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University of Southampton Research Repository ePrints Soton Copyright © and Moral Rights for this thesis are retained by the author and/or other copyright owners. A copy can be downloaded for personal non-commercial research or study, without prior permission or charge. This thesis cannot be reproduced or quoted extensively from without first obtaining permission in writing from the copyright holder/s. The content must not be changed in any way or sold commercially in any format or medium without the formal permission of the copyright holders. When referring to this work, full bibliographic details including the author, title, awarding institution and date of the thesis must be given e.g. AUTHOR (year of submission) "Full thesis title", University of Southampton, name of the University School or Department, PhD Thesis, pagination http://eprints.soton.ac.uk University of Southampton THE MIGRATION AND ACCUMULATION OF RADIONUCLIDES IN THE RAVENGLASS SALTMARSH, CUMBRIA, UK December 1999 A thesis submitted for the degree of Doctor of Philosophy Jung-Suk Oh (BSc, MSc) Faculty of Science School of Ocean and Earth Science Southampton Oceanography Centre ABSTRACT Profiles of 241Am, 137Cs, 238Pu, 239240pu & 24lPu have been studied in four cores collected from the Ravenglass saltmarsh, Cumbria and one core collected from the Irish Sea, near the effluent pipeline of the Sellafield nuclear reprocessing plant. Major and trace elements have also been measured to look at the effects of sediment composition and any redox controls on element redistribution. In addition, almost one hundred surface scrape samples were collected from the Ravenglass saltmarsh and the same radionuclides were measured to study the lateral distribution of radionuclides. Three of the Ravenglass cores have well preserved the of Sellafield history discharge since the plant became operational in 1952. There are no significant post depositional and processes redox changes for all the cores studied. However, one of the saltmarsh cores collected from the front of the marsh shows that surface erosion has occurred. Surface results scrape sample also show that erosion is a significant which process results in the redistribution of sediments within the marsh. The core collected from the Irish Sea adjacent to the effluent pipeline shows sediment mixing has operated and these mixed sediments are the main source of material to the saltmarsh. Using the Sellafield records from discharge 1952 onwards, sediment mixing rates have been estimated a mathematical using simple model and they are inferred to be between 80 % and 90 %. ratios of Isotopic Pu isotopes have been compared to those estimated ratios corresponding to particular sediment rates and show mixing good agreement up to 30 cm below the surface. There is less correlation between Sellafield discharge ratios and measured ratios in cores below 30 cm and this be due to unreliable may discharge data or more likely the advective redistribution of material in the saltmarsh. A contribution of 241Am originating from the of 24IPu decay in cores was determined. The ingrown 241Am contributes significantly to the total 241Am measured. Based on the Sellafield discharge record, it is estimated that 46 approximately % of total 24IAm in the system has originated from the of 241Pu from decay discharged the plant since 1952. Spatial distribution of radionuclides in the saltmarsh Ravenglass is controlled by sediment accumulation associated with tidal inundation frequency and the clay content in the sediments. Surface erosion also plays a major role in redistributing saltmarsh sediment labelled with older Sellafield discharge within the marsh together with the sediments originated from the River Esk. ACKNOWLEDGMENTS I would like to acknowledge the guidance and help of Dr. Ian Croudace, Dr. Phillip Warwick and Dr. Arthur Sanchez this during project. They are not only my supervisors but also good friends. I also thank Mrs. Sonia Bryant (formerly of the Geosciences Advisory Unit) and Mrs. Wink Janes in every aspect while I was in the Geology Department (Sadly, it does not exist anymore). Dr. Rex Taylor, Dr. Andy Milton, Dr. Andy Cundy, Mr. Frank and Mr. Thorsten Wigley Warneke have me with provided every help I needed while I was carrying out this There project. are some Koreans I would like to thank for their wonderful friendship. Dr. Ki-Hong Shin, Mr. Young-Seog Kim, Mr. Kyu-Yong Choi & Mr. Jae-Kyoon are those Koreans Kang always willing to drink a of couple pints with me whenever I was happy or depressed. I am also grateful to my parents for their financial assistance, and grandmother and two lovely sisters for their encouragement. In addition, the support from and my parents-in-law my wife's two sisters and a brother is also very appreciated. All my friends in Korea working hard in their have areas given me motivation to pursue the PhD. Finally, special thanks to veiy my wife, Ok-Kyung, who always encouraged and supported me in all aspects. She devoted herself to look after three kids (?), me and our lovely two children, Sang-Hoon & Seung-Yeon. Without her support, I would not have completed this project. Radionuclides 4-c ^i^} ^$3 *i 1 *<I4-S. AJ-4 -S.^ ^-f ^4 -& ^H i-i-l 4^J *li S4 4) 4 (Dr. Ian Croudace, Dr. Phil Warwick & Dr. Arthur Sanchez) *fl 4^d #4 4 ^^4 ^-4^ ^^-f i^ > ^"4 J5Le.3Ä^M4. Geosciences Advisory Unit ^ Mrs. Sonya Bryant, Mrs. Wink Janes, Dr. Andy Cundy JlzJji TCP-MS LAB^ Dr. Andy Milton, TIMS LAB^ Dr. Rex Taylor, ^1 1] 1H i*! 4-^4^ tzi Frank, Thorsten, J-r-f <fl ) ^-2. v^ Southampton^ 4. -fH-l- ^4 4^-^ i t^ ^ 4-1 >i-foM #- -J- id, 4^4 ^4A> 4-i-f 4 ^ t> 4^-f 44 4 4 4 CONTENTS 1. Introduction 1 1.1. Introduction to the study 1 1.2. Aims of the study 4 1.3. Background information to the study 5 1.3.1. Radionuclides of interests in this study 5 1.3.1.1.241Am 5 1.3.1.2.137Cs 7 1.3.1.3. Plutonium isotopes 8 1.3.2. Distribution coefficients (Kj) 10 1.3.3. Behaviour of 137Cs in saline and freshwater environment 11 1.3.4. Behaviour of redox sensitive elements 12 1.3.5. a for Establishing chronology the marshes 14 1.3.5.1.210Pb method 15 1.3.5.2. The use of artificial radionuclides in dating 16 1.3.6. Estuaries 17 1.3.7. Saltmarshes 18 1.3.8. and Transportation interaction of Sellafield radionuclides 19 1.3.9. Bioturbation 20 2. Areas under investigation 22 2.1. Overview of study area 22 2.1.1. Sellafield site 22 2.1.2. Nuclear fuel reprocessing at Sellafield 25 2.1.3. Fate of radionuclides following discharge to the Irish Sea 28 2.2. Ravenglass saltmarsh 31 3. Sampling locations and methods used for the research 32 3.1. Sampling locations 32 3.2. Gamma spectrometry 3 5 3.3. XRF analysis 36 3.3.1. Bead preparation 3 6 3.3.2. Pellet preparation 3 6 3.4. Separation of plutonium 37 3.4.1. Introduction 37 3.4.2. Experimental 38 3.5. Determination of 241Pu in sediments 41 3.5.1. Introduction 41 3.5.2. Experimental 44 4. Results 47 4.1. Core samples 47 4.1.1. Major and trace element results in cores 47 4.1.2. Radionuclide results in cores 49 4.2. Surface scrape samples 57 4.2.1.241Am and I37Cs activities in surface scrape samples (1980 and 1997) 57 4.2.2.238Pu, 239'240Pu and 241Pu activities in surface scrape samples (1997) 57 5. Evaluation of sediment mixing 61 5.1. Introduction to sediment m ixing 61 5.2. Determination of the sediment mixing using core results 65 5.3. Conclusions 70 6. Irish Sea sediments 71 6.1. Major and trace element data 71 6.2. Vertical distribution of radionuclides 71 6.3. Pu ratios in the isotopic core 73 6.4. 241Am from Ingrown the decay of 241Pu 77 6.5. Conclusions 79 7. Vertical variation of radionuclides in the Ravenglass saltmarsh 80 7.1. and Major trace element data 80 7.2. Sediment accumulation rates in the saltmarsh 83 7.3.210Pb for dating R-96-007 core 85 7.4. Erosion of the saltmarsh 86 7.5. Vertical distribution of radionuclides in saltmarsh cores 87 7.6. Variations in Pu isotopic ratios in saltmarsh cores 92 7.7. of 241Pu Implication activities in saltmarsh cores 94 7.8. Conclusions 96 8. Spatial variations across the Ravenglass saltmarsh 97 8.1. Spatial distribution of radionuclides in the saltmarsh in 1980 and 1997 97 8.2. Variations in Pu ratios in isotopic 1997 surface scrape samples 103 8.3. Erosion of the saltmarsh 106 8.4. Loss on ignition data 107 8.5. Conclusions 109 9. Overall conclusions 110 10. References 112 Appendices 128 A. 1. Details of collected cores 128 A.2. methods Analytical 128 A.2.1. and Sampling storage 128 A.2.2. Sample preparation 128 A.2.3.210Pb determination 129 A.2.4. of Pu Electrodeposition & U 130 A.2.5. Detection limits in routine XRF analysis using a Rh anode X-ray tube 131 A.3. Geochemical data, 1-96-002 (subtidal) core 132 A.4. Geochemical data, R-96-000 (saltmarsh) core 133 A.5. Geochemical data, R-96-007 (saltmarsh) core 135 A.5.1. X-radiograph of core R-96-007 137 A.6. Geochemical data, R-96-008 (saltmarsh) core 138 A.7. Geochemical data, R-97-003 (saltmarsh) core 140 A.8.1. Cumulative activities of 241Am with various mixing rates 142 A.8.2.
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