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

Dandeneau, Christopher S.; Hong, Tao; Brinkman, Kyle S.; Vance, Eric R.; Amoroso, Jake W.

doi:10.1016/j.jnucmat.2018.02.006

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 Ba_1.0Cs_0.3Cr_1.0Al_0.3Fe_1.0Ti_5.7O₁₆ 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:

Dandeneau, Christopher S. ^[1]; Hong, Tao ^[2];

^[2]; Vance, Eric R. ^[3]; Amoroso, Jake W. ^[1]

Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Clemson Univ., SC (United States)
Australian Nuclear Science and Technology Organisation (ANSTO), Lucas Heights, NSW (Australia)

Publication Date:: Thu Feb 08 00:00:00 EST 2018

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.

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                    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.  https://doi.org/10.1016/j.jnucmat.2018.02.006

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                    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.  https://doi.org/10.1016/j.jnucmat.2018.02.006.  https://www.osti.gov/servlets/purl/1427454.

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@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         = {Thu Feb 08 00:00:00 EST 2018},

  month        = {Thu Feb 08 00:00:00 EST 2018}

}

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https://doi.org/10.1016/j.jnucmat.2018.02.006

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Cited by: 10 works

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

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

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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

Citation Formats

Figures / Tables:

Materials Science of High-Level Nuclear Waste Immobilization journal, January 2009

Cold crucible induction melter studies for making glass ceramic waste forms: A feasibility assessment journal, January 2014

The SYNROC process: A geochemical approach to nuclear waste immobilization. journal, January 1979

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Preparation and characterization of (Ba,Cs)(M,Ti)8O16 (M=Al3+, Fe3+, Ga3+, Cr3+, Sc3+, Mg2+) hollandite ceramics developed for radioactive cesium immobilization journal, June 2007

Synthesis and characterization of hollandite-type material intended for the specific containment of radioactive cesium journal, October 2006

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Nuclear waste disposal—pyrochlore (A2B2O7): Nuclear waste form for the immobilization of plutonium and “minor” actinides journal, June 2004

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Cold crucible induction melter test for crystalline ceramic waste form fabrication: A feasibility assessment journal, April 2017

Crystal field effects in chromium and its partitioning in the mantle journal, June 1975

Crystallization behavior during melt-processing of ceramic waste forms journal, May 2016

Influence of Lubricants and Attrition Milling Parameters on the Quality of Zirconolite Ceramics, Consolidated by Hot Isostatic Pressing, for Immobilization of Plutonium journal, February 2014

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The evolution of ‘sol–gel’ chemistry as a technique for materials synthesis journal, January 2016

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Synthesis and phase structure of (Cs0.8−xBa0.4+x)(Al3+1.6+ xTi4+6.4− x)O16 ceramics using sol-spray pyrolysis route for immobilizing radioactive cesium journal, May 2019

Materials Science of High-Level Nuclear Waste Immobilization
journal, January 2009

Cold crucible induction melter studies for making glass ceramic waste forms: A feasibility assessment
journal, January 2014

The SYNROC process: A geochemical approach to nuclear waste immobilization.
journal, January 1979

Disposal of high-level nuclear wastes: a geological perspective
journal, April 1985

Immobilisation of high level nuclear reactor wastes in SYNROC
journal, March 1979

Comparative Study of Synroc-C Ceramics Produced by Hot-Pressing and Inductive Melting
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The crystal structure of hollandite.
journal, January 1986

Preparation and characterization of (Ba,Cs)(M,Ti)8O16 (M=Al3+, Fe3+, Ga3+, Cr3+, Sc3+, Mg2+) hollandite ceramics developed for radioactive cesium immobilization
journal, June 2007

Synthesis and characterization of hollandite-type material intended for the specific containment of radioactive cesium
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Thermochemistry of Barium Hollandites
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Nuclear waste disposal—pyrochlore (A2B2O7): Nuclear waste form for the immobilization of plutonium and “minor” actinides
journal, June 2004

Ceramic Waste Forms for Actinides
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Structural Transformations and Disordering in Zirconolite (CaZrTi ₂ O ₇ ) at High Pressure
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journal, November 2014

Immobilisation of radioactive waste in glasses, glass composite materials and ceramics
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