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Quantifying the Climate and Air Quality Impacts of Non-CO2 Species

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Quantifying the Climate and Air Quality Impacts of Non-CO2 Species Quantifying the climate and air quality impacts of non- CO2 species from the combustion of standard and alternative fuels in aviation Zarashpe Zarir Kapadia Submitted in accordance with the requirements for the degree of Doctor of Philosophy as part of the Integrated PhD with MSc in Low Carbon Technologies November 2015 Doctoral Training Centre in Low Carbon Technologies, Energy Research Institute, School of Chemical and Process Engineering, University of Leeds and School of Earth and Environment, University of Leeds and School of Civil Engineering ii Declaration of authorship The candidate confirms that the work submitted is his own, except where work which has formed part of jointly-authored publications has been included. The contribution of the candidate and the other authors to this work has been explicitly indicated below. The candidate confirms that appropriate credit has been given within the thesis where reference has been made to the work of others. Work from Chapters 4, 5 and 6 of this thesis appears in publication as follows: Kapadia, Z. Z., Spracklen, D. V., Arnold, S. R., Borman, D. J., Mann, G. W., Pringle, K. J., Monks, S. A., Reddington, C. L., Benduhn, F., Rap, A., Scott, C. E., Butt, E. W., and Yoshioka, M.: Impacts of aviation fuel sulfur content on climate and human health, Atmos. Chem. Phys. Discuss., 15, 18921-18961, doi:10.5194/acpd-15-18921-2015, 2015 The candidate, Zarashpe Zarir Kapadia, was responsible for the development of aviation emissions inventories, simulations, data interpretation, interpretation of work within the publication. The candidate wrote the manuscript with guidance from the co-authors. The contributions of the other authors was as follows: A. Rap and C. E. Scott performed calculations of ozone radiative, aerosol direct radiative and aerosol cloud albedo effects. E. W. Butt developed the mortality impacts code, and aviation emissions were integrated in to GLOMAP-mode with the assistance of K. J. Pringle, S. A. Monks and D. V. Spracklen. G. W. Mann, K. J. Pringle and C. L. Reddington helped set up the nitrate-extended version of the TOMCAT-GLOMAP-mode coupled model. This copy has been supplied on the understanding that it is copyright material and that no quotation from the thesis may be published without proper acknowledgement. The right of Zarashpe Zarir Kapadia to be identified as Author of this work has been asserted by him in accordance with the Copyright, Designs and Patents Act 1988. © 2015 The University of Leeds and Zarashpe Zarir Kapadia iii iv Acknowledgements Firstly I would like to thank my supervisors: Dominick Spracklen, Steve Arnold, Duncan Borman and Paul Williams. For without their invaluable support, advice, guidance, time and feedback over the past years this work and thesis would not have been possible, and for the opportunities and enthusiasm they have provided over the years. I would also like to thank Piers Forster for the support, guidance and opportunities he has provided me with. I would like to thank Kirsty Pringle, Graham Mann, Catherine Scott, Carly Reddington and Sarah Monks for all their assistance and time helping me get set-up on TOMCAT-GLOMAP-mode, the nitrate-extended version of this model, and simulation processing codes. The Aerosol Modellers and BAG (Biosphere Atmosphere Group) research groups for their feedback, and Richard Rigby for his invaluable IT support. I would like to thank the management committee of the Doctoral Training Centre in Low Carbon Technologies (DTC in LCT) for providing me with this opportunity. Paul Williams, James McKay, David Haynes, Eleanor Barham, Rachael Brown and Emily Bryan-Kinns for all their help, support, and for providing the DTC with an encouraging environment. Being part of the DTC in LCT I have also been privileged to meet some amazing people working on a range of interesting projects feeding in to the topic of low carbon technologies, while making some very good friends along the way. You are all too numerous to mention, but I’ll give it try... Jayne Windeatt, Gemma Brady, Ramzi Cherad, David Wyatt and Philippa Usher from my cohort, we have certainly been on a journey together – you guys have been amazing! Karaoke?... Tom Lynch, Shemaiah Weekes, (Aunty) Philippa Hardy, Sam Pickard, Hannah James and Gillian Harrison for all your pearls of wisdom and World Food nights. Catherine Scott for being a great friend and fake sister, Jayne Windeatt there’s no better way to sum you up than “you all round star!” – Thank you two for your invaluable friendship and advice. Sam Pickard for the care packages, advice and food discussions, and Edward Butt. Emma Tetstall the toughest running partner ever. Annabel Lea, Andrew Logue and Dwit Mehta who have provided much needed breaks away from work. Thom Best a great flatmate and friend, Andrew Dixon, David “Davey-J” Jacques, quiz and food guru Joanne Robinson, Berlin and fitness guru Paula McNamee for our coffee breaks and fun chats, James Gooding, Clare Linton and the otter aficionado Holly “Alfredo” Edwards for all your support and advice, and to the rest of you all – thank you. Thank you all for making this memorable and enjoyable time; one that I will never forget. v I also would like to mention some of my friends away from university; Bijan Talei Faz for all the advice and entertainment, Dahlia Revah, Matthew Cave, Sam Grove and Daniel Ivatt for all the encouragement, and helping me make the decision to back to University. Almost finally I would like to thank some people, who in my eyes, are stars of the pre-higher education process: John Pickering who helped me overcome my barriers with maths and helped me realise my abilities; and Stephen Persaud who always had faith in my skills and always pushed me to see to realise them, despite my resistance to Chemistry. Finally I would like to thank my mum, dad and brothers who have been there for me throughout this journey. Especially my parents for their endless support through all my endeavours, the much needed sanity checks, and for leading by example – thank you. Oh, I expect you two have pretended to have read this! vi Abstract Aviation has the capacity to drive changes in atmospheric composition, and therefore climate and air quality, increasing human mortality through increases in cases in cardiopulmonary disease. Non-CO2 aviation emissions are estimated to have a considerable effect on the climate, and with rapid growth in the aviation sector their associated impacts could increase. There is much uncertainty surrounding the climatic impact of aviation-induced ozone and aerosols, in part due to broad range of emissions species emitted, which are not always reported in aviation emissions inventories. This thesis assesses the impact of aviation on atmospheric trace gas and aerosol concentrations, climate, air quality and human health effects for year 2000 civil aviation. These impacts are estimated through: (i) the development of an extended aviation emissions inventory, inclusive of speciated hydrocarbons; (ii) assessing the atmospheric and climatic impact from aviation based on an extend aviation emissions inventory, a comparison of these impacts with a reduced emissions aviation emissions inventory, along with a sensitivity study for emissions species included; (iii) assessing the impact of aviation on human health effects when variations in fuel sulfur content (FSC) are applied along with resulting impacts on radiative effects, and; (iv) the atmospheric, climatic, air quality and human health impacts of the use of alternative fuels in aviation. An aviation emissions inventory was developed to represent aviation-borne non-CO2 emissions: nitrogen oxides, carbon oxide, speciated hydrocarbons, sulfur dioxide, black carbon and organic carbon emissions while taking in to account the geometric mean diameter of carbonaceous particles released. Aviation non-CO2 emissions are assessed to result in a radiative effect of –13.29 mW m-2 [assessed from the ozone (O3DRE) and aerosol (aDRE) direct radiative effects, and aerosol cloud albedo effect (aCAE)], primarily driven by a cooling aCAE. In comparison an emissions inventory which only considers aviation nitrogen dioxide and black carbon emissions results in a radiative effect of –8.19 mW m-2 primarily driven by reductions in the cooling aCAE assessed. It is found that air pollution from aviation reaches ground level, as such modifying surface PM2.5 (particulate matter within the 2.5 µm size range) which results in increased human exposure. Standard aviation is estimated to result in 3597 mortalities a-1. Variations in FSC from 0–6000 ppm aviation’s human health effects range from 2950–9057 mortalities a-1. These -2 variations in FSC result in an aviation non-CO2 radiative effect ranging from –6.08 mW m to – 75.48 mW m-2. It is found that variations in aviation FSC elicit a near-linear relationship vii between aviation-induced mortality and non-CO2 radiative effect. Additional investigations in the vertical release of aviation-borne sulfur dioxide emissions show that it possible to reduce aviation-induced mortality and increase aviation-induced cooling by adjusting the FSC of fuel used at different altitudes. An investigation of the use of Fischer-Tropsch (FT) and fatty acid methyl ester (FAME) fuels (FT50, FT100, FAME20 and FAME40 fuel blends) within aviation found that aviation-induced nitrogen dioxide and ozone concentrations were reduced in tandem with associated ozone radiative effects. Additionally due relative reductions between sulfur dioxide and carbonaceous aerosol emissions FT fuel blends were estimated to produce negative aDREs, while FAME fuel blends gave a positive aDRE. In all cases FT and FAME fuel blends decreased the aCAE induced cooling effect from aviation. FT50 is the only fuel blend currently specified for use in today’s civil aviation fleet. This fuel blend is simulated to reduce aviation’s non-CO2 emissions cooling radiative effect to –10.89 mW m-2 and reduce aviation-induced mortality by 460 mortalities a-1.
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