Potential benefit of amorphization in the retention of gaseous species in irradiated pyrochlores

Holesinger, Terry G.; Valdez, James A.; Janish, Matthew T.; Wang, Yongqiang; Uberuaga, Blas P.

doi:10.1016/j.actamat.2018.10.049

Title: Potential benefit of amorphization in the retention of gaseous species in irradiated pyrochlores

Abstract

Understanding the structure-property relationship for materials destined for irradiation extremes is a key step in developing materials with reliable, long-term performance. One crucial relationship is the ability of a material to withstand or accommodate amorphization, as this dictates its potential use as a nuclear waste form. Pyrochlores are one such class of materials for consideration as waste forms and there has been significant work examining how both the crystal structure and chemistry impacts amorphization resistance, leading to the important conclusion that the amorphization resistance of pyrochlores (A₂B₂O₇) is very sensitive to the nature of the B cations. For example, pyrochlores with B=Ti amorphize much more readily than B=Zr compounds. However, there are still questions regarding how these types of materials respond to prolonged or high-dose irradiation conditions. Gd₂Ti₂O₇ (GTO) and Gd₂Zr₂O₇ (GZO) pyrochlores were implanted with 400 keV Kr++ ions at room temperature to calculated peak damages of 119 and 135 displacements per atom (dpa), respectively. As expected, GTO amorphized completely under irradiation. However, discrete bubbles of Kr coalesced within the amorphous matrix without micro-cracking or spallation. In contrast, GZO transforms to a disordered fluorite structure under irradiation with no indications of localized amorphization. But, the accumulation of Kr withinmore »« less

Authors:

^[1]; Valdez, James A. ^[1]; Janish, Matthew T. ^[1];

^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Publication Date:: Mon Oct 29 00:00:00 EDT 2018

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1482005

Alternate Identifier(s):: OSTI ID: 1636974

Report Number(s):: LA-UR-18-25544
Journal ID: ISSN 1359-6454

Grant/Contract Number:: AC52-06NA25396; 2013LANL8400

Resource Type:: Accepted Manuscript

Journal Name:: Acta Materialia

Additional Journal Information:: Journal Volume: 164; Journal ID: ISSN 1359-6454

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; pyrochlore microscopy amorphous irradiation

Citation Formats


                    Holesinger, Terry G., Valdez, James A., Janish, Matthew T., Wang, Yongqiang, and Uberuaga, Blas P. Potential benefit of amorphization in the retention of gaseous species in irradiated pyrochlores.  United States: N. p., 2018. 
Web.  doi:10.1016/j.actamat.2018.10.049.

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                    Holesinger, Terry G., Valdez, James A., Janish, Matthew T., Wang, Yongqiang, & Uberuaga, Blas P. Potential benefit of amorphization in the retention of gaseous species in irradiated pyrochlores.  United States.  https://doi.org/10.1016/j.actamat.2018.10.049

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                    Holesinger, Terry G., Valdez, James A., Janish, Matthew T., Wang, Yongqiang, and Uberuaga, Blas P. Mon .  
"Potential benefit of amorphization in the retention of gaseous species in irradiated pyrochlores".  United States.  https://doi.org/10.1016/j.actamat.2018.10.049.  https://www.osti.gov/servlets/purl/1482005.

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@article{osti_1482005,

  title        = {Potential benefit of amorphization in the retention of gaseous species in irradiated pyrochlores},

  author       = {Holesinger, Terry G. and Valdez, James A. and Janish, Matthew T. and Wang, Yongqiang and Uberuaga, Blas P.},

  abstractNote = {Understanding the structure-property relationship for materials destined for irradiation extremes is a key step in developing materials with reliable, long-term performance. One crucial relationship is the ability of a material to withstand or accommodate amorphization, as this dictates its potential use as a nuclear waste form. Pyrochlores are one such class of materials for consideration as waste forms and there has been significant work examining how both the crystal structure and chemistry impacts amorphization resistance, leading to the important conclusion that the amorphization resistance of pyrochlores (A2B2O7) is very sensitive to the nature of the B cations. For example, pyrochlores with B=Ti amorphize much more readily than B=Zr compounds. However, there are still questions regarding how these types of materials respond to prolonged or high-dose irradiation conditions. Gd2Ti2O7 (GTO) and Gd2Zr2O7 (GZO) pyrochlores were implanted with 400 keV Kr++ ions at room temperature to calculated peak damages of 119 and 135 displacements per atom (dpa), respectively. As expected, GTO amorphized completely under irradiation. However, discrete bubbles of Kr coalesced within the amorphous matrix without micro-cracking or spallation. In contrast, GZO transforms to a disordered fluorite structure under irradiation with no indications of localized amorphization. But, the accumulation of Kr within the host material leads to sub-grain structures, extended defects, and the development of micro-cracks. Thus, while GTO readily amorphizes even under low dose irradiations, the resistance of the amorphous GTO matrix to micro cracking and gas release, even in the presence of large bubble formation, suggests an enhanced propensity to retain gaseous species. Finally, consideration of long-term dose accumulation effects in nuclear waste forms would suggest reconsideration of amorphization processes in pyrochlores and related materials as a potential beneficial effect for immobilization and long-term storage of actinide materials.},

  doi          = {10.1016/j.actamat.2018.10.049},

  journal      = {Acta Materialia},

  number       = ,

  volume       = 164,

  place        = {United States},

  year         = {Mon Oct 29 00:00:00 EDT 2018},

  month        = {Mon Oct 29 00:00:00 EDT 2018}

}

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https://doi.org/10.1016/j.actamat.2018.10.049

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Figure 1: SRIM estimates of the peak damage and Kr deposition profiles as a function of thickness from the sample surface for a 400 keV Kr irradiation dose of 5.36 x 10¹⁶Kr/cm² for (a) Gd₂Ti₂O₇and (b) Gd₂Zr₂O₇.

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Title: Potential benefit of amorphization in the retention of gaseous species in irradiated pyrochlores

Abstract

Citation Formats

Figures / Tables:

Preparation and properties of some phases in the system Nd2O3−CeO2−ZrO2−RuO2 journal, December 1980

Natural Pyrochlores: Analogues For Actinide Host Phases in Radioactive Waste Forms journal, January 1984

Crystal Chemical Constraints on the Formation of Actinide Pyrochlores journal, January 1984

Lanthanide-Containing Zirconotitanate Solid Solutions journal, December 1996

Syntheses of Titanate-Based Hosts for the Immobilization of Pu(III) and Am(III) journal, January 1996

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

Nuclear waste forms for actinides journal, March 1999

Ceramic matrices for plutonium disposition journal, November 2007

Radiation stability of gadolinium zirconate: A waste form for plutonium disposition journal, December 1999

Radiation Tolerance of Complex Oxides journal, August 2000

Ion-irradiation-induced amorphization of La 2 Zr 2 O 7 pyrochlore journal, August 2002

Radiation-induced amorphization of rare-earth titanate pyrochlores journal, October 2003

Swift heavy ion track formation in Gd2Zr2−Ti O7 pyrochlore: Effect of electronic energy loss journal, October 2014

Nature of the chemical bond and prediction of radiation tolerance in pyrochlore and defect fluorite compounds journal, April 2007

Structural response of titanate pyrochlores to swift heavy ion irradiation journal, September 2016

Disorder in Pyrochlore Oxides journal, August 2000

Using Machine Learning To Identify Factors That Govern Amorphization of Irradiated Pyrochlores journal, November 2016

Radiation effects in nuclear waste forms for high-level radioactive waste journal, January 1995

Radiation effects in crystalline ceramics for the immobilization of high-level nuclear waste and plutonium journal, June 1998

Bubble formation and lattice parameter changes resulting from He irradiation of defect-fluorite Gd2Zr2O7 journal, August 2016

Combined effects of radiation damage and He accumulation on bubble nucleation in Gd2Ti2O7 journal, October 2016

The radiation-induced crystalline-to-amorphous transition in zircon journal, March 1994

Probing disorder in isometric pyrochlore and related complex oxides journal, February 2016

Intricate disorder in defect fluorite/pyrochlore: a concord of chemistry and crystallography journal, June 2017

Response of Gd2Ti2O7 and La2Ti2O7 to swift-heavy ion irradiation and annealing journal, July 2015

Radiation and Thermal Ageing of Nuclear Waste Glass journal, January 2014

Large swelling and percolation in irradiated zircon journal, December 2002

Helium bubble formation in nuclear glass by in-situ TEM ion implantation journal, September 2014

Helium mobility in SON68 borosilicate nuclear glass: A nuclear reaction analysis approach journal, November 2013

Superior radiation tolerant materials: Amorphous silicon oxycarbide journal, June 2015

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Preparation and properties of some phases in the system Nd2O3−CeO2−ZrO2−RuO2
journal, December 1980

Natural Pyrochlores: Analogues For Actinide Host Phases in Radioactive Waste Forms
journal, January 1984

Crystal Chemical Constraints on the Formation of Actinide Pyrochlores
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Lanthanide-Containing Zirconotitanate Solid Solutions
journal, December 1996

Syntheses of Titanate-Based Hosts for the Immobilization of Pu(III) and Am(III)
journal, January 1996

Immobilisation of high level nuclear reactor wastes in SYNROC
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Nuclear waste forms for actinides
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Ceramic matrices for plutonium disposition
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Radiation stability of gadolinium zirconate: A waste form for plutonium disposition
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Radiation Tolerance of Complex Oxides
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Ion-irradiation-induced amorphization of ${La}_{2} {Zr}_{2} O_{7}$ pyrochlore
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Radiation-induced amorphization of rare-earth titanate pyrochlores
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The radiation-induced crystalline-to-amorphous transition in zircon
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Probing disorder in isometric pyrochlore and related complex oxides
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Intricate disorder in defect fluorite/pyrochlore: a concord of chemistry and crystallography
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