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Thesis Style Document Application of Membrane Technologies in Water Purification Junjie Shen Submitted for the degree of Doctor of Philosophy Heriot-Watt University School of Engineering and Physical Sciences Institute of Chemical Sciences Edinburgh, United Kingdom May 2016 The copyright in this thesis is owned by the author. Any quotation from the thesis or use of any of the information contained in it must acknowledge this thesis as the source of the quotation or information. Abstract The world is facing a serious water crisis due to rapid population growth, industrialization and climate change. Water purification using membrane technologies provides a promising solution to address this problem. This thesis investigated the feasibility of membrane technologies in a wide range of applications covering drinking water purification and wastewater treatment. Target contaminants included fluoride, natural organic matter (NOM), emerging contaminants bisphenol A (BPA) and cimetidine, and the waterborne parasite Cryptosporidium. The first part of the thesis explored the solute- solute interactions of fluoride and humic substances (HS) in order to understand the behaviour of fluoride in natural water and during membrane filtration processes. It is shown that, at low pH and high ionic strength, fluoride ions are temporarily trapped inside the structure of HS aggregates. The second part of the thesis examined the feasibility of nanofiltration (NF) and reverse osmosis (RO) in treating challenging natural waters in Tanzania containing high fluoride and NOM concentrations, with the aim to increase the availability of drinking water sources. Fluoride retention was found to be dependent on ionic strength and recovery, which was predominantly due to a solution-diffusion mechanism. NOM retention was independent of water matrices but was governed by a size exclusion mechanism. NOM was observed to have a positive impact on fluoride removal. The third part of this work evaluated the on-site performance of a pilot-scale renewable energy powered membrane system in remote areas under varying solar conditions. While the technology is well established, the adaptation to remote areas is far from achieved. The system used in this study reliably produced high-quality drinking water despite of solar fluctuations. This area requires further work in terms of integration, technology adaptation and operation and maintenance schemes. The last part of the thesis reported the development of a series of novel photocatalytic polymers and tested their capabilities in removing wastewater contaminants. The photoactive polymers were highly capable of degrading BPA and cimetidine, as well as inactivating Cryptosporidium. These are very promising materials for simultaneous decontamination and disinfection of wastewater. The results obtained from this thesis provide new insights into solute-solute interactions, solute transport mechanisms, decentralized membrane system and novel membrane materials, which are hoped to contribute to advancements in current membrane technologies. i Acknowledgements Foremost, I would like to express my deepest gratitude to my two academic supervisors, Dr Valeria Arrighi and Professor Martin McCoustra, for your invaluable guidance and support throughout my PhD. Valeria, you have always encouraged me to find my own path but also provided wise advice when I felt lost. Your philosophy of never forcing but suggesting suits me perfectly. You have managed to fire fight my worries, concerns and anxieties, and helped me develop confidence in both myself and my work. Martin, when I desperately needed a new supervisor to save my PhD, you came on board and connected me with Valeria. Your deep insights and prompt feedback have benefitted me greatly. Both of you have been steady hands to steer me through to the end. My PhD studentship was provided by Energy Technology Partnership (ETP) with Drinking Water Quality Regulator for Scotland (DWQR) being the industrial sponsor. I would like to thank my industrial supervisor, Matthew Bower, from DWQR. Thank you for your unswerving support for me no matter I was in Tanzania, in China or in Edinburgh. Your insights into the water industry are inspiring to me. I have had a great time with your team at the membrane workshop. Professor Andrea Schäfer and Professor Bryce Richards (Karlsruhe Institute of Technology, Germany) were my supervisors during the field trip in Tanzania. Your vision, knowledge and experience have contributed to the success of the field trip. I particularly appreciate your scientific input on my PhD, such as designing research projects and commenting on papers. I also appreciate your investment into my personal development, such as encouraging me to climb Mt. Kilimanjaro and attend the Oxford Leadership Academy. My four-year PhD journey started from Edinburgh in July 2012. Just four months later I found myself on the plane flying to Tanzania and the planned three-month field trip turned to be as long as one and a half years! The long stay in Tanzania is a formative experience for me, which has changed the way I view my life and the world. I have learned to appreciate my abundance in every aspect, and to embrace the good days and the bad ones. I would like to say Asante Sana (thank you in Swahili) to several people who have made my life in Tanzania enjoyable. Professor Felix Mtalo (University of Dar es Salam, ii Tanzania) provided me office, laboratory and accommodation in Dar es Salam. Professor Eli Dahi (Defluoridation Technology Project, Tanzania) and his son William Dahi let me stay in their lovely family at Usa River. William, I hope we will have more adventures together! Mr Godfrey Mkongo (Ngurdoto Defluoridation Research Station, Tanzania) allowed me to use all the facilities in his station and helped me with water sampling and field trip. Mr Geert Aschermann (Technical University of Berlin, Germany) assisted with lab work and accompanied me on holidays. Geert, thank you for helping me practice driving even after you realized I was a terrible driver. Many people have contributed to different parts of this thesis. Dr Simona Gagliardi (Edinburgh Napier University) helped me with dynamic light scattering measurement. Dr Gudrun Abbt-Braun and Professor Harald Horn (Karlsruhe Institute of Technology, Germany) offered ICP-OES and ion chromatography analysis for Tanzanian water samples. Mr David McMullan (Scottish Water) provided ICP-OES and TOC analysis for the water samples that arrived in Scotland. Professor Anthony Szymczyk (Université de Rennes, France) offered streaming potential measurement for flat sheet membrane samples. Dr Silvia Ceppi (Oikos East Africa, Tanzania) provided information on Tanzanian community history regarding fluoride problem and commented on technology integration. Dr Edda Vuhahula (Muhimbli University of Health and Allied Sciences, Tanzania) provided valuable comments on health impacts of fluoride. Dr Filipe Vilela, Mr John Tobin and Mr Roman Steinbach (Heriot-Watt University) helped with the development of photocatalytic polymers. Thank you, Filipe, for your patience and for showing me the world of organic chemistry. Last but not least, my PhD examiners Dr Xue Jin (University of Glasgow) and Professor David Bucknall (Heriot-Watt University) provided valuable and constructive comments on my thesis. Thank you very much for your time and input. A special thank you goes to my closest friend Yue Heng. Thank you for talking things out with me, supporting my decisions, and always giving me the extra push when I need. Finally I would like to thank my parents and my girlfriend. You have given me unconditional love and encouragement all the time. I would not have been able to complete this PhD journey without your support. I hope I have made you proud. iii ACADEMIC REGISTRY Research Thesis Submission Name: Junjie Shen School/PGI: School of Engineering and Physical Science Version: (i.e. First, Final Degree Sought PhD Resubmission, Final) (Award and Chemistry Subject area) Declaration In accordance with the appropriate regulations I hereby submit my thesis and I declare that: 1) the thesis embodies the results of my own work and has been composed by myself 2) where appropriate, I have made acknowledgement of the work of others and have made reference to work carried out in collaboration with other persons 3) the thesis is the correct version of the thesis for submission and is the same version as any electronic versions submitted*. 4) my thesis for the award referred to, deposited in the Heriot-Watt University Library, should be made available for loan or photocopying and be available via the Institutional Repository, subject to such conditions as the Librarian may require 5) I understand that as a student of the University I am required to abide by the Regulations of the University and to conform to its discipline. * Please note that it is the responsibility of the candidate to ensure that the correct version of the thesis is submitted. Signature of Date: Candidate: Submission Submitted By (name in capitals): JUNJIE SHEN Signature of Individual Submitting: Date Submitted: For Completion in the Student Service Centre (SSC) Received in the SSC by (name in capitals): Method of Submission (Handed in to SSC; posted through internal/external mail): E-thesis Submitted (mandatory for final theses) Signature: Date: iv Contents Abstract ............................................................................................................................. i Acknowledgements .........................................................................................................
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