSW (Australia)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1427454
Alternate Identifier(s):
OSTI ID: 1548737
Report Number(s):
SRNL-STI-2017-00651
Journal ID: ISSN 0022-3115; PII: S0022311517314241; TRN: US1802593
Grant/Contract Number:  
AC09-08SR22470
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 502; Journal Issue: C; Journal ID: ISSN 0022-3115
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Dandeneau, Christopher S., Hong, Tao, Brinkman, Kyle S., Vance, Eric R., and Amoroso, Jake W. Comparison of structure, morphology, and leach characteristics of multi-phase ceramics produced via melt processing and hot isostatic pressing. United States: N. p., 2018. Web. doi:10.1016/j.jnucmat.2018.02.006.
Dandeneau, Christopher S., Hong, Tao, Brinkman, Kyle S., Vance, Eric R., & Amoroso, Jake W. Comparison of structure, morphology, and leach characteristics of multi-phase ceramics produced via melt processing and hot isostatic pressing. United States. doi:10.1016/j.jnucmat.2018.02.006.
Dandeneau, Christopher S., Hong, Tao, Brinkman, Kyle S., Vance, Eric R., and Amoroso, Jake W. Thu . "Comparison of structure, morphology, and leach characteristics of multi-phase ceramics produced via melt processing and hot isostatic pressing". United States. doi:10.1016/j.jnucmat.2018.02.006. https://www.osti.gov/servlets/purl/1427454.
@article{osti_1427454,
title = {Comparison of structure, morphology, and leach characteristics of multi-phase ceramics produced via melt processing and hot isostatic pressing},
author = {Dandeneau, Christopher S. and Hong, Tao and Brinkman, Kyle S. and Vance, Eric R. and Amoroso, Jake W.},
abstractNote = {Melt processing of multi-phase ceramic waste forms offers potential advantages over traditional solid-state synthesis methods given both the prevalence of melters currently in use and the ability to reduce the possibility of airborne radionuclide contamination. In this work, multi-phase ceramics with a targeted hollandite composition of Ba1.0Cs0.3Cr1.0Al0.3Fe1.0Ti5.7O16 were fabricated by melt processing at 1675 °C and hot isostatic pressing (HIP) at 1250 and 1300 °C. X-ray diffraction analysis (XRD) confirmed hollandite as the major phase in all specimens. Zirconolite/pyrochlore peaks and weaker perovskite reflections were observed after melt processing, while HIP samples displayed prominent perovskite peaks and low-intensity zirconolite reflections. Melt processing produced specimens with large (>50 μm) well-defined hollandite grains, while HIP yielded samples with a more fine-grained morphology. Elemental analysis showed “islands” rich in Cs and Ti across the surface of the 1300 °C HIP sample, suggesting partial melting and partitioning of Cs into multiple phases. Photoemission data revealed multiple Cs 3d spin-orbit pairs for the HIP samples, with the lower binding energy doublets likely corresponding to Cs located in more leachable phases. Among all specimens examined, the melt-processed sample exhibited the lowest fractional release rates for Rb and Cs. However, the retention of Sr and Mo was greater in the HIP specimens.},
doi = {10.1016/j.jnucmat.2018.02.006},
journal = {Journal of Nuclear Materials},
number = C,
volume = 502,
place = {United States},
year = {2018},
month = {2}
}

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Figures / Tables:

Table 1 Table 1: Targeted oxide concentrations for the baseline CAF-131 composition.*

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