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Development of Analytical Methods to Characterize Organic Aerosol and Black Carbon

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Development of Analytical Methods to Characterize Organic Aerosol and Black Carbon Development of Analytical Methods to Characterize Organic Aerosol And Black Carbon by Yiyi Wei, B. S. A Dissertation In CHEMISTRY Submitted to the Graduate Faculty of Texas Tech University in Partial Fulfillment of the Requirements for the Degree of DOCTOR OF PHILOSOPHY Approved Jonathan E. Thompson Chair of Committee Dimitri Pappas Yehia Mechref Mark Sheridan Dean of the Graduate School May, 2014 Copyright 2014, Yiyi Wei Texas Tech University, Yiyi Wei, May 2014 ACKNOWLEDGMENTS I would first like to express my appreciation to my research advisor, Dr. Jonathan Thompson, for his patient guidance and encouragement throughout the past four years in Texas Tech University. I have learned a lot from him in both class and lab. His diligent and persistent in research will encourage me all my life. I am also grateful to Dr. Pappas and Dr. Mechref for serving as my committee members and providing me valuable suggestions in many aspects. I also wish to thank my group members: Hao Tang, Kathy Dial, Haley Redmond, Fang Qian, Lulu Ma, Tingting Cao and Qing Zhang, for their help in both research and daily life. At last, I would like to thank my parents and friends for their support, love, and encouragement to finish my Ph. D. program. ii Texas Tech University, Yiyi Wei, May 2014 TABLE OF CONTENTS ACKNOWLEDGMENTS ...................................................................................................... ii ABSTRACT ............................................................................................................................ vi LIST OF TABLES ............................................................................................................... viii LIST OF FIGURES ............................................................................................................... ix LIST OF ABBREVIATIONS .............................................................................................. xii I. INTRODUCTION ............................................................................................................... 1 1.1 A General Description of Atmospheric Aerosols ......................................................... 1 1.1.1 Importance of Studying Aerosols ........................................................................ 1 1.1.2 Size Distribution and Growth of Aerosols ........................................................... 2 1.2 Composition of Aerosols .............................................................................................. 2 1.2.1 Organic Aerosols ................................................................................................. 3 1.2.1.1 Volatile Organic Compounds (VOCs) ........................................................ 3 1.2.1.2 Kinetics of VOCs ........................................................................................ 3 1.2.1.3 Gas-to-particle Phase Partitioning and Viscosity ....................................... 4 1.2.1.4 Measurement Techniques for Organic Aerosol. ......................................... 5 1.2.2 Black Carbon (BC) .............................................................................................. 6 1.2.2.1 Measurement Techniques of Black Carbon ................................................ 7 1.2.3 Inorganic Aerosols ............................................................................................... 9 1.3 Optical Properties of Atmospheric Aerosols .............................................................. 11 1.4 Motivation of dissertation work .................................................................................. 12 II. THE CHEMICAL EVOLUTION & PHYSICAL PROPERTIES OF ORGANIC AEROSOL: A MOLECULAR STRUCTURE BASED APPROACH ............................. 21 2.1 Introduction ................................................................................................................. 21 2.2 Methods....................................................................................................................... 23 2.2.1 The 3D Coordinate System ................................................................................ 23 2.2.2 Test Compound Database & QSPR Modeling................................................... 23 2.2.3 Squalene Ozonolysis Experiment ...................................................................... 24 2.2.4 Ambient Aerosol Sampling................................................................................ 25 2.2.5 High-resolution Mass Analysis .......................................................................... 26 2.2.6 Assigning Molecular Formulas .......................................................................... 26 2.3 Results and discussion ................................................................................................ 27 2.3.1 Advantages of The Approach ............................................................................ 27 iii Texas Tech University, Yiyi Wei, May 2014 2.3.2 Prediction of Physical & Chemical Properties................................................... 28 2.3.3 Prediction of Chemical Reactivity ..................................................................... 30 2.3.4 Comparison of 3D Approach to Alternate Schemes .......................................... 30 2.3.5 Properties of Chamber & Ambient Organic Aerosol ......................................... 32 2.3.6 General Trends: Similarity between Aerosol Types .......................................... 34 2.3.7 Current Limitations & Future Directions ........................................................... 35 2.4 Acknowledgments....................................................................................................... 36 III. LIGHT SCATTERING AND EXTINCTION MEASUREMENTS COMBINED WITH LASER-INDUCED INCANDESCENCE FOR THE REAL-TIME DETERMINATION OF SOOT MASS ABSORPTION CROSS SECTION .................. 44 3.1 Introduction ................................................................................................................. 44 3.2 Methods....................................................................................................................... 46 3.2.1 Description of Optical Measurements Using the Aerosol Albedometer with Laser-induced Incandescence. .................................................................................... 46 3.2.2 Scanning Mobility Particle Sizing (SMPS) and Particle Size Selection............ 48 3.2.3 Transmission Electron Microscopy (TEM) Analysis. ....................................... 48 3.2.4 Generation & Characteristics of Soot and Ambient Sampling. ......................... 49 3.2.5 Thermal Denuding. ............................................................................................ 50 3.3 Results and Discussion ............................................................................................... 50 3.3.1 LII Response Function and Effect of Coating/Mixing State. ............................ 50 3.3.2 Consequences of the LII Measurement: ns-Soot Morphology Changes ........... 52 3.3.3 Effect of Coating/Mixing State on ns-Soot M.A.C............................................ 54 3.3.4 M.A.C. Values for Dispersed Kerosene ns-Soot and Ambient Aerosol ............ 56 3.4 Conclusions ................................................................................................................. 56 3.5 Acknowledgments....................................................................................................... 57 IV. ATMOSPHERIC BLACK CARBON CAN EXHIBIT ENHANCED LIGHT ABSORPTION AT HIGH RELATIVE HUMIDITY ....................................................... 65 4.1 Introduction ................................................................................................................. 65 4.2 Experimental methods. ............................................................................................... 66 4.2.1 Sampling conditions........................................................................................... 66 4.2.2 Measurements .................................................................................................... 67 4.3 Results and Discussion ............................................................................................... 68 4.3.1 BC Mixing State Analysis ................................................................................. 68 4.3.2 BC Size and Mass Concentration ...................................................................... 69 4.3.3 Optical Measurement Results ............................................................................ 69 4.3.3.1 Mechanism of Enhanced Absorption ........................................................ 72 4.4 Significance and Conclusion....................................................................................... 74 iv Texas Tech University, Yiyi Wei, May 2014 4.5 Acknowledgement ...................................................................................................... 74 V. CONCLUSION AND FUTURE WORK ....................................................................... 85 APPENDICES ....................................................................................................................... 88 A. SUPPLEMENTARY INFORMATION FOR CHAPTER II ....................................... 88 B. SUPPLEMENTARY FIGURES FOR CHAPTER III .................................................. 92 C. SUPPLEMENTARY FIGURES FOR CHAPTER IV .................................................. 98 REFERENCE .....................................................................................................................
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