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Wallace Wsu 0251E 10875.Pdf (8.549Mb) EXPERIMENTAL OBSERVATIONS OF NON-METHANE HYDROCARBONS AND NOX SOURCES IN URBAN AND RURAL LOCATIONS By Henry William Wallace IV A dissertation submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy WASHINGTON STATE UNIVERSITY College of Engineering and Architecture July 2013 To the Faculty of Washington State University: The members of the Committee appointed to examine the dissertation of Henry William Wallace IV find it satisfactory and recommend that it be accepted. ___________________________________ B. Thomas Jobson, Ph.D, Chair ___________________________________ Brian K. Lamb, Ph.D ___________________________________ Timothy M VanReken, Ph.D ___________________________________ Heping Liu, Ph.D ii DEDICATION I dedicate this dissertation and the educational achievement that comes with it to my mother and to the loving memory of my father. I know she is proud of me and that he would be. iii ATTRIBUTION This dissertation addresses the sources of nonmethane hydrocarbons NMHCs and NOx in urban and rural environments by developing instrumentation to measure C2 to C12 VOCs and by making experimental observations. It is organized into 6 major chapters: introduction (Chapter 1), instrumentation development and testing for measurement of Volatile Organic Compounds (VOCs) (Chapter 2), rural observations of NMHCs and NOx through a forest canopy (Chapter 3), wintertime observations of NMHCs, CO, and NOx in an urban environment and comparison to vehicle emissions models (Chapter 4 published in Atmospheric Environment as Wallace et al. (2012)), and summertime observations of NMHCs, CO and NOx (Chapter 5), and conclusions (Chapter 6). Henry W. Wallace IV was the primary author of this dissertation. Dr. B Thomas Jobson, Dr. Timothy VanReken, Dr. Brian K. Lamb, and Dr. Heping Liu have contributed to this work by editing and providing guidance to the quality of the content. Dr. B. Thomas Jobson made many intellectual contributions to the design and implementation of the VOC preconcentratioin system during numerous brainstorming sessions throughout the author’s time at WSU. The phase modulation circuit that supplys power to heat the adsorbent tubes was designed and constructed by Fred Schuetze at the Electronics Shop which is a part of WSU’s Technical Services. The nitrous acid source, which serves as the radical source during the photochemical chamber oxidatioin experiments was designed and constructed by Claudia Toro. Mrs. Toro also assisted with the re-plumbing of the VOC preconcentration system. The photochamber was constructed by a number of people including Dr. B.Thomas Jobson, Jacob McCoskey, Claudia Toro and myself. The PTR-MS and CO measurements reported in this iv dissertation were made by Matthew H. Erickson, Jacob McCoskey (Chapter 4 only), and Dr. B. Thomas Jobson. Figure 3.1 was a modified from a file that was generated by Dr. Shelley N. Presseley and Figure 3.5 was taken with permission from VanReken et al., (Submitted). The jNO2 values used in chapter 3 were provided by Dr. Barry Lefer and Dr. James Flynn. Output for the vehicle emissions models was provided by Dr. Brian K. Lamb and Dr. Joseph Vaughn (Chapter 4: MOBILE6.2) and Dr. Rick C. Hardy, Dr. Jennifer L. Cole, Dr. Sarah M. Strahan, and Dr. Wei Zhang (Chapter 4: MOVES). The organic aerosol mixing ratios presented in Chapter 5 were measured and by Dr. Chen Song and were downloaded from the ARM database. v EXPERIMENTAL OBSERVATIONS OF NON-METHANE HYDROCARBONS AND NOX SOURCES IN URBAN AND RURAL LOCATIONS ABSTRACT by Henry William Wallace IV, PhD. Washington State University July 2013 Chair: B. Tom Jobson Non-methane hydrocarbons (NMHCs) and NO + NO2 (NOx) are precursors for photochemical smog which includes particulate matter and ozone. NMHCs and NOx have both biogenic and anthropogenic sources. This work characterizes sources of NMHCs and NOx by developing and deploying instrumentation for the quantification of NMHCs emitted from vegetation and spark ignition engines. A two channel volatile organic compound (VOC) preconcentration system was designed and constructed to measure C2 to C12 VOCs with a gas chromatograph-ion trap mass spectrometer GC-ITMS and a gas chromatography-flame ionization detector. Observations from three field experiments are used to characterize sources of VOC and NOx, and the impact these pollutants have on local air chemistry. Focus is given to mobile sources emissions as they are an important, often dominant, source of NHMCs and NOx in urban environments. Morning rush hour CO to NOx ratios of 4.2 ± 0.59 mol/mol and 6.9 ± 1.1 mol/mol are reported for Boise, ID and Sacramento, CA, respectively. VOC to CO ratios for both Boise, ID and Sacramento, CA are reported as well. Toluene to CO ratios during the morning rush hour were observed at 2.4 ± 0.04 vi nmol/mol in Boise, ID and 4.7 ± 0.34 nmol/mol in Sacramento, CA while benzene to CO was 1.3 ± 0.02 nmol/mol and 1.1 ± 0.05 nmol/mol in Boise, ID and Sacramento, CA, respectively. A thorough evaluation of the US EPA’s vehicle emissions models MOBILE6.2 and MOVES is presented. The analysis shows that MOVES represents a significant improvement over MOBILE6.2. The preconcentration system was used quantify VOCs emissions from automobiles in an urban environment. Emissions measured from mobile sources are compared to predicted values from the models and the MOVES model was found to greatly improve the prediction of CO to NOx when compared to the older MOBILE6.2 model. Biogenic sources of VOCs and NOx are examined in a rural location using a profiling sample inlet to spatially resolve chemical gradients in a forest. Evidence of mixing in the canopy has been explored using the Leighton relationship and the gradients presented can be analyzed to determine sources and sinks in the canopy. vii TABLE OF CONTENTS ABSTRACT ....................................................................................................................... vi TABLE OF CONTENTS ................................................................................................. viii LIST OF FIGURES ......................................................................................................... xiii LIST OF TABLES ....................................................................................................... xxviii CHAPTER 1: INTRODUCTION ....................................................................................... 1 1.1. NMHC MEASUREMENT TECHNIQUES .......................................................... 4 1.2. DISSERTATION OVERVIEW............................................................................. 6 1.3. REFRENCES ....................................................................................................... 10 CHAPTER 2: INSTRUMENT DESCRIPTION AND DEVELOPMENT ...................... 18 2.1. NOxy INSTRUMENT DESCRIPTION ............................................................... 18 2.1.1. Principle of Measurement ........................................................................... 18 2.1.1.1. Nitric Oxide (NO) .............................................................................. 19 2.1.1.2. Nitrogen Dioxide (NO2) ..................................................................... 20 2.1.1.3. Reactive Odd Nitrogen (NOy) ............................................................ 22 2.1.2. Sample Handling ......................................................................................... 23 2.1.3. Calibration and Zeros .................................................................................. 24 2.1.4. Instrument Response ................................................................................... 25 2.1.5. Artifacts and Corrections ............................................................................ 27 2.2. PRECONCENTRATION GC-ITMS/FID ........................................................... 28 2.2.1. Instrument Description................................................................................ 28 2.2.1.2. Adsorbent Traps ................................................................................. 38 2.2.1.3. Trap Temperature Control ................................................................. 40 viii 2.2.1.4. Water Trap Temperature Control ....................................................... 41 2.2.1.5. DAQFactory Control Program ........................................................... 42 2.2.2. Principle of Measurement ........................................................................... 43 2.2.2.1. FID ..................................................................................................... 43 2.2.2.2. ITMS .................................................................................................. 48 2.2.3. Sample Handling ......................................................................................... 50 2.2.3.1. Water Trap ......................................................................................... 50 2.2.3.2. VOC Pre-concentration ...................................................................... 52 2.2.4. Calibration Gases ........................................................................................ 53 2.2.4.1. GCMS Calibration Gas ...................................................................... 54 2.2.4.2. PTR-MS Calibration Gas ................................................................... 54 2.2.4.3. SPECTRA Calibration Gas ................................................................ 55
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