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The Oxidation of a Gasoline Fuel Surrogate in the Negative Temperature Coefficient Region David Burton Lenhert Dr

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The Oxidation of a Gasoline Fuel Surrogate in the Negative Temperature Coefficient Region David Burton Lenhert Dr The Oxidation of a Gasoline Fuel Surrogate in the Negative Temperature Coefficient Region A Thesis Submitted to the Faculty of Drexel University by David Burton Lenhert in partial fulfillment of the requirements for the degree of Masters of Science in Mechanical Engineering July 2004 © Copyright 2004 David B. Lenhert. All Rights Reserved. ii Acknowledgements I would like to thank all of the people that have contributed and supported me during this lengthy endeavor to complete my Masters Thesis. Of special note, I would like to thank my advisors Dr. Nicholas P. Cernansky, Dr. David L. Miller, and Dr. Kevin G. Owens for their support, guidance, tolerance, and friendship throughout this enterprise. Most importantly, I appreciate their willingness to allow me the opportunity and time to modify various aspects of the experimental and analytical facilities and to conduct this research independently. I must acknowledge the assistance of Abdul Rafey Kahn, Suqing Wang, and Alessandro Agosta as they have helped me during various stages of this work. In addition, Dr. Richard Billmers and Mary Emig have provided the much needed outlet to keep my spirits up over the past six years at Drexel. Furthermore, the past and present staff at the Hess Laboratories, namely Richard Miller, Lou Hass, and Dr. Bill Danley, have been helpful in the completion of this project. Finally, I would like to give special thanks to Dawn Carolan who has supported me through good and bad times and has dragged me out of the lab for some desperately needed distraction. This research was funded by the U.S. Army Research Office (Grant No. DAAG55- 98-1-0286, Project No. 37699-EG, Grant No. DAAG55-97-1-0196, Project No. 36910- EG-AAS and Grant No. DAAD19-03-1-0070, Project No. 44458-EG), the National Science Foundation (Grant No. CTS-9910563), and the Hess Fellowship. Their funding was greatly appreciated. iii Table of Contents LIST OF TABLES............................................................................................................ vii LIST OF FIGURES .........................................................................................................viii ABSTRACT..................................................................................................................... xiv 1. INTRODUCTION .......................................................................................................... 1 1.1 Introduction............................................................................................................. 1 1.2 Autoignition and Knock.......................................................................................... 3 1.3 Interaction of Hydrocarbon Families...................................................................... 6 1.4 Closure .................................................................................................................... 7 2. BACKGROUND & LITERATURE REVIEW.............................................................. 8 2.1 Introduction............................................................................................................. 8 2.2 Hydrocarbon Oxidation Chemistry......................................................................... 8 2.3 Low & Intermediate Temperature Chemistry....................................................... 10 2.3.1 Alkane Oxidation Chemistry ............................................................................ 11 2.3.2 Alkene Oxidation Chemistry ............................................................................ 17 2.3.3 Aromatic Oxidation Chemistry......................................................................... 21 2.3.4 Aldehyde Oxidation Chemistry ........................................................................ 25 2.4 Past 1-Pentene Studies .......................................................................................... 27 2.5 Past n-Heptane Studies ......................................................................................... 30 2.6 Past iso-Octane Studies......................................................................................... 35 2.7 Past Toluene Studies............................................................................................. 40 2.8 Past Functional Group Interaction Studies ........................................................... 46 2.9 Closure .................................................................................................................. 51 3. EXPERIMENTAL FACILITY & METHODOLOGY ................................................ 53 3.1 Introduction........................................................................................................... 53 iv 3.2 Pressurized Flow Reactor Facility ........................................................................ 53 3.2.1 Facility Upgrades.............................................................................................. 57 3.3 Experimental Methodology.................................................................................. 61 3.3.1 Controlled Cool Down Operation..................................................................... 62 3.3.2 Constant Inlet Temperature Operation.............................................................. 66 3.4 Gas Analysis System............................................................................................. 67 3.4.1 Introduction....................................................................................................... 67 3.4.2 Fuel Flow Rate Calibration and Analysis ......................................................... 70 3.4.3 Intermediate Species Analysis .......................................................................... 72 3.4.3.1 Siemens Ultramat NDIR................................................................................... 72 3.4.3.2 Multiple Loop Sample Storage System ............................................................ 73 3.4.3.3 Thermo Finnigan GC/MS System .................................................................... 76 3.4.3.4 Calibration and Quantification.......................................................................... 79 3.5 Reactant Gasses and Fuels.................................................................................... 82 3.6 Closure .................................................................................................................. 86 4. RESULTS OF 1-PENTENE OXIDATION.................................................................. 87 4.1 Introduction........................................................................................................... 87 4.2 Experimental Conditions ...................................................................................... 87 4.3 Results of the 1-Pentene CCD Experiment........................................................... 89 4.4 Discussion of 1-Pentene Results and Governing Chemistry ................................ 95 4.5 Closure ................................................................................................................ 102 5. RESULTS OF N-HEPTANE OXIDATION .............................................................. 104 5.1 Introduction......................................................................................................... 104 5.2 Experimental Conditions .................................................................................... 104 5.3 Model Conditions............................................................................................... 105 v 5.4 Results of n-heptane CCD Experiment............................................................... 107 5.5 Results of n-Heptane CIT Experiment................................................................ 117 5.6 Discussion of n-Heptane Results and Governing Chemistry.............................. 124 5.7 Closure ................................................................................................................ 129 6. RESULTS OF ISO-OCTANE OXIDATION............................................................. 131 6.1 Introduction......................................................................................................... 131 6.2 Experimental Conditions .................................................................................... 131 6.3 Model Conditions............................................................................................... 132 6.4 Results of iso-Octane CCD Experiment ............................................................. 133 6.5 Results of iso-Octane CIT Experiment............................................................... 144 6.6 Discussion of iso-Octane Results and Governing Chemistry............................. 149 6.7 Closure ................................................................................................................ 153 7. RESULTS OF GASOLINE SURROGATE OXIDATION........................................ 155 7.1 Introduction......................................................................................................... 155 7.2 Experimental Conditions .................................................................................... 155 7.3 Model Conditions............................................................................................... 156 7.4 Results of Surrogate CCD Experiment............................................................... 158 7.5 Results of Surrogate CIT Experiment................................................................
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