NSUF 20-4102: Development of radiation tolerant matrices for rare-earths designed for burnable poisons as part of the nuclear fuel array

NSUF RTE Argonne National Labs IVEM – Tandem facility. March 2020 Investigators: Nestor Zaluzec (PI) Robert D. Aughterson Gregory R. Lumpkin Technical Abstract: Objectives Rare-earth titanates with pyrochlore and fluorite structures have been synthesised and characterised with a focus on creating materials suitable for use as burnable poisons and waste-form matrices. The aim of this study is to develop the fabrication of highly radiation tolerant matrices containing rare- earths. The objective of monitoring the test materials’ response to irradiating ions is to attain a quantifiable characteristic; the critical dose of irradiating ions required to facilitate a transition from a crystalline to amorphous state, Dc. This provides a means of comparing the radiation tolerance between the materials of interest. Also by measuring the Dc at various temperatures and plotting the response we attain a second quantity; the critical temperature of crystallinity, Tc, (the temperature above which the rate of crystalline structure recovery is greater than the rate of defect accumulation). This gives us another means of comparing material response to ion-irradiation along with testing at temperatures applicable to nuclear-based application environments. Methods The complex ceramic oxides are exposed to high energy ions (Kr 1 MeV, and/or He 20 keV) whilst being monitored in-situ using the transmission electron microscope (TEM) (IVEM-tandem facility). Collection of bright field images (BF) and electron diffraction patterns (SADP) are used to monitor the crystalline to amorphous phase transition. The TEM specimens consist of finely ground ceramic crystalline fragments dispersed on holey carbon film supported on TEM specimen grids. TEM characterisation involves the collection of BF and SADPs of 5 grains. After collection of images the sample is irradiated to a certain dose. Selected ion doses followed by BF and SADP collection are continued until there are no observable Bragg diffraction spots left in the SADP. This approach is used to measure the irradiating ion dose required to cause amorphisation. The critical dose of amorphisation gives a quantitative approach for comparing radiation tolerance between different test materials. This same experimental approach is repeated for the test material whilst holding it at a range of temperatures. The duration of each critical dose measurement is dependent on both the dose of ions required to render the sample amorphous and the time it takes to cool or heat the sample. Potential Impact to state-of-the Knowledge

The proposed test materials have pyrochlore / fluorite structure types, structures associated with flexibility in radionuclide incorporation along with radiation tolerance. The proposed test materials consist of novel compounds that may lend to improvement in these properties. The proposed radiation response study will have considerable impact on the decision making process for down-selection of the best candidates for further development as burnable poisons, and waste form matrices. Period of performance On average 1 critical dose measurement takes approximately 2 hours. 3 to 5 specimens are tested per day. There are 9 samples proposed requiring approximately 1 day per sample. This proposal is requesting the maximum 10 days.

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Abstract NSUF RTE Argonne National Labs IVEM – Tandem facility. March 2020 Investigators: Nestor Zaluzec (PI) Robert D. Aughterson Gregory R. Lumpkin Technical Abstract: Objectives Rare-earth titanates with pyrochlore and fluorite structures have been synthesised and characterised with a focus on creating materials suitable for use as burnable poisons and waste-form matrices. The aim of this study is to develop the fabrication of highly radiation tolerant matrices containing rare- earths. The objective of monitoring the test materials’ response to irradiating ions is to attain a quantifiable characteristic; the critical dose of irradiating ions required to facilitate a transition from a crystalline to amorphous state, Dc. This provides a means of comparing the radiation tolerance between the materials of interest. Also by measuring the Dc at various temperatures and plotting the response we attain a second quantity; the critical temperature of crystallinity, Tc, (the temperature above which the rate of crystalline structure recovery is greater than the rate of defect accumulation). This gives us another means of comparing material response to ion-irradiation along with testing at temperatures applicable to nuclear-based application environments. Methods The complex ceramic oxides are exposed to high energy ions (Kr 1 MeV, and/or He 20 keV) whilst being monitored in-situ using the transmission electron microscope (TEM) (IVEM-tandem facility). Collection of bright field images (BF) and electron diffraction patterns (SADP) are used to monitor the crystalline to amorphous phase transition. The TEM specimens consist of finely ground ceramic crystalline fragments dispersed on holey carbon film supported on TEM specimen grids. TEM characterisation involves the collection of BF and SADPs of 5 grains. After collection of images the sample is irradiated to a certain dose. Selected ion doses followed by BF and SADP collection are continued until there are no observable Bragg diffraction spots left in the SADP. This approach is used to measure the irradiating ion dose required to cause amorphisation. The critical dose of amorphisation gives a quantitative approach for comparing radiation tolerance between different test materials. This same experimental approach is repeated for the test material whilst holding it at a range of temperatures. The duration of each critical dose measurement is dependent on both the dose of ions required to render the sample amorphous and the time it takes to cool or heat the sample. Potential Impact to state-of-the Knowledge The proposed test materials have pyrochlore / fluorite structure types, structures associated with flexibility in radionuclide incorporation along with radiation tolerance. The proposed test materials consist of novel compounds that may lend to improvement in these properties. The proposed radiation response study will have considerable impact on the decision making process for down-selection of the best candidates for further development as burnable poisons, and waste form matrices. Period of performance On average 1 critical dose measurement takes approximately 2 hours. 3 to 5 specimens are tested per day. There are 9 samples proposed requiring approximately 1 day per sample. This proposal is requesting the maximum 10 days.
Award Announced Date 2020-07-14T14:04:48.91
Awarded Institution None
Facility None
Facility Tech Lead Wei-Ying Chen
Irradiation Facility None
PI Nestor Zaluzec
PI Email [email protected]
Project Type RTE
RTE Number 4102