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Partitioning of Sr and Cs in Nuclear Fuel Storage Ponds Partitioning of 90Sr and 137Cs in Nuclear Fuel Storage Ponds A thesis submitted to the University of Manchester for the degree of Doctor of Philosophy in the Faculty of Science and Engineering. 2017 Hollie Ashworth School of Chemistry Table of Contents List of Figures .................................................................................................................. 8 List of Tables ................................................................................................................. 11 List of Equations ........................................................................................................... 12 List of Abbreviations and Acronyms .......................................................................... 13 Abstract .......................................................................................................................... 15 Declaration ..................................................................................................................... 16 Copyright Statement ..................................................................................................... 16 Acknowledgements ....................................................................................................... 17 1. Introduction ........................................................................................................... 18 1.1. Research Outline ............................................................................................................ 18 1.2. Thesis Structure .............................................................................................................. 19 1.3. Collaborator Contributions ........................................................................................... 19 1.4. Nuclear Power in the UK – An Overview .................................................................... 21 1.5. Principles of Nuclear Power .......................................................................................... 22 1.5.1. Fission of 235U ........................................................................................................... 22 1.5.2. The Uranium Fuel Cycle ........................................................................................... 23 1.6. UK Radioactive Waste ................................................................................................... 24 1.7. Sellafield .......................................................................................................................... 26 1.7.1. Magnox Reactors ...................................................................................................... 27 1.7.2. The First Generation Magnox Storage Pond (FGMSP) ............................................ 27 1.8. References ....................................................................................................................... 29 2. Literature Review ................................................................................................. 31 2.1. Scope of Review .............................................................................................................. 31 2.2. FGMSP Chemistry ......................................................................................................... 31 2.3. The Solid-Liquid Interface ............................................................................................ 33 2.3.1. Colloids ..................................................................................................................... 35 2.3.1.1. Colloid Stability ................................................................................................. 36 2.4. Adsorption at a Surface ................................................................................................. 38 2.4.1. Chemisorption ........................................................................................................... 39 2.4.2. Physisorption ............................................................................................................. 39 2.4.3. Adsorption Isotherms ................................................................................................ 40 2.4.4. Extended Sorption-Desorption Processes ................................................................. 40 3 2.4.5. The Distribution Coefficient, Kd ............................................................................... 41 2.5. Strontium ......................................................................................................................... 42 2.6. Caesium ........................................................................................................................... 43 2.7. Investigations on Pond Sludge Samples ....................................................................... 43 2.8. Brucite and Corroded Magnox Sludge (CMS) ............................................................ 44 2.8.1. Radionuclide Sorption to Brucite and CMS Simulants ............................................. 47 2.9. Other Hydroxide Phases ................................................................................................ 47 2.10. Uranium Phases ............................................................................................................ 48 2.10.1. UO2 and Oxidative Dissolution ............................................................................... 49 2.10.1.1. Influence of Radioactive Decay ....................................................................... 50 2.10.1.2. Influence of Carbonate .................................................................................... 50 2.10.1.3. Influence of pH ................................................................................................. 50 2.10.2. UO3 and Other U(VI) Phases ................................................................................... 50 2.10.3. Uranium Colloids .................................................................................................... 51 2.10.4. Radionuclide Sorption to Uranium Phases ............................................................. 52 2.11. Organic Molecules ........................................................................................................ 54 2.11.1. Humic Substances ................................................................................................... 54 2.11.2. Radionuclide Sorption to Humic Substances .......................................................... 56 2.11.2.1. Strontium-Humics ............................................................................................ 56 2.11.2.2. Caesium-Humics .............................................................................................. 57 2.11.3. Cyanobacteria .......................................................................................................... 57 2.12. Literature Summary .................................................................................................... 58 2.13. References ..................................................................................................................... 59 3. Aims ........................................................................................................................ 65 4. Methodology and Analytical Techniques ........................................................... 66 4.1. Experimental Approaches ............................................................................................. 66 4.1.1. Safety ......................................................................................................................... 66 4.1.2. CO2-free Glovebox .................................................................................................... 66 4.1.3. N2 Glovebox .............................................................................................................. 66 4.1.4. Sorption ..................................................................................................................... 67 4.1.5. Desorption ................................................................................................................. 69 4.1.6. Experimental Errors .................................................................................................. 69 4.1.7. Terminology .............................................................................................................. 69 4.2. Analytical Techniques .................................................................................................... 70 4.2.1. PHREEQC Modelling ............................................................................................... 70 4.2.2. Scanning Electron Microscopy (SEM) ..................................................................... 70 4.2.3. Liquid Scintillation Counting (LSC) ......................................................................... 71 4 4.2.4. Ultraviolet-Visible (UV-Vis) Spectroscopy .............................................................. 72 4.2.5. Inductively Coupled Plasma (ICP) Techniques ........................................................ 73 4.2.5.1. Atomic Emission Spectroscopy (AES) ................................................................ 74 4.2.5.2. Mass Spectrometry (MS) .................................................................................... 75 4.2.6. Laser Induced Breakdown Spectroscopy (LIBS) ...................................................... 75 4.2.7. X-Ray
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