1. Tribute to Eric Raymond (Lou) Vance (15th November, 1942–7th March, 2019).
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Finlayson, Trevor R., Gregg, Daniel J., and Sorrell, Charles C.
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HIGH temperature superconductivity , *EARTH sciences , *HOT pressing , *ELECTRICAL conductivity measurement , *MANUFACTURING processes , *DIAMONDS , *PHYSICAL sciences , *THERMAL stresses - Abstract
Begg and E.R. Vance
Leaching of Synroc in D 2 O E.R. Eric Raymond Vance, known as Lou to almost all of his friends and colleagues, was born in Ararat but during his childhood the family moved to Stawell where his father, Albert Louis Vance, established a pharmacy business. Vance , M.L. Carter, K.S. Finnie, B.D. Begg, M.W. Stewart, R.A. Day, Z. Zhang and S.J. Thomson2003 Geopolymers for Radioactive Waste Immobilisation E.R. Vance , J.D. Cashion, J.V. Hanna, Z. Garrett and M. Bhati2006 Positron Annihilation Lifetime Spectroscopy on Cation Vacancies in Synroc Minerals-Perovskite, Zirconolite and Pyrochlore Structures E.R. [Extracted from the article] - Published
- 2022
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2. The role of certification, risk and time preferences in promoting adoption of climate-resilient citrus varieties in Indonesia.
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Hasibuan, Abdul Muis, Gregg, Daniel, and Stringer, Randy
- Abstract
The adoption rate of certified climate-resilient crop seedling varieties in developing countries is generally low, impacting on the ability of smallholder perennial crop farmers to adapt to climate change. Given the long-lived nature of perennial crop investments and the high level of uncertainty regarding both the quality of the seedlings and the climate to which they will be exposed as mature trees, there are clear linkages to farmers’ subjective beliefs regarding yield differentials between certified and uncertified seedlings, risk behaviours, and time preferences. We consider these aspects using a recently developed survey-based tool for measuring risk and time preferences and link those to stated preferences and observations on the adoption of certified seedlings. Results show that farmers’ beliefs regarding yield and variance of yields of certified and uncertified seedling along with the risk attitudes are significant correlates with seedling choice behaviours. Our results also indicate that information asymmetries in the certified seedling market may play a role in limiting the benefits of certification programs both due to cheating and due to lower levels of adoption. [ABSTRACT FROM AUTHOR]
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- 2021
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3. Synroc technology: Perspectives and current status (Review).
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Gregg, Daniel J., Farzana, Rifat, Dayal, Pranesh, Holmes, Rohan, and Triani, Gerry
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REACTOR fuel reprocessing , *WASTE treatment , *RADIOACTIVE wastes , *FISSION products , *NUCLEAR science , *RADIOACTIVE waste repositories - Abstract
Dr Eric (Lou) Vance spent 32 years at the Australian Nuclear Science and Technology Organisation (ANSTO), where he was dedicated to the development of Synroc technology, a waste treatment solution for intractable nuclear wastes. The original form of Synroc, a multiphase ceramic wasteform based on stable and leach resistant titanate minerals, was invented by Australian scientists in the late 1970s. This formulation was directed toward the immobilization of PUREX wastes from the reprocessing of nuclear fuels. Synroc at ANSTO under the scientific leadership of Dr Vance since evolved beyond these original titanate ceramics into a waste treatment technology platform. This platform can be applied to produce glass, glass‐ceramic and ceramic wasteforms and offers distinct advantages in terms of waste loading and suppressing volatile losses. The platform therefore provides an opportunity to treat those waste streams that are problematic for glass matrices alone or existing vitrification process technologies. Such wastes include, for example, actinide‐bearing wastes, those that contain large proportions of refractory elements, those with significant fission product or corrosive volatile emissions and those wastes resulting from radiopharmaceutical production. The implementation of the latter will see the industrialization of Synroc technology via a first‐of‐a‐kind Synroc Waste Treatment Facility that is currently under construction at ANSTO. This paper will review Synroc technology, particularly noting the substantial and essential contributions from the late Dr Vance. The review will also provide some perspective on the development of the technology for nuclear waste immobilization and describe the significant recent advancements at ANSTO. [ABSTRACT FROM AUTHOR]
- Published
- 2020
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4. Hot Isostatically Pressed (HIPed) fluorite glass‐ceramic wasteforms for fluoride molten salt wastes.
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Gregg, Daniel J., Vance, Eric R., Dayal, Pranesh, Farzana, Rifat, Aly, Zaynab, Holmes, Rohan, Triani, Gerry, and Franks, George
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FUSED salts , *NUCLEAR fuels , *HOT pressing , *RADIOACTIVE wastes , *CALCIUM fluoride , *FLUORIDES , *NUCLEAR reactors - Abstract
Molten pyroprocessing salts can be used to dissolve used nuclear fuel from a reactor allowing recovery of the actinides. Previously, ANSTO have demonstrated hot isostatically pressed (HIPed) sodalite glass‐ceramic wasteforms for eutectic (Li,K)Cl salts containing fission products, but this system cannot be used for the analogous molten alkali fluoride salts (eg, FLiNaK), which have utility in the application of the next generation of nuclear reactors. In this work, a novel glass‐ceramic composite wasteform has been prepared by HIPing, as a candidate for the immobilization of fission product‐bearing FLiNaK salts. The wasteform has been tailored to immobilize the high fluoride content of the waste within fluorite, whereas the waste alkali elements are incorporated in a durable sodium aluminoborosilicate glass, with total waste loadings of ~17‐21 wt% achieved. It was also demonstrated that the speciation of Mo‐ and Sb‐simulated fission products was altered by adding Ti metal due to a controlled redox environment. The resulting candidate wasteform has been studied by X‐ray diffraction and scanning electron microscopy, including the HIP canister‐wasteform interaction zone, and its performance assessed via leaching studies using the PCT and ASTM C1220 leaching protocols. Dr Vance very much enjoyed the challenge of wasteform design for problematic nuclear wastes, for which fission product‐bearing FLiNaK salts are a clear example. His ability to hone in on a wasteform solution with viable waste loadings that meet performance requirements was testament to his nearly 40 years experience in nuclear waste immobilization. The samples discussed in this work represent the last wasteform materials that he prepared. [ABSTRACT FROM AUTHOR]
- Published
- 2020
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5. Understanding the role of social desirability bias and environmental attitudes and behaviour on South Australians' stated purchase of organic foods.
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Wheeler, Sarah Ann, Gregg, Daniel, and Singh, Mrinila
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SELF-deception , *ORGANIC foods , *STRUCTURAL equation modeling , *SOCIAL desirability ,ORGANIC food labeling - Abstract
Highlights • Image management and self-deception bias are explored in a survey of organic food purchase in Australia. • Structural equation modelling assessed the drivers of organic food purchasing frequency. • Self-deception bias had a significant impact on food purchasing frequency. • No significant evidence that image management bias influenced organic purchasing behaviour. • Failure to account for self-deception bias generates considerable upward bias in estimated purchasing frequency. Abstract Organic food purchase choices are a product of consumers' concern about the environment, food safety and food quality, in addition to being influenced by socio-demographics, social pressures and identity. However, in addition to real-world social pressures, respondents to surveys that include questions on organic food purchases may often feel pressure to respond in a socially desirable way. In many survey contexts this means responding more positively to preferences regarding organic food choices or the frequency of purchase decisions. We explore two aspects of socially desirable reporting: (1) image management bias wherein respondents seek to please surveyors through attempting to select answers that may be considered more positively; and (2) self-deception bias wherein respondents unconsciously answer in a way that reflects how they would like to think they behave or will behave. Using an established measure of these social desirability biases, we present a structural equation model to assess the drivers of South Australian consumers' self-reported organic food purchasing frequency (n = 1000). Results indicate that self-deception has a significant and substantive impact on reported organic food purchasing frequency. But, there was no evidence that image management bias directly or indirectly influences organic purchasing behaviour; confirming previous findings that people are motivated to purchase organic food primarily for unselfish reasons (e.g. environment and public good). Failure to account for self-deception bias generates considerable upward bias in estimated purchasing frequency, indicating the need for future organic purchasing surveys to control for social desirability bias. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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6. How can we value an environmental asset that very few have visited or heard of? Lessons learned from applying contingent and inferred valuation in an Australian wetlands case study.
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Gregg, Daniel and Wheeler, Sarah Ann
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CITIES & towns in art , *VALUATION , *CONTINGENT valuation , *ENVIRONMENTAL economics , *ENVIRONMENTAL activism - Abstract
To date, the majority of environmental assets studied in the economic valuation literature clearly have high amenity and recreational use values. However there are many cases where small, but nevertheless unique and important, ecosystems survive as islands amongst large areas of modified, productive, or urban, landscapes. Development encroaches on the landscape and as urban landscapes become more concentrated these types of conservation islands will become increasingly more important. Previous experience with economic valuation suggests that lower total values for smaller contributions to conservation are more liable to be swamped by survey and hypothetical bias measures. Hence there needs to be more understanding of approaches to economic valuation for small and isolated environmental assets, in particular regarding controlling stated preference biases. This study applied the recently developed method of Inferred Valuation (IV) to a small private wetland in South-East Australia, and compared willingness to pay values with estimates from a standard Contingent Valuation (CV) approach. We found that hypothetical bias did seem to be slightly lower with the IV method. However, other methods such as the use of log-normal transformations and median measures, significantly mitigate apparent hypothetical biases and are easier to apply and allow use of the well-tested CV method. [ABSTRACT FROM AUTHOR]
- Published
- 2018
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7. Risk Behaviours and Grazing Land Management: A Framed Field Experiment and Linkages to Range Land Condition.
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Gregg, Daniel and Rolfe, John
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RANGE management , *NONLINEAR statistical models , *DECISION making , *SOCIODEMOGRAPHIC factors , *LAND management - Abstract
We use a framed field experiment considering hypothetical stocking rate decisions made by grazing enterprise managers and estimate non-linear multinomial logit models for a range of nested non-expected utility and expected utility models. The risk and decision-bias parameters for five models estimated for individual responses are shown to be significantly related to land condition but in ways which suggest behavioural aspects of decision making are critical in understanding land management and stocking rate decisions. Our results show that individual heterogeneity in decision making amongst farming groups is likely to be a significant source of variation in farming intensity and technology adoption decisions. This heterogeneity does not appear to be a reflection of socio-demographic characteristics. Furthermore, decision functions appear to be biased toward selection of simpler representative functions (e.g. Expected Utility) for sample averages. This suggests that experimental findings that Expected Utility is representative for actual decisions may be due to sample averaging rather than reflect actual behaviour. [ABSTRACT FROM AUTHOR]
- Published
- 2017
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8. Zirconolite glass-ceramics for plutonium immobilization: The effects of processing redox conditions on charge compensation and durability.
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Zhang, Yingjie, Gregg, Daniel J., Kong, Linggen, Jovanovich, Miodrag, and Triani, Gerry
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PLUTONIUM , *ENCAPSULATION (Catalysis) , *CERAMIC materials , *ISOSTATIC pressing , *OXIDATION-reduction reaction - Abstract
Zirconolite glass-ceramic samples doped with plutonium have been prepared via hot isostatic pressing. The effects of processing redox and plutonium loadings on plutonium valences, the presence of cation vacancies, zirconolite phase compositions, microstructures and durability have been investigated. Either tetravalent or trivalent plutonium ions may be incorporated on the Ca-site of CaZrTi 2 O 7 zirconolite with the Ca-site cation vacancies and the incorporation of Al 3+ ions on the Ti-site for charge compensation. Plutonium and gadolinium (as a neutron absorber) are predominantly partitioned in zirconolite phases leading to the formation of chemically durable glass-ceramics suitable for the immobilization of impure plutonium wastes arising from the nuclear fuel cycle. [ABSTRACT FROM AUTHOR]
- Published
- 2017
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9. Preparation of cerium titanate brannerite by solution combustion, and phase transformation during heat treatment.
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Kong, Linggen, Gregg, Daniel J., Vance, Eric R., Karatchevtseva, Inna, Lumpkin, Gregory R., Blackford, Mark G., Holmes, Rohan, Jovanovic, Miodrag, and Triani, Gerry
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OXIDE minerals , *TOXICOLOGY of combustion gases , *PHASE transitions , *HEAT treatment of metals , *RAMAN spectroscopy - Abstract
An aqueous solution route was employed to prepare cerium titanate oxide brannerite. Thermal analysis, X-ray diffraction, Raman spectroscopy, transmission and scanning electron spectroscopy, were used to investigate the brannerite structure formation and bulk properties. Mixed metal oxides (TiO 2 , CeO 2 and brannerite CeTi 2 O 6 ) were formed upon calcination at 800 °C for 12 h. The amount of brannerite phase decreased to form the constituent oxides with increasing calcination temperature and only pure TiO 2 and CeO 2 were present after 1200 °C calcination. The brannerite CeTi 2 O 6 phase reformed at 1300 °C, and its relative amount was increased with dwell time. After 48 h calcination at 1300 °C, brannerite with only minor metal oxide impurities (<1%) was observed. The sample melted at 1400 °C which led to the collapse of brannerite back to its constituent oxides. Further, the phase formation was influenced by pelletization of the powders, which may be explained by a molar volume increase during brannerite formation. Attempts to confirm this hypothesis using Pu brannerite were inconclusive. [ABSTRACT FROM AUTHOR]
- Published
- 2017
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10. Incorporation of Ba in Al and Fe pollucite.
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Vance, Eric R., Gregg, Daniel J., Griffiths, Grant J., Gaugliardo, Paul R., and Grant, Charmaine
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TRANSMUTATION (Chemistry) , *SOL-gel processes , *CESIUM compounds , *ALUMINUM analysis , *GLASS structure - Abstract
Ba, the transmutation product of radioactive Cs, can be incorporated at levels of up to ∼0.07 formula units in Cs (1−2x) Ba x AlSi 2 O 6 aluminium pollucite formed by sol-gel methods and sintering at 1400 °C, with more Ba forming BaAl 2 Si 2 O 8 phases. The effect of Ba substitution in pollucite-structured CsFeSi 2 O 6 was also studied and no evidence of Ba substitution in the pollucite structure via cation vacancies or Fe 2+ formation was obtained. The Ba entered a Fe-silicate glass structure. Charge compensation was also attempted with a Cs + + Fe 3+ ↔ Ba 2+ + Ni 2+ scheme but again the Ba formed a glass and NiO was evident. PCT leaching data showed CsFeSi 2 O 6 to be very leach resistant. [ABSTRACT FROM AUTHOR]
- Published
- 2016
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11. The value of environment across efficiency quantiles: A conditional regression quantiles analysis of rangelands beef production in north Eastern Australia.
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Gregg, Daniel and Rolfe, John
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BEEF industry , *AGRICULTURAL productivity , *PERFECT competition , *ENVIRONMENTAL health , *REGRESSION quantiles - Abstract
In agricultural systems the value of environmental inputs can be measured using the production function approach whereby the marginal contributions of factors are associated with a shadow value under perfect competition and rationality assumptions. However, empirical studies show that inefficiency in production is common indicating that the rationality assumption is not met. Furthermore, substantial evidence exists to suggest that the contributions of environmental inputs in particular may be differentiated across the efficiency distribution. This means that the frontier technology may not be an appropriate reflection of the technology in use by inefficient enterprises. This article presents the use of conditional regression quantiles to consider how the value of environmental inputs, measured by their contributions to production, vary across efficiency quantiles. We employed a case study of rangelands beef production in Australia to consider how environmental health differentially contributes to production values across efficiency quantiles. Our approach generates detailed insights into the nature of environmentally-sourced technical inefficiency and suggests that conditional quantile regression approaches are ideal for consideration of issues wherein substantial heterogeneity exists limiting the information content of conditional mean based analyses. [ABSTRACT FROM AUTHOR]
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- 2016
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12. Factors affecting adoption of improved management practices in the pastoral industry in Great Barrier Reef catchments.
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Rolfe, John and Gregg, Daniel
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WATER quality , *LANDOWNERS , *MONETARY incentives , *COST analysis - Abstract
Substantial efforts are being made by industry and government in Australia to reduce adverse impacts of pastoral operations on water quality draining to the Great Barrier Reef. A key target is to achieve rapid adoption of better management practices by landholders, but current theoretical frameworks provide limited guidance about priorities for improving adoption. In this study information from direct surveys with landholders in the two largest catchments draining into the Great Barrier Reef has been collected and analysed. Study outcomes have important implications for policy settings, because they confirm that substantial variations in adoption drivers exist across landholders, enterprises and practices. The results confirm that the three broad barriers to adoption of information gaps, financial incentives and risk perceptions are relevant. This implies that different policy mechanisms, including extension and incentive programs, remain important, although financial incentives were only identified as important to meet capital and transformational costs rather than recurrent costs. [ABSTRACT FROM AUTHOR]
- Published
- 2015
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13. He and Au ion radiation damage in sodalite, Na4Al3Si3O12Cl.
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Vance, Eric R., Gregg, Daniel J., Karatchevtseva, Inna, Davis, Joel, and Ionescu, Mihail
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HELIUM ions , *GOLD compounds , *RADIOLYSIS , *SODALITE , *SODIUM compounds , *X-ray diffraction - Abstract
Sodalite, a candidate ceramic for the immobilisation of pyroprocessing nuclear waste, showed no observable lattice dilatation in grazing incidence X-ray diffraction when irradiated with up to 1017 5 MeV He ions/cm². However micro-Raman scattering showed considerable spectral broadening characteristic of radiation damage near the end of the ~22 μm He range. Partial amorphism plus nepheline formation was observed in grazing incidence X-ray diffraction when sodalite was irradiated by 1016 12 MeV Au ions/cm². Nepheline appeared less susceptible to 12 MeV Au ion damage than sodalite, with ~25% less amorphous fraction at 1016 ions/cm². [ABSTRACT FROM AUTHOR]
- Published
- 2014
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14. Cation antisite disorder in uranium-doped gadolinium zirconate pyrochlores.
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Gregg, Daniel J., Zhang, Zhaoming, Thorogood, Gordon J., Kennedy, Brendan J., Kimpton, Justin A., Griffiths, Grant J., Guagliardo, Paul R., Lumpkin, Gregory R., and Vance, Eric R.
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ANTISITE defects , *URANIUM , *GADOLINIUM zirconate , *PYROCHLORE , *DOPING agents (Chemistry) , *X-ray powder diffraction - Abstract
The incorporation of uranium into gadolinium zirconate (Gd2Zr2O7) is investigated by synchrotron X-ray powder diffraction and X-ray absorption near-edge structure (XANES) spectroscopy. The results suggest that the uranium cation is largely located on the pyrochlore B-site instead of the targeted A-site. Cation disorder in Gd2Zr2O7 and U-doped Gd2Zr2O7 is investigated by positron annihilation lifetime spectroscopy (PALS) which demonstrates the absence of cation vacancies in these systems. This work provides direct evidence for cation antisite (A- and B-site mixing) disorder in U-doped and off-stoichiometric Gd2Zr2O7 pyrochlore. [ABSTRACT FROM AUTHOR]
- Published
- 2014
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15. Novel Chemical Synthesis and Characterization of CeTi206 Brannerite.
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Kong, Linggen, Gregg, Daniel J., Karatchevtseva, Inna, Zhang, Zhaoming, Blackford, Mark G., Middleburgh, Simon C., Lumpkin, Gregory R., and Triani, Gerry
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COMPLEX compounds synthesis , *CERIUM compounds , *BRANNERITE , *AQUEOUS solutions , *X-ray diffraction , *THERMAL analysis - Abstract
Cerium titanate CeTi2O6 was prepared by a new soft chemistry route in aqueous solution. A suite of characterization techniques, including X-ray diffraction, thermal analysis, vibrational spectroscopy, and scanning and transmission electron spectroscopy, were employed to S investigate the brannerite structure formation and its bulk properties. The J synthesized powder formed the brannerite crystal structure upon calcination at temperatures as low as 800°C. Samples sintered at 1350 °C possess a high level of crystallinity. X-ray absorption near-edge structure results indicate the presence of six-coordinated Ce4+ in the brannerite samples. [ABSTRACT FROM AUTHOR]
- Published
- 2014
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16. Ion beam irradiation effects in strontium zirconium phosphate with NZP-structure type.
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Gregg, Daniel J., Karatchevtseva, Inna, Thorogood, Gordon J., Davis, Joel, Bell, Benjamin D.C., Jackson, Matthew, Dayal, Pranesh, Ionescu, Mihail, Triani, Gerry, Short, Ken, Lumpkin, Gregory R., and Vance, Eric R.
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ION beams , *STRONTIUM compounds , *ZIRCONIUM phosphate , *CERAMIC materials , *RADIATION damage , *HELIUM ions , *METAL ions - Abstract
Abstract: Ceramics with the sodium zirconium phosphate or NZP type structure have potential as nuclear waste form and inert matrix materials. For both applications the material will be subjected to self-radiation damage from α-decay of the incorporated actinides. In this study, ion-beam irradiation using Au- and He-ions has been used to simulate the consequences of α-decay and the effects of irradiation on the structural and macroscopic properties (density and hardness) have been investigated. Irradiation by Au-ions resulted in a significant volume contraction of ∼7%, a reduction in hardness of ∼30% and a loss in long-range order at fluences above 1014 Au-ions/cm2. In contrast, little effect on the material properties was noted for samples irradiated with He-ions up to a fluence of 1017 ions/cm2. Thermal annealing was investigated for the highest fluence Au-ion irradiated sample and significant decomposition was observed. [Copyright &y& Elsevier]
- Published
- 2014
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17. The incorporation of neptunium and plutonium in thorutite (ThTi2O6).
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Zhang, Yingjie, Gregg, Daniel J., Lumpkin, Gregory R., Begg, Bruce D., and Jovanovic, Miodrag
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NEPTUNIUM , *PLUTONIUM compounds , *UNIT cell , *VALENCE (Chemistry) , *DOPING agents (Chemistry) , *X-ray diffraction , *SCANNING electron microscopy - Abstract
Highlights: [•] The incorporation of neptunium (Np) and plutonium (Pu) in thorutite (ThTi2O6) has been studied. [•] The effect of Np/Pu doping on the unit cell parameter changes has been discussed from the structure point of view. [•] The effect of Y as charge compensator to encourage the formation of higher valences of Np and Pu has been explored. [•] The resulting Np/Pu doped thorutite samples have been characterised by using XRD, SEM and DRS. [ABSTRACT FROM AUTHOR]
- Published
- 2013
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18. The incorporation of plutonium in lanthanum zirconate pyrochlore.
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Gregg, Daniel J., Zhang, Yingjie, Middleburgh, Simon C., Conradson, Steven D., Triani, Gerry, Lumpkin, Gregory R., and Vance, Eric R.
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PYROCHLORE , *PLUTONIUM , *LANTHANUM compounds , *SINTERING , *CHARGE exchange , *WAVENUMBER - Abstract
Abstract: The incorporation of plutonium (Pu) within lanthanum zirconate pyrochlore was investigated using air, argon, and N2–3.5%H2 sintering atmospheres together with Ca2+ and Sr2+ incorporation for charge compensation. The samples have been characterised in the first instance by X-ray diffraction (XRD), scanning electron microscopy (SEM) and diffuse reflectance spectroscopy (DRS). The results show Pu can be exchanged for La3+ on the A-site with and without charge compensation and for Zr4+ on the B-site. DRS measurements were made over the wavenumber range of 4000–19,000cm−1 and the Pu in all air- and argon-sintered samples was found to be present as Pu4+ while that in samples sintered in N2–3.5%H2 was present as Pu3+. The Pu valence was confirmed for three of the samples using X-ray near-edge absorption spectroscopy (XANES). Pu valences >4+ were not observed in any of the samples. [Copyright &y& Elsevier]
- Published
- 2013
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19. The thermophysical properties of calcium and barium zirconium phosphate.
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Gregg, Daniel J., Karatchevtseva, Inna, Triani, Gerry, Lumpkin, Gregory R., and Vance, Eric R.
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THERMOPHYSICAL properties , *CALCIUM phosphate , *BARIUM compounds , *CERAMIC metals , *NUCLEAR reactors , *THERMAL stability - Abstract
The thermophysical and structural properties of calcium and barium zirconium phosphate ceramics (CZP and BZP) have been investigated for their potential candidacy as actinide hosts for inert matrix fuels (IMF) in nuclear reactors. These phosphate ceramics, which can accommodate minor actinides as well as the resulting fission products, are found to be thermally stable to 1600°C in air, however they begin to decompose in an inert atmosphere above approximately 1400°C. The heat capacity, thermal conductivity and bulk thermal-expansion were measured from room temperature up to 1200°C. Structural changes in this temperature region as well as the anisotropic thermal-expansion behaviour were studied using high-temperature X-ray diffraction. A phase change from R-3 to R-3c was identified for Ba0.5Zr2(PO4)3 near 880°C. The thermal conductivity for these ceramics at 1000°C was found to be 1.0Wm−1 K−1, a relatively low thermal conductivity that was increased to 5.0Wm−1 K−1 at 1000°C for BZP:Ni (25:75 mass ratio) cermet composites. [ABSTRACT FROM AUTHOR]
- Published
- 2013
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20. Crystal chemistry and structures of uranium-doped gadolinium zirconates.
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Gregg, Daniel J., Zhang, Yingjie, Zhang, Zhaoming, Karatchevtseva, Inna, Blackford, Mark G., Triani, Gerry, Lumpkin, Gregory R., and Vance, Eric R.
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CRYSTAL structure , *URANIUM , *DOPING agents (Chemistry) , *GADOLINIUM zirconate , *X-ray diffraction , *PYROCHLORE - Abstract
Abstract: A series of uranium-containing gadolinium zirconate samples have been fabricated at 1450°C in oxidizing, inert and reducing atmospheres. X-ray diffraction, Raman spectroscopy and transmission electron microscopy have been utilized to confirm adoption of pyrochlore or defect fluorite structures. X-ray diffraction allowed determination of the bulk averaged structure while Raman spectroscopy and transmission electron microscopy were used to determine ordering at the microdomain scale. Diffuse reflectance, X-ray absorption near edge structure and X-ray photoelectron spectroscopies indicated a predominantly U6+ oxidation state for all the air-sintered samples, even when Ca2+ or A-site vacancies were incorporated to charge balance for U4+, a mixed U5+/U6+ oxidation state was found for samples sintered in argon, while a mixed U4+/U5+ oxidation state occurred for sintering under N2–3.5%H2. This demonstrates a degree of uranium oxidation state control through sintering conditions, and the potential of using gadolinium zirconates as host materials for uranium in nuclear waste applications. [Copyright &y& Elsevier]
- Published
- 2013
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21. Extending the Nitrogen-Heterosuperbenzene Family: The Spectroscopic, Redox, and Photophysical Properties of "Half-Cyclized" N-½HSB and Its Ru(Il) Complex.
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Gregg, Daniel J., Bothe, Eberhard, Höfer, Petra, Passaniti, Paolo, and Draper, Sylvia M.
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NITROGEN compounds , *RUBIDIUM , *INORGANIC chemistry , *CHEMISTRY , *DEHYDROGENATION - Abstract
Oxidative cyclodehydrogenation is an important process in the formation of the new graphene, N-½HSB 2. This heteropolyaromatic results from the FeCl3-catalyzed oxidative cyclodehydrogenation of 1,2-dipyrimidyl-3,4,5,6-tetra(4-tert-butylphenyl)benzene. Three new C-C bonds are formed that lock the two pyrimidines in a molecular platform comprising eight fused aromatic rings flanked by two remaining "uncyclized" phenyl rings. Mechanistically intriguing is the fact that N-HSB 1, the product of six C-C bond fusions, is co-synthesized with its "half-cyclized" daughter in this reaction. 1 and 2 have the same bidentate N-atom arrangement. This facilitates formation of the heteroleptic Ru(II) complexes, [Ru(bpy)2(2)](PF6)2 4 and [Ru(bpy)2(1)](PF6)2 3, which differ in the size and planarity of their aromatic ligands. The new ligand 2 and its complex 4 are characterized by ¹H NMR, IR, ESI-MS, and accurate mass methods. 2 exhibits photophysical properties that are consistent with a reduction of the π/π* framework, a concomitant increase in the energy of the LUMO, and a blue-shift of the solvent-dependent fluorescence (λem = 474 nm, ϕF = 0.55, toluene) as compared to its parent. Complex 4 absorbs throughout the visible region and borders on near-IR emitter character, exhibiting a slightly blue-shifted ³MLCT emission (868 nm, CH3CN) as compared to that of [Ru(bpy)2(1)](PF6)2 3 (880 nm, CH3CN). Electrochemical analyses permit further elucidation of the intermolecular interactions of 3 and 4. These and the concentration and temperature-dependent NMR spectra of 4 confirm it to be nonaggregating, a direct result of the two uncyclized and rotatable phenyl rings in 2. [ABSTRACT FROM AUTHOR]
- Published
- 2005
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22. Complexed Nitrogen Heterosuperbenzene: The Coordinating Properties of a Remarkable Ligand.
- Author
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Draper, Sylvia M., Gregg, Daniel J., Schofield, Emma R., Browne, Wesley R., Duati, Marco, Vos, Johannes O., and Passaniti, Paolo
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NITROGEN , *NONMETALS , *BIPYRIDINE , *BIPYRIDINIUM compounds , *ELECTROCHEMISTRY , *PHYSICAL & theoretical chemistry - Abstract
Tetra-peri-(tert-butyl-benzo)-di-peri-(pyrimidino)-cororiene 1, the parent compound of the nitrogen heterosuperbenzene family N-HSB, is employed as a novel monotopic ligand in the formation of [Pd(n3- C3H3)(1)]PF3 2 and [Ru(bpy)2(1)](PF6)2 (where bpy = 2,2′-bipyridine 3a and d8-2,2′-bipyridine 3b). These N-coordinated complexes are fully characterized by 1H NMR and IR spectroscopy and ESI-MS. Metal coordination has a profound effect on both the absorption and the emission properties of 1. Pd(ll) coordination causes a red-shift in the low-energy absorptions, a decrease in the intensity of the n-π absorptions, and a quenching of the emission. Ru(ll) coordination causes absorption throughout the visible region and creates two new complexes that join an elite group of compounds known as "black" absorbers. 3a and 3b possess two discernible 1MLCT bands. The one of exceptionally low energy (λmax = 615 nm) has an associated 3MLCT emission (λmax = 880 nm) due to the unprecedented electron delocalization and acceptor properties of the rigid aromatic N-HSB 1. Both Ru(ll) complexes are near-IR emitters with unusually protracted emission lifetimes of 320 ns at 77 K. They are photochemically inert, and their electrochemical properties are consistent with the presence of a low-lying π orbital on 1. The first two reversible reductions (E&frac;12 (CH3CN), -0.54 V, -1.01 V vs SCE) are due to the stepwise reduction of 1 and are anodically shifted as compared to [Ru(bpy)3]2+. Temperature- and concentration-dependent NMR studies on 2 and 3a suggest extensive aggregation is occurring in solution. [ABSTRACT FROM AUTHOR]
- Published
- 2004
- Full Text
- View/download PDF
23. Effect of Ti‐metal addition on hot‐isostatically pressed (HIPed) Synroc‐C.
- Author
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Farzana, Rifat, Dayal, Pranesh, Peristyy, Anton, Sutton, Phillip, Aly, Zaynab, Aughterson, Robert D., Nguyen, Thanh Ha, Yeoh, Michelle, Koshy, Pramod, and Gregg, Daniel J.
- Subjects
- *
ISOSTATIC pressing , *HOT pressing , *WASTE treatment , *FUEL cycle , *NUCLEAR fuels , *RADIOACTIVE wastes - Abstract
Synroc, a candidate nuclear wasteform and Synroc technology, a waste treatment solution utilizing hot‐isostatic pressing (HIPing) have significant potential for the immobilisation of challenging nuclear wastes from both current and innovative reactors and fuel cycles. Hot isostatic press (HIP) consolidation is undertaken within sealed metal HIP canisters, where metal buffers (e.g., Ti, Fe and Ni) can be incorporated to control the redox environment within the canister. This study, for the first time, reports the effect of varying Ti‐metal addition (0, 2, 4, and 8 wt.%) on phase formation, microstructural characteristics, and wasteform performance for HIP consolidated Synroc‐C containing 20 wt.% simulated PUREX type (PW‐4b) high level waste. Quantitative X‐ray diffraction analysis, scanning electron microscopy‐energy dispersive X‐ray spectroscopy (EDS) and transmission electron microscopy‐EDS analyses were undertaken for analytical investigations. The chemical durability of the samples was assessed using ASTM C1220‐21 standard test. Hot‐isostatically pressed (HIPed) samples with 0 and 8 wt.% Ti added for redox control produced unfavourable phase formation. However, the HIPed samples with Ti additions of 2 and 4 wt.% as a redox buffer showed the desired phase formation of Synroc‐C without any significant change to the partitioning of waste elements among the phases along with compatible durability results, when compared to previous literature for hot uniaxial pressing (HUPed) or sintered materials. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
24. Ion beam irradiation of ABO4 compounds with the fergusonite, monazite, scheelite, and zircon structures.
- Author
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Reyes, Massey, Aughterson, Robert D., Gregg, Daniel J., Middleburgh, Simon C., Zaluzec, Nestor J., Huai, Ping, Ren, Cuilan, and Lumpkin, Gregory R.
- Subjects
- *
ION bombardment , *SCHEELITE , *MONAZITE , *IRRADIATION , *CRITICAL temperature , *ZIRCON - Abstract
The effects of irradiation on CaWO4, SrWO4, BaWO4, YVO4, LaVO4, YNbO4, and LaNbO4 were investigated on thin crystals using 1.0 MeV Kr ions at 50‐1000 K. All of the ABO4 compounds can be amorphized with calculated damage cross sections (σa = 1/Fc0) in the range of ~0.30‐1.09 × 10‐14 cm2 ion−1 at zero Kelvin. The analysis of fluence‐temperature data returned critical temperatures for amorphization (Tc) of 311 ± 1, 358 ± 90, 325 ± 19, 415 ± 17, 541 ± 6, 636 ± 26, and 1012 ± 1 K, respectively, for the compounds listed above. Compared with previous in situ irradiation of ABO4 orthophosphate samples using 0.8 MeV Kr ions, the Tc values of LaVO4 and YVO4 are higher than those of LaPO4 and YPO4 by 82 K and 124 K, respectively. The Tc values of the three scheelite structures, CaWO4, SrWO4, and BaWO4, indicate that they are the most radiation tolerant compounds under these conditions. The A‐B cation anti‐site energies, EfAB, determined by DFT range from 2.48 to 10.58 eV and are highly correlated with the A‐B cation ionic radius ratio, rA/rB, but are not correlated with Tc across the different structure types, suggesting that the formation and migration energies of Frenkel defects play a more important role in damage recovery in these compounds. We also discuss the role of cation and anion charge/iconicity as determined by DFT. ABO4 compounds with the zircon structure and B = P or V have a distinct advantage over those with B = Si as the damaged regions do not appear to be significantly affected by polymerization of (PO4)3− or (VO4)3− groups which might stabilize the amorphous fraction and ultimately lead to phase separation as observed in zircon (ZrSiO4). [ABSTRACT FROM AUTHOR]
- Published
- 2020
- Full Text
- View/download PDF
25. Ceramic conversion and densification of zirconium phosphonate sorbent materials.
- Author
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Veliscek-Carolan, Jessica, Thorogood, Gordon J., Gregg, Daniel J., Tansu, Margaux, and Hanley, Tracey L.
- Subjects
- *
CONDENSED matter , *HEAT engineering , *HEATING load , *CERIUM group , *VENTILATION - Abstract
Abstract The simple conversion of zirconium phosphonate sorbent materials, with known affinity for lanthanide elements, to durable ceramic waste forms via thermal treatment has been demonstrated. The use of zirconium phosphonate enables both removal of targeted elements from spent nuclear fuel and immobilisation into leach resistant solid products to be achieved using a single material. Thermal conversion was performed on the zirconium phosphonate both before and after loading with europium, which acted as a surrogate for the chemically similar minor actinides. Without europium loaded, the zirconium phosphonate sorbent formed predominantly KZr 2 (PO 4) 3 upon heating, independent of the processing conditions used. A maximum relative density of 87% was achieved with cold isostatic pressing (200 MPa) and sintering at 1200 °C for 12 h. When the zirconium phosphonate sorbent was loaded with europium, the phase composition formed upon thermal treatment was more complex. Specifically, mixtures of ZrP 2 O 7 , Eu 0.33 Zr 2 (PO 4) 3 , EuPO 4 and Zr 2 O(PO 4) 2 were formed, with phase compositions depending on the temperatures and pressures used. The simplest phase composition for the europium loaded material was achieved via uniaxial pressing (120 MPa) and sintering at 1300 °C for 1 h, although the ceramic pellet produced under these conditions had a relative density of only 53%. The loaded europium deported primarily to a EuPO 4 phase, which is known to be highly stable and leach resistant. As such, these zirconium phosphonate materials have potential utility for treatment of nuclear wastes. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
26. Heterosuperbenzenes: A New Family of Nitrogen-Functionalized, Graphitic Molecules.
- Author
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Draper, Sylvia M., Gregg, Daniel J., and Madathil, Rethi
- Subjects
- *
BENZENE , *MOLECULES - Abstract
Examines the development of heterosuperbenzenes, a family of nitrogen-functionalized and graphitic molecules. Electrical and optoelectronic properties of heterosuperbenzenes; Introduction of heteroatoms into polyphenylene precursor; Establishment of a host of heterosuperbenzenes with intrinsic carbon–nitrogen frameworks.
- Published
- 2002
- Full Text
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27. A tribute to Eric Raymond (Lou) Vance: Ceramic materials physicist and nuclear wasteform expert – 15th November, 1942‐7th March, 2019.
- Author
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Finlayson, Trevor R., Franks, George V., and Gregg, Daniel G.
- Subjects
- *
RADIOACTIVE substances , *GLASS recycling , *NEUTRON irradiation , *SMALL-angle neutron scattering , *EARTH sciences , *NUCLEAR energy , *CERAMIC engineering , *CERAMIC materials - Published
- 2020
- Full Text
- View/download PDF
28. ChemInform Abstract: Novel Chemical Synthesis and Characterization of CeTi2O6 Brannerite.
- Author
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Kong, Linggen, Gregg, Daniel J., Karatchevtseva, Inna, Zhang, Zhaoming, Blackford, Mark G., Middleburgh, Simon C., Lumpkin, Gregory R., and Triani, Gerry
- Subjects
- *
TITANIUM , *AMMONIUM compounds , *X-ray diffraction , *SCANNING electron microscopy , *RAMAN spectroscopy , *CRYSTALLINITY - Abstract
The title compound is synthesized in aqueous medium from a mixture of titanium(IV) bis(ammonium lactato)dihydroxide and Ce(NO3)3 (sintering between 800 and 1400 °C). [ABSTRACT FROM AUTHOR]
- Published
- 2014
- Full Text
- View/download PDF
29. Technology Heterogeneity and Poverty Traps: A Latent Class Approach to Technology Gap Drivers of Chronic Poverty.
- Author
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Hill, Daniel, McWhinnie, Stephanie F., Kumar, Shalander, and Gregg, Daniel
- Subjects
- *
DIGITAL divide , *HETEROGENEITY , *POVERTY , *SOCIOECONOMIC factors , *HOUSEHOLDS - Abstract
The analysis of household wealth dynamic remains an important methodology in the identification of poverty traps. To overcome measurement issues in survey data, livelihoods-based approaches of the dynamics of poverty are typically examined using panel regressions of a livelihoods regression on household assets and other socio-economic factors over time. In this paper, we characterise the livelihoods regression as a 'livelihoods technology', and use a latent class-technology approach to account for heterogeneity in how households generate a livelihood. We use a detailed dataset from rural India covering 213 households across 2001–2014, and control for selection issues through a Heckman Selection model. Our results are the first in the wealth dynamics literature to show that substantial heterogeneity exists in the technologies with which households generate their livelihoods. Importantly, we show that accounting for heterogeneity in household livelihoods 'technologies' more readily identifies different equilibria in wealth levels and provides previously foregone information on who is poor and why they remain poor. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
30. Profiling hot isostatically pressed canister–wasteform interaction for Pu‐bearing zirconolite‐rich wasteforms.
- Author
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Dayal, Pranesh, Farzana, Rifat, Zhang, Yingjie, Lumpkin, Gregory R., Holmes, Rohan, Triani, Gerry, and Gregg, Daniel J.
- Subjects
- *
HOT pressing , *ISOSTATIC pressing , *SCANNING electron microscopy , *CERAMIC materials , *X-ray spectroscopy , *STAINLESS steel - Abstract
Zirconolite‐rich full ceramic wasteforms designed to immobilize Pu‐bearing wastes were produced via hot isostatic pressing (HIP) using stainless steel (SS) and nickel (Ni) HIP canisters. A detailed profiling of the elemental compositions of the major and minor phases over the canister–wasteform interaction zone was performed using scanning electron microscopy combined with energy‐dispersive X‐ray spectroscopy (SEM‐EDS) characterization. Bulk sample analyses from regions near the center of the HIP canister were also conducted for both samples using X‐ray diffraction and SEM‐EDS. The sample with the Ni HIP canister showed almost no interaction zone with only minor diffusion of Ni from the inner wall of the canister into the near‐surface region of the wasteform. The sample with the SS HIP canister showed ∼100–120 μm of interaction zone dominated by high‐temperature Cr diffusion from canister materials to the wasteform with the Cr predominantly incorporated into the durable zirconolite phase. We also examined, for the first time, changes to the HIP canister wall thickness caused by HIPing and demonstrated that no canister wall thinning occurred. Instead, in the areas examined, the canister wall thickness was observed to increase (up to ∼20%) due to the compression occurring during the HIP cycle. Further, only sparse formation of (Cr, Mn)‐rich oxide particles were noted within the HIP canister inner wall area immediately adjacent to the ceramic material, with no evidence for reverse diffusion of ceramic materials. Though the HIP canister–wasteform interaction extends to ∼120 μm when using an SS HIP canister for the system investigated, this translates to <<1 vol.% for an industrial scale HIPed wasteform. Importantly, the HIP canister–wasteform interactions did not produce any obviously less durable phases in the wasteform or had any detrimental impact on the HIP canister properties. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
31. Current advances on titanate glass-ceramic composite materials as waste forms for actinide immobilization: A technical review.
- Author
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Zhang, Yingjie, Kong, Linggen, Ionescu, Mihail, and Gregg, Daniel J.
- Subjects
- *
COMPOSITE materials , *WASTE products , *CERAMICS , *GLASS-ceramics , *RADIOACTIVE wastes , *CHEMICAL processes , *FUEL cycle - Abstract
A comprehensive review of the current advances on titanate glass-ceramic composite materials as waste forms for actinide immobilization is given. Apart from providing a comprehensive summary of earlier works in the field, some technical analysis and perspectives are provided pointing to the potential future studies. [Display omitted] • A comprehensive review on titanate glass-ceramic waste forms for actinide immobilization is provided. • Current advances on the titanate glass-ceramic composite materials are summarised. As the emerging versatile waste forms for immobilizing actinide-rich radioactive wastes, glass-ceramic composite materials based on some durable ceramic phases are being developed. They have apparent advantages over the conventional borosilicate glasses and multi- or single- phase ceramics as they essentially combine the chemical and processing flexibilities of glasses to accommodate processing impurities and excellent chemical durability of ceramic phases to host actinides. More recently, some new advances have been made on scientific and technological aspects including new glass-ceramic systems; improved understanding of ceramic phase evolution in glass; actinide validation studies and simplified processing techniques. This review is intended to cover the current advances on the development of glass-ceramic composite waste forms focusing on titanate ceramic phases (zirconolite, pyrochlore and brannerite) for immobilizing various actinide-rich radioactive wastes arising from the nuclear fuel cycle. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
32. Sodium zirconium phosphate‐based glass‐ceramics as potential wasteforms for the immobilization of nuclear wastes.
- Author
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Scales, Nicholas, Dayal, Pranesh, Aughterson, Robert D., Zhang, Yingjie, and Gregg, Daniel J.
- Subjects
- *
RADIOACTIVE waste disposal , *GLASS-ceramics , *RADIOACTIVE wastes , *WASTE treatment , *ZIRCONIUM , *WASTE management - Abstract
A comprehensive study on the development of sodium zirconium phosphate (NZP)‐based glass‐ceramic composites as potential wasteforms for the immobilization of nuclear wastes is reported. Two complementary waste treatment routes, the ex situ and in situ crystallisation of NZP with a sodium aluminoborosilicate glass, were investigated with various processing conditions including sintering temperature, cooling rate and NZP to glass ratios. While the ex situ route with mixing of pre‐made NZP and glass is a robust and reliable means of producing the glass‐ceramic composites, the in situ crystallisation of NZP from an amorphous NZP precursor is a more realistic processing route. The formation of ZrO2 as a minor phase was observed especially for high NZP to glass ratios due to the solubility difference between Zr and P oxides in glass. The addition of extra phosphate can overcome this and yield glass‐ceramic composites with appropriate NZP stoichiometry. Overall, the NZP glass‐ceramic system is versatile offering multiple processing options for nuclear waste management. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
33. Gd2Zr2O7 and Nd2Zr2O7 pyrochlore prepared by aqueous chemical synthesis.
- Author
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Kong, Linggen, Karatchevtseva, Inna, Gregg, Daniel J., Blackford, Mark G., Holmes, Rohan, and Triani, Gerry
- Subjects
- *
GADOLINIUM compounds , *PYROCHLORE , *AQUEOUS solutions , *CHEMICAL synthesis , *PRECIPITATION (Chemistry) , *METAL complexes , *ELECTRON diffraction - Abstract
Pyrochlore structured Gd2Zr2O7 and Nd2Zr2O7 are produced via complex precipitation processing. A suite of characterization techniques, including FTIR, Raman, X-ray and electron diffraction, TEM, SEM as well as nitrogen sorption are employed to investigate the structural and grain size evolution of the synthesized and calcined powder. Results show that Gd2Zr2O7 with the pyrochlore structure are produced after calcination at 1400°C for 12h while Nd2Zr2O7 has already formed the pyrochlore structure at 1200°C. This method allows the formation of dense materials at relatively low temperature, with bulk densities over 92% of the theoretical values achieved after sintering at 1400°C for 50h. This unique aqueous synthetic method provides a simple pathway to produce pyrochlore lanthanide zirconate without using either organic solvent and/or mechanical milling procedures, making the synthesis protocol an attractive potential scale-up production of highly refractory ceramics. [ABSTRACT FROM AUTHOR]
- Published
- 2013
- Full Text
- View/download PDF
34. Glass-bonded ceramic waste forms for immobilization of radioiodine from caustic scrubber wastes.
- Author
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Lere-Adams, Arumala J., Dixon Wilkins, Malin C., Bollinger, David, Stariha, Sarah, Farzana, Rifat, Dayal, Pranesh, Gregg, Daniel J., Chong, Saehwa, Riley, Brian J., Heiden, Zachariah M., and McCloy, John S.
- Subjects
- *
RADIOACTIVE wastes , *NUCLEAR activation analysis , *REACTOR fuel reprocessing , *IODINE isotopes , *ISOSTATIC pressing , *LIQUID waste , *CRUMB rubber - Abstract
Glass-bonded sodalite composite waste forms have been developed for the immobilization of liquid radioactive wastes resulting from off-gas treatment during aqueous reprocessing of used nuclear fuel, with a particular focus on 129I. The proposed composite waste form is comprised of aluminosilicate ceramic phases containing volatile radionuclides bonded with a glassy matrix. In this work, a suite of ten candidate low-temperature glass binders (ZnO-Bi 2 O 3 -based glasses and a Na 2 O-B 2 O 3 -SiO 2 glass) were examined. Six glasses were mixed with caustic scrubber waste simulant previously converted into a sodalite-rich material (to provide glass fractions of 10 and 20 wt.%), uniaxially pressed into pellets, and sintered at 350 °C or 550 °C for 8 h in air. Iodine retention after heat treatment was assessed by neutron activation analysis, showing retention of 67–100 % of expected iodine. The aqueous durabilities of the resulting materials were then determined, following the ASTM C1308 standard test, showing iodine releases of 1 to 23 g m−2 after 4 d. The cumulative iodine release for the best performing system (a zinc-bismuth-borate glass binder) was <1 g m−2, and its iodine retention from processing was 67 %. The iodine releases compared favorably with other waste forms. In parallel, this best-performing composition was also consolidated via hot isostatic pressing (HIP) in a stainless-steel canister at 550 °C for 2 h under 100 MPa pressure. The HIPed sample was produced at the ∼20 g scale and showed improved densification and minimal reaction with the canister. [ABSTRACT FROM AUTHOR]
- Published
- 2024
- Full Text
- View/download PDF
35. Characterisation of hot isostatically pressed (HIPed) hollandite wasteform-canister interaction zone.
- Author
-
Mann, Jodie, Farzana, Rifat, Aughterson, Robert D., Dayal, Pranesh, Sorrell, Charles C., Koshy, Pramod, and Gregg, Daniel J
- Subjects
- *
RADIOACTIVE wastes , *HOT pressing , *RADIOACTIVE waste disposal , *FOCUSED ion beams , *ISOSTATIC pressing , *TRANSMISSION electron microscopy , *STAINLESS steel , *TIN - Abstract
• Hollandite wasteform fabricated by HIP to immobilise Cs/Sr separated waste. • Phase formation and microstructures were identified at the interaction zone. • Hollandite incorporated minor HIP-canister chemistry at the interaction zone. • No deleterious phases were observed that would reduce wasteform performance. A potential hollandite wasteform for immobilising waste containing Cs, Ba, Sr, and Rb, projected from a solvent extraction process that separates Cs/Sr from spent nuclear fuel, was fabricated via hot isostatic pressing (HIPing) within a stainless-steel (SS) canister at 1250 °C / 30 MPa / 2 h. Before HIPing, 2 wt.% Ti metal was added to the precursor, as a redox control additive. Detailed elemental profiling and microstructural analysis at the interaction zone between the wasteform and the SS HIP canister were thoroughly investigated with transmission electron microscopy (TEM) using a lamella extracted by focused ion beam (FIB) milling, scanning electron microscopy (SEM) and X-ray diffraction (XRD). The interaction zone towards the wasteform was ∼20–30 µm in distance and in this region, a hollandite composition with varying chemistry was observed relative to the bulk wasteform. Moreover, the regular Cr-oxide layer, often observed previously for HIPed Synroc-type materials, was not present due to the achievement of reducing condition by adding Ti-metal as redox additive and simultaneous diffusion of canister material towards the ceramic. Predominant Cr-diffusion was observed with incorporation in the hollandite phase along with minor Fe, Mn and Co from the SS canister. This study provides a detailed understanding of the HIP canister – wasteform interaction zone for a hollandite-rich wasteform design for the first time. Importantly, no deleterious phases were formed that may otherwise reduce the performance of the wasteform. This study further demonstrates the flexibility of HIPing as a consolidation process for the treatment of radioactive wastes. [ABSTRACT FROM AUTHOR]
- Published
- 2024
- Full Text
- View/download PDF
36. Hot isostatic pressed pyrochlore glass‐ceramics: Revealing structure insides at the reaction interface.
- Author
-
Zhang, Yingjie, Wei, Tao, Xu, Alan, Dayal, Pranesh, and Gregg, Daniel J.
- Subjects
- *
ISOSTATIC pressing , *PYROCHLORE , *RADIOACTIVE waste disposal , *FOCUSED ion beams , *RADIOACTIVE wastes , *GLASS-ceramics , *HOT pressing - Abstract
As potential waste forms for immobilizing actinide‐rich radioactive wastes, Eu2Ti2O7 (Eu as a surrogate for minor actinides) pyrochlore glass‐ceramics were fabricated via hot isostatic pressing (HIPing) at 1200°C. The structure and microstructure at the reaction interface between the glass‐ceramic waste form and the stainless steel (SS) canister under HIPing conditions were carefully investigated with scanning electron microscopy (SEM), transmission electron microscopy (TEM), and synchrotron single crystal X‐ray diffraction (SC‐XRD). The interactions at the reaction interface led to the formations of a ~10‐µm‐thick Cr2O3 layer as the oxidation front of the SS and a layer of a mixed oxide phase (Eu1.25SiCr0.8Ti1.2O7.5) on the glass‐ceramic side of the reaction interface. The crystal structure of such a unique mixed oxide phase was revealed indubitably with a combination of synchrotron SC‐XRD and TEM assisted with a focused ion beam (FIB) SEM system. The improved structural understanding of the reaction interface will help to support the utilization of HIPing as a versatile hot consolidation process for the treatment of radioactive wastes. [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
- View/download PDF
37. Pyrochlore glass-ceramics for the immobilization of molybdenum-99 production wastes: Demonstrating scalability and flexibility to waste stream variance.
- Author
-
Farzana, Rifat, Zhang, Yingjie, Dayal, Pranesh, Aly, Zaynab, Holmes, Rohan, Triani, Gerry, Vance, Eric R., and Gregg, Daniel J.
- Subjects
- *
GLASS-ceramics , *PYROCHLORE , *ENERGY dispersive X-ray spectroscopy , *ISOSTATIC pressing , *REFLECTANCE spectroscopy , *SCALABILITY - Abstract
[Display omitted] Pyrochlore glass ceramics have been fabricated via in-situ crystallization under reducing conditions by both sintering and hot isostatic pressing (HIPing) as candidate wasteforms for the acidic waste biproduct of Mo-99 radiopharmaceutical production. The tailored wasteform demonstrates flexibility in the wasteform design to receive the required waste variability, it also suitably passes high-level waste performance requirement, and successfully scales to 1 kg scale with 45 wt.% waste loading. U-rich pyrochlore as the major phase was confirmed by X-ray diffraction, scanning electron microscopy and energy dispersive X-ray spectroscopy, with residual glass and minor secondary phases. The presence of both U4+ and U5+ valences in the wasteforms was revealed by diffuse reflectance spectroscopy. Addition of glass content had little influence on the pyrochlore composition but facilitated minor perovskite formation. The up-scaled dense, HIPed sample showed elemental releases of < 2 g/L for all elements in durability experiments. [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
- View/download PDF
38. A Novel Chemical Route to Prepare La2 Zr2 O7 Pyrochlore.
- Author
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Kong, Linggen, Karatchevtseva, Inna, Gregg, Daniel J., Blackford, Mark G., Holmes, Rohan, Triani, Gerry, and Vanderah, T.
- Subjects
- *
LANTHANUM , *AQUEOUS solutions , *PYROCHLORE , *ISOSTATIC pressing , *POWDER metallurgy , *ELECTRON diffraction - Abstract
Lanthanum zirconate has been prepared via a new chemical synthesis method by combining sol-gel processing and complex precipitation. The synthesis was carried out in aqueous solution under ambient conditions. The synthesized powder possessed the pyrochlore superstructure upon calcination above 1200°C. A suite of characterization techniques, including FTIR, Raman, X-ray and electron diffraction, TEM, SEM, and nitrogen sorption were employed to investigate the microstructural evolution and bulk properties. Dense ceramics (>90% relative density) were obtained after sintering at 1400°C, without need for additional processing (i.e., hot or cold isostatic pressing) or any milling steps. A mechanism has been proposed that elucidates molecular assembly of this chemical synthesis method. [ABSTRACT FROM AUTHOR]
- Published
- 2013
- Full Text
- View/download PDF
39. Pyrochlore glass‐ceramics fabricated via both sintering and hot isostatic pressing for minor actinide immobilization.
- Author
-
Zhang, Yingjie, Zhang, Zhaoming, Wei, Tao, Kong, Linggen, Kim, Young J., and Gregg, Daniel J.
- Subjects
- *
ISOSTATIC pressing , *HOT pressing , *PYROCHLORE , *CHEMICAL processes , *GLASS-ceramics , *TRANSPARENT ceramics - Abstract
Pyrochlore glass‐ceramics (GCs) have been investigated with samples fabricated via both sintering and hot isostatic pressing (HIPing) of a mixed oxide precursor. It has been demonstrated that sintering at 1200°C in air is necessary to obtain well‐crystallized pyrochlore crystals in a sodium aluminoborosilicate glass through a one‐step controlled cooling. The crystallization, structure, and microstructure of Eu2Ti2O7 pyrochlore as the major phases in residual glass were confirmed with X‐ray diffraction (XRD), scanning electron microscopy‐energy dispersive spectroscopy, transmission electron microscopy, and Raman spectroscopy. The structures of major Eu2Ti2O7 pyrochlore and minor [Eu4.67O(SiO4)3] apatite in both sintered and HIPed samples were refined using synchrotron XRD data. While the processing atmosphere did not appear to affect the cell parameter of the main pyrochlore phase, very small volume expansion (~0.3%) was observed for the minor apatite phase in the HIPed sample. In addition, static leaching of the HIPed sample confirmed that pyrochlore GCs are chemically durable. Overall, pyrochlore GCs prepared via both sintering and HIPing with the Eu partitioning factor of ~23 between ceramics and the residual glass are suitable waste forms for minor actinides with processing chemicals. [ABSTRACT FROM AUTHOR]
- Published
- 2020
- Full Text
- View/download PDF
40. Micro-compression testing of gold ion irradiated zirconolite glass-ceramics as nuclear waste forms.
- Author
-
Xu, Alan, Wei, Tao, Gregg, Daniel J., Vance, Eric R., Zhang, Yingjie, and Lumpkin, Gregory R.
- Subjects
- *
RADIOACTIVE wastes , *TRANSMISSION electron microscopes , *GLASS-ceramics , *IONS , *BIOCERAMICS - Abstract
The mechanical properties of zirconolite glass-ceramics designed for immobilising actinide-rich nuclear wastes, have been investigated through micro-compression tests pre and post 12 MeV gold ion irradiation at room temperature to a peak damage level of 100 displacements per atom (dpa). Whilst zirconolite crystals have become amorphized because of irradiation, transmission electron microscope analysis found no voids within the irradiated zirconolite. Nevertheless, voids of ∼25 nm in diameter were observed within the glass phase and appear to be homogeneously distributed. Surprisingly, micro-compression testing found the zirconolite glass-ceramic to exhibit a lower modulus, lower compression yield and greater toughness post irradiation. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
41. Objectives versus realities: Spatial, temporal, financial and social deficiencies in Australia's public revegetation investment model.
- Author
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Collard, Stuart J., O'Connor, Patrick J., Prowse, Thomas A. A., Gregg, Daniel, and Bond, Anthelia J.
- Subjects
- *
PUBLIC investments , *BIOTIC communities , *PRIVATE equity funds , *BIOLOGICAL extinction , *ENDANGERED species - Abstract
Summary: Past and continuing fragmentation and modification of ecosystems, as well as other threatening processes, cause ongoing biodiversity losses and species extinctions in Australia. At the same time as biodiversity declines, government funding for conservation and restoration is diminishing, leading to reduced action and greater reliance on private investment and community groups. In order to maintain and restore biodiverse ecosystems and the essential services they provide, both conservation of existing vegetation and habitat reconstruction are required. In this paper, we summarise the available data on planting area and cost from the Australian Government's 20 Million Trees programme (2014–2020), the largest recent national‐scale revegetation incentives programme in Australia. We find that the current spatial scale of effort and investment in habitat reconstruction is insufficient to match the scale required to meet national conservation objectives. Furthermore, the funding rate ($/ha) and contracting arrangements are inadequate for the establishment of high‐quality self‐sustaining vegetation needed for the recovery of Australia's threatened species and ecological communities. We estimate that the minimum amount of funding required for habitat reconstruction is at least five times higher than is provided for current national flagship programmes such as 20 Million Trees. We provide recommendations, designed to assist future habitat reconstruction programmes achieve their long‐term biodiversity objectives. [ABSTRACT FROM AUTHOR]
- Published
- 2020
- Full Text
- View/download PDF
42. Uranium brannerite with Tb(III)/Dy(III) ions: Phase formation, structures, and crystallizations in glass.
- Author
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Zhang, Yingjie, Wei, Tao, Zhang, Zhaoming, Kong, Linggen, Dayal, Pranesh, and Gregg, Daniel J.
- Subjects
- *
TERBIUM , *URANIUM , *URANIUM oxides , *CRYSTALLIZATION , *PHASE equilibrium , *IONS , *HEAT treatment , *GLASS-ceramics - Abstract
Uranium brannerite phases with terbium(III) or dysprosium(III) ions have been investigated. The precursors with molar ratio of 0.5:0.5:2 (Ln: U: Ti with Ln = Tb or Dy) were prepared and calcined at 750°C in argon. Sintering the pelletized samples in argon at 1200°C led to the formation of pyrochlore phases with TiO2 rutile and U‐rich oxides while sintering in air led to the formation of brannerite phases with the nominal composition close to Ln0.5U0.5Ti2O6 together with trace amounts of TiO2 rutile and LnUO4. Incorporating an excess of TiO2 (20 wt%) and sintering at higher temperature (1300°C) resulted in no obvious change to the phase equilibrium. As designed, pentavalent uranium has been proven to be dominant in these brannerite phases with diffuse reflectance spectroscopy. The relationships between the cell parameters and the ionic radii of the A‐site cations have been explored and rationalized from the structure point of view for a range of titanate brannerite phases (ATi2O6). In addition, the crystallization of Ln0.5U0.5Ti2O6 brannerite in glass has been achieved via heat treatment at 1200°C and confirmed with X‐ray diffraction, scanning electron microscopy‐energy dispersive spectroscopy and transmission electron microscopy–selected area electron diffraction. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
43. Surface evolution and radiation damage of a zirconolite glass-ceramic by Au ion implantation.
- Author
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Wei, Tao, Zhang, Yingjie, Xu, Alan, Gregg, Daniel J., Karatchevtseva, Inna, Kong, Linggen, Ionescu, Mihail, and Vance, Eric R.
- Subjects
- *
ION implantation , *PARTICLE accelerators - Abstract
Abstract Ion implantation using particle accelerators is a promising avenue to emulate the property-controlling microstructures created in nuclear materials. In the present study, the 21 MeV Au ion implantations with fluence up to 1 × 1015 ion/cm2 have been conducted on the surface of a zirconolite glass-ceramic. The microstructure modifications on the surface have been investigated by X-ray diffraction, Raman spectrometry, scanning electron microscopy and transmission electron microscopy. The amorphous behavior of the crystalline zirconolite and the structural change in the glassy phase has been identified subject to different fluences. The amorphization of zirconolite crystals occurred on the surface of sample subjected to 1 × 1014 ion/cm2 and the deformation of glass and zirconolite crystals near the surface were observed at the fluence of 1 × 1015 ion/cm2. Highlights • Au ion implantation using accelerator on a zirconolite glass-ceramic to emulate the radiation effect • Amophization behavior of zirconolite crystal subject to 21 MeV Au implantation • Structural changes in glass up to the fluence of 1 × 1015 ion/cm2 [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
44. Hot isostatically pressed Y2Ti2O7 and Gd2Ti2O7 pyrochlore glass-ceramics as potential waste forms for actinide immobilization.
- Author
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Wei, Tao, Zhang, Yingjie, Kong, Linggen, Kim, Young Jip, Xu, Alan, Karatchevtseva, Inna, Scales, Nicholas, and Gregg, Daniel J.
- Subjects
- *
ISOSTATIC pressing , *GLASS-ceramics , *ACTINIDE elements , *PYROCHLORE , *RADIOACTIVE wastes , *CRYSTALLIZATION - Abstract
Graphical abstract Both Y 2 Ti 2 O 7 and Gd 2 Ti 2 O 7 pyrochlore glass-ceramics have been prepared with a typical oxide route and consolidated via hot isostatic pressing, and characterized as potential waste forms for the immobilization of actinide-rich radioactive wastes. Abstract Both Y 2 Ti 2 O 7 and Gd 2 Ti 2 O 7 pyrochlore glass-ceramics (GCs) have been prepared with an oxide route and consolidated via hot isostatic pressing (HIPing) as waste forms for actinide immobilization. The crystallization of Y 2 Ti 2 O 7 /Gd 2 Ti 2 O 7 pyrochlore as the major actinide host phase in the residue glass has been confirmed with XRD, SEM-EDS and Raman spectroscopy. The static leaching tests confirmed that both GCs are chemically durable with normalized Y/Gd and Ti leach rates ∼10−4–10-5 g m-2 d-1 after 28 days. In addition, the interactions between the 316L stainless steel (SS) HIP-can and the GCs have been investigated. Interactions occur at the interface with a layer of mixed Cr/Ti oxide and CrTi 2 O 5 crystals observed for the Y 2 Ti 2 O 7 GC and a layer (∼10 μm) of Cr 2 O 3 observed for the Gd 2 Ti 2 O 7 GC as the reaction fronts from the SS cans. Furthermore, a layer (∼10 μm) of Gd-(Si/Ti)-oxide phase formed on the GC side of the interface. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
45. Durability of hot uniaxially pressed Synroc derivative wasteform for EURO-GANEX wastes.
- Author
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Hsieh, Yun-Hao, Humphry-Baker, Samuel A., Horlait, Denis, Gregg, Daniel J., Vance, Eric R., and Lee, William E.
- Subjects
- *
WASTE management , *DURABILITY , *TITANATES , *SYNROC , *SURFACE roughness , *PEROVSKITE , *MICROSTRUCTURE - Abstract
A new titanate wasteform, Synroc-Z, was developed to contain minimal host phases for actinides and thus better suit the EURO-GANEX process. The processing conditions, waste loading and surface roughness were varied, and their effects on wasteform durability and microstructure were examined. Hot uniaxial pressing temperature was the most important factor in controlling density (<0.5 vol% porosity) and phase composition. Synroc-Z was found to have similar aqueous durability to Synroc-C. Leached samples formed Ti-oxide films and crystals on their surfaces as found by other researchers. At low waste loadings (<20 wt%), Synroc-Z showed slightly poorer durability performance than Synroc-C owing to its greater perovskite content (30 vs. 20 wt% respectively). However, at 35 wt% waste loading, Synroc-Z maintained its durability performance. This result is explained by the higher volume fraction of buffer phase, rutile, which allows greater flexibility for waste loading. [ABSTRACT FROM AUTHOR]
- Published
- 2018
- Full Text
- View/download PDF
46. Immobilization of iodine via copper iodide.
- Author
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Vance, Eric R., Grant, Charmaine, Karatchevtseva, Inna, Aly, Zaynab, Stopic, A., Harrison, Jennifer, Thorogood, Gordon, Wong, Henri, and Gregg, Daniel J.
- Subjects
- *
IODINE , *NUCLEAR reactors , *MICROSTRUCTURE , *NANOPARTICLES , *SINTERING - Abstract
CuI is a candidate wasteform for the immobilization of the fission product 129 I. CuI can be made simply by the addition of CuCl to an I − bearing solution such that exchange of Cl − with I − takes place. The CuI material can then be consolidated into a wasteform by sintering at approximately 550 °C in argon or by hot isostatically pressing at 550 °C with 100 MPa of pressure. A waste loading of greater than 60 wt.% is achievable with good water leach resistance, in keeping with the low solubility product of CuI. However, like the well known wasteform candidate AgI, CuI decomposes in water containing metallic Fe. To compensate this deficiency, the sintered CuI wasteform can be further protected by surrounding it by Sn powder and HIPing at the low temperature of 200 °C. [ABSTRACT FROM AUTHOR]
- Published
- 2018
- Full Text
- View/download PDF
47. Development of brannerite glass-ceramics for the immobilization of actinide-rich radioactive wastes.
- Author
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Zhang, Yingjie, Kong, Linggen, Karatchevtseva, Inna, Aughterson, Robert D., Gregg, Daniel J., and Triani, Gerry
- Subjects
- *
RADIOACTIVE wastes , *ENCAPSULATION (Catalysis) , *GLASS-ceramics , *ACTINIDE elements , *BRANNERITE , *PLUTONIUM - Abstract
Brannerite-based glass-ceramics have been developed as potential waste forms for the immobilization of actinide-rich radioactive wastes. For the first time, the formation of brannerite phases in glass has been demonstrated using uranium (U) and plutonium (Pu) with additions of gadolinium and hafnium as neutron absorbers. Both XRD and SEM- EDS confirm that brannerite is the dominating phase with compositions close to Y0.5U0.5Ti2O6, Gd0.2Pu0.3U0.5Ti2O6, and Gd0.1Hf0.1Pu0.2U0.6Ti2O6 internally crystallized in the glass. TEM SAED and Raman spectroscopy reveal the typical structure and vibration modes for brannerite. In addition, the presence of U5+ species as designed in the formulations has been confirmed by diffuse reflectance spectroscopy. More importantly, the U and Pu were partitioned exclusively in the ceramic phases with no detectable actinide in the glass. [ABSTRACT FROM AUTHOR]
- Published
- 2017
- Full Text
- View/download PDF
48. Novel synthesis and thermal property analysis of MgO–Nd2Zr2O7 composite.
- Author
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Kong, Linggen, Zhang, Ji, Maeda, Yoshitaka, Blackford, Mark G., Li, Sean, Triani, Gerry, and Gregg, Daniel J.
- Subjects
- *
MAGNESIUM oxide , *METALLIC composites , *THERMAL properties of metals , *SELF-propagating high-temperature synthesis , *TRANSMISSION electron microscopy , *X-ray diffraction - Abstract
MgO-Nd 2 Zr 2 O 7 composites with ratios of 50–70 vol% MgO were produced via a one-pot combustion synthesis. A suite of characterization techniques, including X-ray diffraction, scanning and transmission electron microscopy were employed to investigate the structural properties while dilatometry, simultaneous thermal analysis and laser flash analysis were used to characterize the thermal properties of the composites. Dense pellets were produced after sintering at 1400 °C with grain sizes between 200 and 500 nm for both phases. The thermal properties of the composites are similar to those produced using standard methods. The composite with 70 vol% MgO was found to have the highest thermal conductivity below 1000 °C, while above this temperature the thermal conductivity was found to be similar and independent of MgO content. This novel synthesis route produces materials which show significant improvements in homogeneity with smaller particle sizes when compared to current standard synthesis techniques without significantly reducing thermal conductivity. [ABSTRACT FROM AUTHOR]
- Published
- 2016
- Full Text
- View/download PDF
49. Structural and phase evolution in U3Si2 during steam corrosion.
- Author
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Liu, Jiatu, Burr, Patrick A., White, Joshua T., Peterson, Vanessa K., Dayal, Pranesh, Baldwin, Christopher, Wakeham, Deborah, Gregg, Daniel J., Sooby, Elizabeth S., and Obbard, Edward G.
- Subjects
- *
NEUTRON diffraction , *DENSITY functional theory , *CRYSTAL grain boundaries , *RIETVELD refinement , *NUCLEAR fuels , *ULTRACOLD molecules - Abstract
U 3 Si 2 nuclear fuel is corroded in deuterated steam with in situ neutron diffraction. Density functional theory is coupled with rigorous thermodynamic description of the hydride including gas/solid entropy contributions. H absorbs in the 2 b interstitial site of U 3 Si 2 H x and moves to 8 j for x ≥ 0.5. Hydriding forces lattice expansion and change in a/c ratio linked to site preference. Rietveld refinement tracks the corrosion reactions at 350–500 °C and preference for the 8 j site. Above 375 °C, formation of UO 2 , U 3 Si 5 and USi 3 take place in the grain boundaries and bulk. Hydriding occurs in bulk and precedes other reactions. [Display omitted] • In situ neutron diffraction measures U 3 Si 2 corrosion in deuterated steam. • Rigorous thermodynamic description of hydride using key entropy contributions. • H absorption at 2 b interstitial site of U 3 Si 2 H x , moves to 8 j site for x ≥ 0.5. • From 350 °C, U 3 Si 2 H x fragmented by 1–2% anisotropic lattice expansion. • From 375 °C, UO 2 , U 3 Si 5 and USi 3 form in bulk and in grain boundaries. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
50. The incorporation of Li2SO4 into barium borosilicate glass for nuclear waste immobilisation.
- Author
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Farzana, Rifat, Dayal, Pranesh, Karatchevtseva, Inna, Aly, Zaynab, and Gregg, Daniel J.
- Subjects
- *
BOROSILICATES , *GLASS waste , *RADIOACTIVE wastes , *GLASS transition temperature , *BARIUM , *BARIUM oxide , *LEACHING - Abstract
• A glass wasteform was designed for Mo-99 production Li 2 SO 4 -rich wastes. • Incorporation of 2.78 wt% SO 3 was achieved in the glass melted at 1200 °C. • At low temperature an immiscible layer of BaSO 4 and Na 2 SO 4 formed. • Formation of Na 2 SO 4 lowered the sulphur incorporation rate compared of BaSO 4. • PCT leach values showed satisfactory aqueous durability as glass wasteform. This study has systematically investigated the effect of Li 2 SO 4 addition (2.75 −16.5 wt%) in barium borosilicate glass, to provide a pathway to optimise the glass composition and maximise sulphate incorporation. The work also provides a mechanistic understanding as to how SO 4 2- is incorporated within the glass structure. The highest sulphate incorporation of 2.78 wt% SO 3 (from 11 wt% Li 2 SO 4 addition) was achieved without crystallisation following melting at 1200 °C. Sulphate incorporation in glass was confirmed by XRF, ICP, EDS and Raman analysis. Addition of Li 2 SO 4 along with sodium and barium oxides improved the sulphate incorporation by mixed alkali network depolymerisation and the larger Ba cations helped to create sufficient space within the boron-silicate network to incorporate sulphate ions into the glass. An immiscible sulphate layer rich in BaSO 4 and Na 2 SO 4 formed on top of the glass at lower temperature (800–1100 °C) and subsequent diffusion of Na, Ba oxides and sulphur from this layer increased with increasing time and temperature to form a sulphate incorporated amorphous glass. Addition of Na 2 O played an important role to improve sulphate incorporation in the glass, as well as formation of an immiscible layer on top of the glass however, the formation of Na 2 SO 4 lowered the sulphur incorporation rate at high temperature compared to BaSO 4. Increasing the Li 2 SO 4 content in the glass decreased the glass transition temperature. Aqueous durability testing using the standard PCT tests indicated the glass had satisfactory aqueous durability compared to benchmark environmental assessment glass. This study provides opportunities to convert Li+ and SO 4 2- rich nuclear wastes into appropriate glass wasteforms. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
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