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University of Southampton Research Repository Eprints Soton 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 Faculty of Natural and Environmental Sciences Ocean and Earth Science Assessing the Use of Non-Traditional Stable Isotopes as Tracers of Weathering Processes: with Evidence from the Southern Alps, South Island, New Zealand by Sarah L. Wright Thesis for the degree of Doctor of Philosophy April 2015 i ii UNIVERSITY OF SOUTHAMPTON Abstract Faculty of Natural and Environmental Sciences, Ocean and Earth Science Doctor of Philosophy by Sarah L Wright Concentrations of carbon dioxide (CO2) in the Earth’s atmosphere have increased by >100 ppm since pre-industrial times due to the burning of fossil fuels for energy and it is now clear that the consequent warming of the climate system will have widespread impacts on human and natural systems. Chemical weathering of silicate rocks draws down CO2 from the atmosphere, but the significance of this process and the mechanisms which control weathering rates remain poorly constrained. New information with regards to chemical weathering processes, linkages to physical denudation rates, and the effects of certain rock types on global chemical budgets, are all required. This study utilises elemental concentrations together with lithium (δ7Li) and magnesium (δ26Mg) isotopic values of river waters and weathering products to determine the parameters that regulate weathering in a terrestrial environment, and assesses the influence of progressive metamorphism, glacial activity, rainfall patterns, rapid tectonic uplift, climate and geothermal fluid flow. Samples were collected from the Southern Alps on South Island, New Zealand. The Southern Alps represent a relatively pristine environment and a natural laboratory to examine the climatic and tectonic controls on chemical weathering of a largely lithologically homogenous metasilicate terrane with minor metamorphic carbonate, in a temperate, maritime environment. Chemical weathering and atmospheric CO2 consumption rates, calculated from riverine elemental data, demonstrate that CO2 consumed by silicate weathering is relatively low compared to rivers globally. High overall chemical weathering rates (3.1 x 107 g·km-2·yr-1 in the west vs. 1.8 x 107 g·km-2·yr-1 in the east) are associated with high uplift and erosion rates, and high rainfall on the western side of the Southern Alps, where chemical erosion of metamorphic carbonates is more prevalent. However, higher rates of atmospheric CO2 consumption due to silicate weathering were found on the eastern side of the Southern Alps (6.4 x 104 mol·km-2·yr-1 in the west vs. 7.7 x 104 mol·km-2·yr-1 in the east), where uplift and erosion rates are lower. This indicates that uplift accelerates weathering rates of metamorphic carbonates, but has little effect of rates of silicate weathering, which regulates CO2 drawdown from the atmosphere on long timescales. The mechanisms that moderate Li and Mg isotopic fractionation in the Southern Alps were thoroughly investigated. Protolith lithology and metamorphic grade have little effect upon the δ7Li and δ26Mg composition of the bedrock. Secondary clay formation (e.g. illite, kaolinite and smectite) during weathering is the dominant process by which Li and Mg isotope fractionation occurs, and climate only has an indirect influence. The residence time of water-rock interaction imposes an important control upon the δ7Li composition of rivers. However, the effect of this control upon the δ26Mg composition of rivers is less clear. The evidence for coupling between riverine δ7Li and δ26Mg values during chemical weathering is weak with respect to results from this study and global studies. This suggests that the behaviour of these isotopes varies between different weathering environments, adding to the complexity of extrapolating local studies to global interpretations. iii iv Declaration of Authorship I, Sarah L. Wright declare that this thesis titled, ‘Assessing the Use of Non-Traditional Stable Isotopes as Tracers of Weathering Processes: with Evidence from the Southern Alps, South Island, New Zealand’ and the work presented in it are my own and has been generated by me as the result of my own original research. I confirm that: 1. This work was done wholly or mainly while in candidature for a research degree at this University. 2. Where any part of this thesis has previously been submitted for a degree or any other qualification at this University or any other institution, this has been clearly stated. 3. Where I have consulted the published work of others, this is always clearly attributed. 4. Where I have quoted from the work of others, the source is always given. With the exception of such quotations, this thesis is entirely my own work. 5. I have acknowledged all main sources of help. 6. Where the thesis is based on work done by myself jointly with others, I have made clear exactly what was done by others and what I have contributed myself. 7. None of this work has been published before submission. Signed: ................................................................................................................................ Date: .................................................................................................................................... v vi Acknowledgements Firstly, I would like to thank Rachael James for being such a supportive supervisor over the past 3 and a half years. She has been a great teacher and mentor, and my writing style has forever changed for the better. This project has given me invaluable knowledge and experience in geochemistry, which I would not have been able to obtain were it not for advice and help given by Rachael and many others that I would like to thank below. This project was made possible by Damon Teagle, who I have known since my undergraduate degree at the University of Southampton. My interest in the South Island, New Zealand, was first sparked by Damon with my Masters Project, and I have thoroughly enjoyed studying this area ever since. I would like to say a big thank you to Catriona Menzies for all her help and support over the years. Her advice, both scientific and non-scientific, has been instrumental in helping me develop this thesis. I would also like to thank the people who made the analysis of my samples possible, which include Andy Milton, Matt Cooper, Agnes Michalik and Ross Williams. I would also like to thank Chris Pearce for his advice with method development. I would like to thank Carolyn Graves, Cathy Cole, Jessy Klar, Heather Goring-Harford and David Reading for being amazing office mates that I have had the pleasure of knowing over the years. Anything from discussing data to having a moan about the Neptune was invaluable and probably helped me keep my sanity. Finally, I would like to thank my family and friends for all of their support. I would like to thank Tim, Mum, Dad, Mark, Carina, Steve, Ange, Karl, Sabrina, Hannah, Fran, and all of my other friends that have helped support me over the last few years. vii viii Table of Contents Abstract… ................................................................................................................................... iii Declaration of Authorship ...........................................................................................................v Acknowledgements ................................................................................................................... vii Table of Contents ....................................................................................................................... ix List of Figures .............................................................................................................................xv List of Tables ............................................................................................................................ xix Chapter 1 . ....................................................................................................................................1 1.1 Rationale ..............................................................................................................................1 1.2 Weathering and the Carbon Cycle .......................................................................................2 1.3 Present-day CO2 Consumption by Weathering of Silicate Rocks .......................................4 1.4 Assessing the Links Between Silicate Weathering and Climate .........................................5 1.5 What Controls Chemical Weathering Rates? ......................................................................6 1.5.1 Lithology................................................................................................................6
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