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Instruments / Technical Area	Publication Details	Published
I11-High Resolution Powder Diffraction	A potential wasteform for Cs immobilization: synthesis, structure determination, and aqueous durability of Cs2TiNb6O18 Tzu-Yu Chen , Ewan R. Maddrell , Neil C. Hyatt , Joseph A. Hriljac Inorganic Chemistry 55, 12686 - 12695 DOI: 10.1021/acs.inorgchem.6b01826 Diamond Proposal Number(s): [11089] Open Access Show Abstract ▼ Abstract: Cs2TiNb6O18 is a potential ceramic wasteform for the long-term immobilization of radioactive cesium. Cs2TiNb6O18 was synthesized using the aqueous precursor method and a solid-state reaction, and its crystal structure was determined from the Rietveld refinement of synchrotron X-ray and neutron powder diffraction data. The structure is a pyrochlore analogue, space group P3̅m1 with Cs in 9-fold coordination. The calculated bond valence sum from analysis of neutron diffraction data of 0.84 and high coordination number suggest that Cs has a strong bonding environment. The chemical aqueous durability was investigated using the MCC-1 and PCT-B standard test methods. The measured Cs leach rates of 3.8 × 10–3 and 2.1 × 10–3 g m–2 day–1 obtained via the MCC-1 and PCT-B methods, respectively, demonstrate good promise of a safe long-term immobilization material comparable to, if not better than, hollandite—the material in the multiphase titanate ceramics (Synroc) targeted for cesium sequestration.	Dec 2016
	Doped umbite materials for selective abatement of cesium radionuclides from nuclear waste streams Antony Nearchou , Tzu-Yu Chen , Daniel S. Parsons , Luke O’brien , Nicholas A. Hodge , Liam Abrahamsen-Mills , Phoebe K. Allan , Jospeh A. Hriljac Apl Materials 11 DOI: 10.1063/5.0134977 Open Access Show Abstract ▼ Abstract: Sb- and Nb-doped Zr and Sn-umbites have been prepared using hydrothermal synthesis with both high purity and yield. All four materials display excellent removal of Cs+ cations from acidic, neutral, and basic solutions, abating at least 80% of the Cs present. This performance is retained in the presence of competing Na+ cations as well as across the pH range. The most sustained selectivity is observed in acidic media, with evidence of a minor reduction in selectivity under basic conditions. The umbites have successfully been shaped into pellets, introducing macroporosity and retaining the selective uptake of Cs in the presence of excess Na. Through thermal treatment, samples of partially Cs-exchanged umbite can be converted into dense silicate phases where radioactive Cs can be immobilized in a potential wasteform for long term storage. These findings present doped umbites as prospective materials for industrial use with selective abatement properties and capabilities for deployment followed by end of life geological disposal.	Jan 2023
	Nuclear wastewater decontamination by 3D-Printed hierarchical zeolite monoliths Oded Halevi , Tzu-Yu Chen , Pooi See Lee , Shlomo Magdassi , Joseph A. Hriljac Rsc Advances 10, 5766 - 5776 DOI: 10.1039/C9RA09967K Open Access Show Abstract ▼ Abstract: The selective removal of radioactive cationic species, specifically 137Cs+ and 90Sr2+, from contaminated water is critical for nuclear waste remediation processes and environmental cleanup after accidents, such as the Fukushima Daiichi Nuclear Power Plant disaster in 2011. Nanoporous silicates, such as zeolites, are most commonly used for this process but in addition to acting as selective ion exchange media must also be deployable in a correct physical form for flow columns. Herein, Digital Light Processing (DLP) three-dimensional (3D) printing was utilized to form monoliths from zeolite ion exchange powders that are known to be good for nuclear wastewater treatment. The monoliths comprise 3D porous structures that will selectively remove radionuclides in an engineered form that can be tailored to various sizes and shapes as required for any column system and can even be made with fine-grained powders unsuitable for normal gravity flow column use. 3D-printed monoliths of zeolites chabazite and 4A were made, characterized, and evaluated for their ion exchange capacities for cesium and strontium under static conditions. The 3D-printed monoliths with 50 wt% zeolite loadings exhibit Cs and Sr uptake with an equivalent ion-capacity as their pristine powders. These monoliths retain their porosity, shape and mechanical integrity in aqueous media, providing a great potential for use to not only remove radionuclides from nuclear wastewater, but more widely in other aqueous separation-based applications and processes.	Feb 2020
I11-High Resolution Powder Diffraction	Transformation of Cs-IONSIV ® into a ceramic wasteform by hot isostatic pressing Tzu-Yu Chen , Ewan R. Maddrell , Neil C. Hyatt , Amy S. Gandy , Martin C. Stennett , Joseph A. Hriljac Journal Of Nuclear Materials DOI: 10.1016/j.jnucmat.2017.10.011 Diamond Proposal Number(s): [11089] Open Access Show Abstract ▼ Abstract: A simple method to directly convert Cs-exchanged IONSIV® IE-911 into a ceramic wasteform by hot isostatic pressing (1100 °C/190 MPa/2 hr) is presented. Two major Cs-containing phases, Cs2TiNb6O18 and Cs2ZrSi6O15, and a series of mixed oxides form. The microstructure and phase assemblage of the samples as a function of Cs content were examined using XRD, XRF, SEM and TEM/EDX. The chemical aqueous durability of the materials was investigated using the MCC-1 and PCT-B standard test methods. For HIPed Cs-IONSIV® samples, the MCC-1 normalised release rates of Cs were <1.57 × 10−1 g m−2 d−1 at 0–28 days, and <3.78 × 10−2 g m−2 d−1 for PCT-B at 7 days. The low rates are indicative of a safe long-term immobilisation matrix for Cs formed directly from spent IONSIV®. It was also demonstrated that the phase formation can be altered by adding Ti metal due to a controlled redox environment.	Oct 2017

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