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Measurement of Proton Transfer Reaction Rates in a Microwave Cavity Discharge Flowing Afterglow George M Old Dominion University ODU Digital Commons Physics Theses & Dissertations Physics Spring 2003 Measurement of Proton Transfer Reaction Rates in a Microwave Cavity Discharge Flowing Afterglow George M. Brooke IV Old Dominion University Follow this and additional works at: https://digitalcommons.odu.edu/physics_etds Part of the Atmospheric Sciences Commons, Atomic, Molecular and Optical Physics Commons, and the Physical Chemistry Commons Recommended Citation Brooke, George M.. "Measurement of Proton Transfer Reaction Rates in a Microwave Cavity Discharge Flowing Afterglow" (2003). Doctor of Philosophy (PhD), dissertation, Physics, Old Dominion University, DOI: 10.25777/6vm5-5117 https://digitalcommons.odu.edu/physics_etds/38 This Dissertation is brought to you for free and open access by the Physics at ODU Digital Commons. It has been accepted for inclusion in Physics Theses & Dissertations by an authorized administrator of ODU Digital Commons. For more information, please contact [email protected]. MEASUREMENT OF PROTON TRANSFER REACTION RATES IN A MICROWAVE CAVITY DISCHARGE FLOWING AFTERGLOW By George M. Brooke IV B.S. May 1994, Virginia Military Institute M.S. December 1997, Old Dominion University A Dissertation Submitted to the Faculty of Old Dominion University in Partial Fulfillment of the Requirement for the Degree of DOCTOR OF PHILOSOPHY PHYSICS OLD DOMINION UNIVERSITY May 2003 Approved by: Leposava Vuskovic (Director) Anatoly V. Radyushkin (Member) Charles I. Sukenik (Member) Paul E. Ulmer (Member) Karl H. Schoenbach (Member) Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. ABSTRACT MEASUREMENT OF PROTON TRANSFER REACTION RATES IN A MICROWAVE CAVITY DISCHARGE FLOWING AFTERGLOW George M. Brooke IV Old Dominion University, 2003 Director: Dr. Leposava Vuskovic The reaction rate coefficients between the hydronium ion and the molecules ethene (C2 H 4), propene (C?//*), 1-butene (C*//*) and hydrogen sulfide (. H2 S) were measured at 296 K. The measured reaction rates were compared to collision rates calculated using average dipole orientation (ADO) theory. Reaction efficiency depends primarily upon the proton affinity of the molecules. All the measurements were obtained using the newly developed microwave cavity discharge flowing afterglow (MCD-FA) apparatus. This device uses an Asmussen-type microwave cavity discharge ion source that is spatially separated from the flow tube, eliminating many of the problems inherent with the original FA devices. In addition to measuring reaction rate coefficients, the MCD-FA was shown to be an effective tool for measuring trace compounds in atmospheric air. This method has many advantages over current detection techniques since compounds can be detected in almost real time, large mass ranges can be scanned quickly, and repeated calibration is not required. Preliminary measurements were made o f car exhaust and exhaled alveolar air. Car exhaust showed the presence of numerous hydrocarbons, such as butene, benzene and toluene while the exhaled alveolar air showed the presence o f various volatile organic compounds such as methanol and acetone. Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. Copyright, 2003, by George M. Brooke IV, All Rights Reserved. Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. This dissertation is dedicated to my loving and ever patient wife, Erika. Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. V ACKNOWLEDGMENTS I would like to acknowledge first and foremost my advisor, Dr. Leposava Vuskovic whose support and guidance throughout my graduate career has been invaluable. Her enthusiasm for physics and concern for her students provides the ideal environment for intellectual development. Additionally, I would like to thank Dr. Svetozar Popovic for all of the support he has provided. His guidance in the laboratory and insight into physics, especially gas discharge physics, has played a critical role in my research. I would also like to acknowledge and thank Dr. Charles Sukenik for all the encouragement and support that he has given me and numerous other students at ODU. His selfless dedication to students and his enthusiasm towards physics is something I will always attempt to emulate. I also want to thank Dr. Gary Copeland for many hours of useful discussions and entertaining lunches. His broad knowledge of physics and inquisitive nature always made me reflect more deeply on my own research. I also want to thank the other graduate students at ODU, especially Hugh (Trey) Thurman. Trey’s depth of knowledge never ceased to amaze me, and his friendship is something I will always cherish. I also want to thank Thao Dinh, Pasad Kulatunga, Prasong Kessaratikoon, Dorin Todor, and Tobias Oed for all the discussions and enjoyable times we shared. Finally I want to say thank you to my family for everything they have done for me, especially my beautiful wife Erika, whose unwavering support and dedication have been paramount to my success. I love you. Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. TABLE OF CONTENTS Page LIST OF TABLES................ ...........viii LIST OF FIGURES...................... ix Section 1. INTRODUCTION............... 1 2. ION-MOLECULE COLLISION THEORY AND CALCULATION OF REACTION RATE COEFFICIENTS..........................5 2.1 Ion-Molecule Collisions ....................... 5 2.2 Proton Transfer Reactions in the Gas Phase ................... 12 2.3 Determination of Charge Transfer Reaction Coefficients ........................................................ 13 3. EXPERIMENT... ................. 17 3.1 Proton Donor Source .................... 19 3.1.1 Hollow Cathode Discharge ..........................................................20 3.1.2 Radio Frequency Discharge ...................................... 25 3.1.2.1 Experiment ............................................. 27 3.1.3 Microwave Cavity Discharge ......................... 33 3.1.3.1 Experiment ............................................. 35 3.1.3.2 Properties of the Microwave Discharge Plasma. ........................................................... 43 3.2 Flow Tube ......................................................... 49 3.2.1 Buffer Gas Flow Properties ................. 50 3.2.2 Venturi Inlet ................... 55 3.2.3 Reactant Gas Injection Ports ............................ 58 3.3 Detection System ............................................. 60 3.3.1 Ion Optics ............................. 61 3.3.2 Quadrupole Mass Spectrometer .................. 65 3.3.3 Signal Detection and Data Acquisition ......................................68 4. RESULTS AND DISCUSSION.............. ...74 4.1 Error Analysis .......................... 75 4.2 Ethene (C2 H4).......................... 77 4.3 Propene (Cjifg)................... 84 4.4 1-Butene ( C ^ ) ........ 89 4.5 Hydrogen Sulfide (H2 S) ......................................................................... 95 Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. Section Page 5. APPLICATION OF THE MCD-FA TO TRACE GAS ANALYSIS........101 5.1 Pollution Monitoring. ..................... 106 5.2 Exhaled Alveolar Air. ............................. ...112 6. CONCLUSIONS.............. ...........117 APPENDICES ....................... 120 A. Theory of the Quadrupole Mass Spectrometer— ....................... 120 B. Theory of Cylindrical Resonant Cavities ................ 126 C. Observed Argon Lines in MCD ............... 136 D. Useful Unit Conversions .............................. 143 REFERENCES............................. 144 VITA ........................... 151 Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. LIST OF TABLES Table Page I. Temperature evaluation data ...... .45 II. Properties of ethene at STP. ...................... 77 III. Rate coefficient for the reaction of the hydronium ion with ethene in units of (cm3/s) .................. 79 IV. Properties ofpropene at STP ...... ..........85 V. Rate coefficient for the reaction of the hydronium ion with propene in units of (cmVs). ...................... 85 VI. Properties ofbutene at STP .................. .90 VII. Rate coefficients for the reaction of the hydronium ion with butene in units of (cm3/s) ...................................... 91 Vni. Properties o f hydrogen sulfide at STP ............... 95 IX. Rate coefficient for the reaction of the hydronium ion with hydrogen sulfide in units of (cm3/s) .................................. 97 X. Proton affinity of various organic and inorganic compounds ......................... 103 XI. Aliphatic alkanes and their applications ............................... 107 XII. Concentration o f several trace compounds in car exhaust ................ ..110 XIII. Summary of cylindrical resonant cavity equations ..................... 135 XIV. Observed argon lines in a water vapor discharge with an admixture of argon (grating 1 - blazed at 500 nm). ............................. 136 XV. Observed argon lines in a water vapor discharge with an admixture of argon (grating 2 - blazed at 800 nm) ....................... 137 XVI. Mass flow conversion table ..................... 143 XVII. Pressure conversion table .......................... 143 XVm. Miscellaneous conversion factors. ......
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