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Thermal Treatment of Fuel Residues and Problematic Nuclear Wastes

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Thermal Treatment of Fuel Residues and Problematic Nuclear Wastes Thermal Treatment of Fuel Residues and Problematic Nuclear Wastes Sean Thomas Barlow BSc(Hons) MInstP MINCOSE Supervisors: Professor Neil C. Hyatt Professor Russell J. Hand Dr. Claire L. Corkhill Dr. Martin C. Stennett A thesis submitted in fulfilment of the requirements for the degree of Doctor of Philosophy Alternative Format Thesis Immobilisation Science Laboratory Department of Materials Science and Engineering The University of Sheffield May 2019 I II Abstract Problematic nuclear wastes and fuel residues plague the nuclear industry worldwide. In this Thesis thermal treatment is demonstrated through the development of various simulated nuclear wasteforms and surrogate materials from a variety of nuclear waste topics. Development of vitreous wasteforms for the treatment of intermediate level Magnox sludge from the Storage Ponds at Sellafield is discussed in this Thesis with both low activity uranium and surrogate materials. Magnesium borosilicate glasses were found to have comparable durability with current UK high level waste (HLW) glass whilst incorporating the whole spectrum of waste anticipated into a single composition. Highly metallic feeds could be incorporated into the wasteform with no adverse effects on the dissolution of such samples. If implemented, this composition could result in a 25% volume reduction in waste to be disposed saving approximately £82 million compared to the current baseline plan. Ascertaining the long-term integrity and safety of fuel residues arising from nuclear meltdowns, such as the Chernobyl and Fukushima accidents, through thermal synthesis of low activity simulants is explored in this Thesis. Two simulant Chernobyl ‘lava-like’ fuel containing materials (LFCM) were developed recreating the typical morphology and microstructure found in real samples, including a World first to successfully document formation of Chernobylite from a glass melt whilst aqueous durability was analogous to that of UK borosilicate HLW glass. Investigating how thermal treatment of americium waste built-up in stockpiles of civil plutonium is outlined in this Thesis. A novel cerium niobite, a simulant for americium, was synthesised with the crystal structure and suitability as a wasteform assessed. One potential use for an americium ceramic could be as a power source in a radioisotope thermoelectric generator (RTG); however it was determined an Am structured niobite for this application would be unsuitable, due to the phase transformation this material exhibited at elevated temperatures. This work opens avenues for further research on other potential materials. III Acknowledgements Reflecting on the past four or so years of my research at Sheffield, I am reminded of what a great learning environment this has been, academically, socially and professionally. Completion of this Thesis has been journey that has taken me across the globe, meeting many new friends and finding me a career I enjoy. Getting to the completion of this Thesis has not been a solo exercise however, a significant number of people have assisted in varying ways along the journey and whom which I would like to give thanks. To my supervisor Professor Neil Hyatt, without whom this research would not have been realised, I give my sincerest thanks for your determination and belief in me, to aid in my development as a scientist and now engineer. Thank you for providing both the independence and support required in my research and for being such a committed and dedicated supervisor. To Professor Russell Hand, Dr Claire Corkhill and Dr Martin Stennett, thank you for all your imparted knowledge and project support. The contributions you’ve made to both my development as a scientist and this work are profound. Thank you for all discussions on glass science Russell, dissolution science Claire and all things-laboratory based Martin. Thanks must also be given to the staff at the University of Sheffield’s Department of Materials Science and Engineering in general; be it administrative, financial or technical support they have been on hand to help. I am reminded of the support given by Dr. Lisa Holland for glass melting advice and support as well as Dr Nik Reeves for XRD and crystallographic refinement support. An acknowledgement is also given to Dr Heath Bagshaw at the University of Manchester and Dr Emma McCabe from the University of Kent for support in data collection and analysis. Importantly I would like to thank EPSRC for their financial support to this research through the Nuclear FiRST DTC programme at both the University of Manchester and University of Sheffield. Additional funding support was provided by the MRS2017 Student Scholarship Award, Margaret Elizabeth Lee Fellowship and Institute of Physics Student Conference Fund for which considerable thanks is given. My time at Sheffield has been invigorated and made one of the most enjoyable times of my life by fellow course-mates and friends from both the Nuclear FiRST DTC and ISL groups, with our weekly pub trips, meals out, walks in the peaks and giving me an international outlook on life. In no particular order, I would like to thank Colleen, Daniel C, Sebastian, Seddon and Michael from my DTC cohort, along with Michal, Shishir, Adam, Dilwar, James, Daniel B, Tannagorn, Joe, Marco and Xinyuan for being such awesome office buddies and providing important breaks from studying though activities such as climbing, swimming, squash, hiking, eating and drinking. Wetherspoons anyone? IV To Natcha, thank you for being by my side this past year. Your kindness and joyous spirit have been a constant source of energy to draw upon in time of need. Your contribution to this Thesis is through your loving support for me. To my parents Stuart and Christine, thank you for making me the person I am today. You have been my bedrock; loving and supporting me in all my ambitions, your contribution is more than can be expressed in words. To my siblings Daniel, James and Sarah-Jane, you have shared with me your joy, laughter and fun times supporting me to see this work through to completion for which I am eternally grateful. V Conferences, Papers, Presentations, Outreach & Professional Training Publications • Sean Barlow and Michael Kirkham, The building blocks of education. Nuclear Future, Vol. 11 (1), 2015, pp. 61–63. • S. T. Barlow, M. C. Stennett, R. J. Hand, S. P. Morgan, and N. C. Hyatt, Thermal Treatment of UK Magnox Sludge. Proceedings of the 2nd Petrus-OPERA PhD and Early Stage Researcher Conference, 2016, pp. 19–22. • S. T. Barlow, D. J. Bailey, A. J. Fisher, M. C. Stennett, C. L. Corkhill and N. C. Hyatt, Synthesis of simulant ‘lava-like’ fuel containing materials (LFCM) from the Chernobyl reactor Unit 4 meltdown. MRS Advances, Vol. 2 (11), 2016, pp. 609-614. doi:10.1557/adv.2016.642 • Sean T. Barlow, Daniel J. Bailey, Adam J. Fisher, Martin C. Stennett, Clemence Gausse, Claire L. Corkhill, Viktor A. Krasnov, Sergey Yu. Sayenko and Neil C. Hyatt, Synthesis, characterisation and corrosion behaviour of simulant Chernobyl nuclear meltdown materials. npj Materials Degradation, submitted on 02/04/19. Conferences Attended • Nuclear FiRST DTC Winter School, Buxton Palace Hotel, UK, 08/01/2014-10/01/2014. • Joint Nuclear CDTs Winter School, Birmingham Crown Plaza Hotel, UK, 06/01/2015- 08/01/2015. • Thermal Treatment Symposium 2015, Warrington, UK, 15/01/2015. • Farewell to Magnox, Wylfa, UK, 28/10/2015. • EPSRC Fission & Fusion Symposium, Manchester, UK, 14/12/2015. • Joint Nuclear CDTs Winter School, Birmingham Royal Angus Hotel, UK, 06/01/2016- 08/01/2016. • ESRC Nuclear Futures Seminar, Sheffield Halifax Hall, UK, 27/01/2016-28/01/2016. • ESRC Nuclear Futures Seminar, Sheffield Leopold Hotel, UK, 06/04/2016-07/04/2016. • 2nd Petrus-OPERA PhD and Early Stage Researcher Conference 2016, Delft University of Technology, Netherlands, 27/06/2016-01/07/2016. • Society of Glass Technology Centenary Conference, Sheffield, UK, 04/09/16-08/09/16 (Chaired session on Waste Vitrification). • MRS Fall 2016 Meeting and Exhibit, Boston, Massachusetts, USA, 27/11/2016- 02/12/2016 • Joint Nuclear CDTs Winter School, St Johns Hotel Solihull, UK, 04/01/2017-06/01/2017 • Institute of Physics Nuclear Industry Group, The Centre at Birchwood Park, Warrington, UK, 28/09/2017 VI • Scientific Basis for Nuclear Waste Management XLI, Sydney, Australia, 29/10/2017- 03/11/2017 Presentations • Thermal Treatment of Magnox Sludge by Immobilisation in Borosilicate Glass (poster) – Joint Nuclear CDTs Winter School, 08/01/2015. • Glass formulations for thermal treatment of Magnox sludges (poster) – Thermal Treatment Symposium, 15/01/2015. • Thermal Treatment of Magnox Sludge ILW (poster) – EPSRC Fission & Fusion Symposium, 14/12/2015. • Thermal Treatment of Magnox Sludge Intermediate Level Waste (oral) – Joint Nuclear CDTs Winter School, 07/01/2016. • Thermal Treatment of UK Magnox Sludge (oral) – 2nd Petrus-OPERA PhD and Early Stage Researcher Conference 2016, 27/06/2016. • Glass formulations for Magnox Sludge Immobilisation (oral) – Society of Glass Technology Centenary Conference, 06/09/2016. • Glass formulations for Thermal Treatment of UK Magnox Sludge Waste (oral) – MRS Fall 2016 Meeting and Exhibit, 30/11/2016 • Synthesis of Simulant Lava-Like Fuel Containing Materials from the Chernobyl Nuclear Disaster (oral) – MRS Fall 2016 Meeting and Exhibit, 30/11/2016 • Simulant Lava-Like Fuel Containing Materials from the Chernobyl Disaster (oral) – Joint Nuclear CDTs Winter School, 04/01/2017 • From Magnox to Chernobyl: A report on clearing-up problematic nuclear waste (Invited Speaker) – Institute of Physics Nuclear Industry Group, 28/09/2017 • Thermal Treatment of Magnox Sludge Intermediate Level Nuclear Waste through Vitrification (oral) – Scientific Basis for Nuclear Waste Management XLI, 31/10/2017 • Synthesis and characterisation of rare Ce3NbO7 compounds for use as nuclear space batteries by neutron powder diffraction and X-ray absorption spectroscopy (oral) – Scientific Basis for Nuclear Waste Management XLI, 01/11/17 Outreach • Meet the Scientist, Museum of Science and Industry, Manchester, 02/08/2014. • Science Spectacular 2014, University of Manchester, Manchester, 25/10/2014.
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