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Development of On-Demand Low Temperature Electrolysers and Their Systems

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Development of On-Demand Low Temperature Electrolysers and Their Systems Development of On-Demand Low Temperature Electrolysers and Their Systems by Daniel Robert Symes Thesis submitted in accordance with the requirements of The University of Birmingham for the degree of DOCTOR OF PHILOSOPHY School of Chemical Engineering College of Engineering and Physical Sciences The University of Birmingham 1st May 2015 University of Birmingham Research Archive e-theses repository This unpublished thesis/dissertation is copyright of the author and/or third parties. The intellectual property rights of the author or third parties in respect of this work are as defined by The Copyright Designs and Patents Act 1988 or as modified by any successor legislation. Any use made of information contained in this thesis/dissertation must be in accordance with that legislation and must be properly acknowledged. Further distribution or reproduction in any format is prohibited without the permission of the copyright holder. Development of On-Demand Low Temperature Electrolysers and their Systems Abstract Water electrolysis represents a technology for converting surplus renewable energy generation into hydrogen energy. With an increasing market penetration of intermittent renewable energy generation, the need for energy storage is more apparent. Options for hydrogen via water electrolysis include injection into the natural gas grid, refuelling of fuel cell vehicles and conversion back into the electricity grid via fuel cell when a deficit in supply/demand chain exists. Industrial on-demand hydrogen generating alkaline electrolysers were electrochemically characterised and analysed on an internal combustion engine. These electrolysers exhibited low efficiencies, low gas flowrates and subsequently zero change in engine emissions due to the poor design and build. An improved alkaline electrolyser was designed, built and tested, and exhibited improved efficiency and gas output compared to the industrial electrolysers and an improved reduction in engine emissions. The increased power consumption of the electrolyser results in a rise in electrode degradation which is responsible for the decrease in electrode lifetime. A method for prolonging the electrode lifetime is proposed through a metallic “oxygen-getter”. This implementation of an oxygen-getter has shown to prevent corrosion of the electrode material and thus reduces oxide content on the surface. The electrode lifetime in an alkaline electrolyser was proven to increase, but the commercial trend is shifting towards the more attractive PEM technology for electrolysis due to higher current densities, ability to handle variable input loads and non-caustic liquid requirement. PEM electrolysis is a rapidly evolving newly commercial electrolyser technology which uses a solid polymer membrane to split pure water into hydrogen and oxygen. The - i - Development of On-Demand Low Temperature Electrolysers and their Systems disadvantages of the technology are high cost due to the expensive PGM electrocatalyst and the ultrapure water requirement, with the latter the source of minimal research. The impact of water quality on two different membranes (Nafion® and Fumea®) performance was compared and tolerance to domestic tap water was highlighted. The cations present in varying grades of water were measured and systematically added to ultrapure water. This cation targeting demonstrated the limitations of specific cations in ultrapure water and the subsequent effect they had on MEA lifetime. The efficiency and degradation characteristics were analysed between alkaline and PEM technology and PEM technology was proven to show better performance and robustness over prolonged operation, along with the other advantages highlighted previously. A commercial on-demand PEM electrolyser was then tested and system designed for integration with an existing hydrogen refuelling station at the University of Birmingham. This mimicked the case for a distributed hydrogen system where the hydrogen is produced onsite for fuel cell vehicles resulting in a carbon neutral fuel. - ii - Development of On-Demand Low Temperature Electrolysers and their Systems I dedicate this thesis to my family for their love, support and encouragement - iii - Development of On-Demand Low Temperature Electrolysers and their Systems Acknowledgements I would like to dedicate this thesis to my first supervisor Waldemar Bujalski without who I would not be in this position on the doctorate programme. I would like to thank my supervisors Dr Bushra Al-Duri for her support, patience and diligence when assessing my work, and Dr Aman Dhir for his knowledge in the research area, I.T. DIY, and his keen eye for a bargain. I would like to thank staff, students and friends at the Centre for Hydrogen and Fuel Cell Research and School of Chemical Engineering for their assistance, entertainment and tolerance over the 4 years. I also thank the EPSRC for funding this PhD as part of the DTC in Hydrogen, Fuel Cells and their Applications. I would like to give thanks to the numerous undergraduate students who have assisted towards this research, specifically Connie Taylor-Cox, Leighton Holyfield, James Girling, Dhiren Mistry & Ailsa Crawford. Without your extra pairs of hands in the lab I would not be in this position to submit this thesis at this time. I also thank Jose Martin Herreros for his knowledge, assistance and support with the engine testing. Simon also wishes to express his gratitude to Bob Sharpster and Bill “Burns” Harris for their assistance in the manufacture of the electrolysers built herein, fire awareness, endless coffees, life lessons, Sara’s Specials and Friday Breakfasts enjoyed. There have been some great memories during the PhD: The Oil Spill, JENNY the Fuel Cell, Tony Bang, Dr Oxbig, Lickey Hills, FCV Snow Testing, Amy Winehands, The QHC Army, Coq au Vin, The Easter Flood, Bingo Backseat Journeys, General Election Debate FCV Debacle, Mandelsongate, Ben Millington. I give thanks for all the laughs. Finally I would like to thank my family for their love and support. It is done. - iv - Development of On-Demand Low Temperature Electrolysers and their Systems "Yes, my friends, I believe that water will one day be employed as fuel, that hydrogen and oxygen which constitute it, used singly or together, will furnish an inexhaustible source of heat and light, of an intensity of which coal is not capable….water will be the coal of the future". Jules Verne – Mysterious Island 1874 - v - Development of On-Demand Low Temperature Electrolysers and their Systems Contents 1. Introduction .............................................................................................................. 1 1.1. Project Motivation ........................................................................................ 2 1.2. Hydrogen Production Overview ................................................................... 5 1.3. Hydrogen Production Methods .................................................................... 8 1.3.1. Fossil Fuel Derived ................................................................................ 8 1.4.2. Biologically Derived ............................................................................ 14 1.3.3. Thermally Derived ............................................................................... 17 1.3.4. Electrically Derived ............................................................................. 19 1.3.5. Summary of Technologies ................................................................... 27 1.4. Project Rationale ........................................................................................ 28 2. Low Temperature Electrolysis for Hydrogen Production ................................. 32 2.1. Principles of Water Electrolysis ................................................................. 33 2.1.1. Thermodynamic Principles .................................................................. 33 2.1.2. Overpotentials ...................................................................................... 41 2.1.3. Electrolysis Efficiencies ...................................................................... 45 2.1.4. Electrolysis Kinetics ............................................................................ 50 2.1.5. Electrolyser Layout .............................................................................. 58 2.1.6. Bubble Dynamics ................................................................................. 62 2.2. Alkaline Electrolysis .................................................................................. 65 2.2.1. Electrodes ............................................................................................ 65 2.2.2. Electrolytes .......................................................................................... 66 2.2.3. Separators ............................................................................................ 67 2.3. PEM Electrolysis ........................................................................................ 67 2.3.1. Electrocatalysts .................................................................................... 68 2.3.2. Ionomer & Proton Exchange Membrane ............................................. 71 2.3.3. Current Collectors ................................................................................ 74 2.3.4. Separator Plates ................................................................................... 75 2.4. PEM Electrolyser Impurities .....................................................................
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