Chamber Investigations of Secondary Organic Aerosol Formation PDF Download
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Author: David Rea Cocker
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ISBN:
Category : Electronic dissertations
Languages : en
Pages : 694
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Author: David Rea Cocker
Publisher:
ISBN:
Category : Electronic dissertations
Languages : en
Pages : 694
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Author: Christine Lauren Loza
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ISBN:
Category : Aerosols
Languages : en
Pages : 336
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Author: Xuan Zhang
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ISBN:
Category : Electronic dissertations
Languages : en
Pages : 562
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Our understanding of the processes and mechanisms by which secondary organic aerosol (SOA) is formed is derived from laboratory chamber studies. In the atmosphere, SOA formation is primarily driven by progressive photooxidation of SOA precursors, coupled with their gas-particle partitioning. In the chamber environment, SOA-forming vapors undergo multiple chemical and physical processes that involve production and removal via gas-phase reactions; partitioning onto suspended particles vs. particles deposited on the chamber wall; and direct deposition on the chamber wall. The main focus of this dissertation is to characterize the interactions of organic vapors with suspended particles and the chamber wall and explore how these intertwined processes in laboratory chambers govern SOA formation and evolution. A Functional Group Oxidation Model (FGOM) that represents SOA formation and evolution in terms of the competition between functionalization and fragmentation, the extent of oxygen atom addition, and the change of volatility, is developed. The FGOM contains a set of parameters that are to be determined by fitting of the model to laboratory chamber data. The sensitivity of the model prediction to variation of the adjustable parameters allows one to assess the relative importance of various pathways involved in SOA formation. A critical aspect of the environmental chamber is the presence of the wall, which can induce deposition of SOA-forming vapors and promote heterogeneous reactions. An experimental protocol and model framework are first developed to constrain the vapor-wall interactions. By optimal fitting the model predictions to the observed wall-induced decay profiles of 25 oxidized organic compounds, the dominant parameter governing the extent of wall deposition of a compound is identified, i.e., wall accommodation coefficient. By correlating this parameter with the molecular properties of a compound via its volatility, the wall-induced deposition rate of an organic compound can be predicted based on its carbon and oxygen numbers in the molecule. Heterogeneous transformation of delta-hydroxycarbonyl, a major first-generation product from long-chain alkane photochemistry, is observed on the surface of particles and walls. The uniqueness of this reaction scheme is the production of substituted dihydrofuran, which is highly reactive towards ozone, OH, and NO3, thereby opening a reaction pathway that is not usually accessible to alkanes. A spectrum of highly-oxygenated products with carboxylic acid, ester, and ether functional groups is produced from the substituted dihydrofuran chemistry, thereby affecting the average oxidation state of the alkane-derived SOA. The vapor wall loss correction is applied to several chamber-derived SOA systems generated from both anthropogenic and biogenic sources. Experimental and modeling approaches are employed to constrain the partitioning behavior of SOA-forming vapors onto suspended particles vs. chamber walls. It is demonstrated that deposition of SOA-forming vapors to the chamber wall during photooxidation experiments can lead to substantial and systematic underestimation of SOA. Therefore, it is likely that a lack of proper accounting for vapor wall losses that suppress chamber-derived SOA yields contribute substantially to the underprediction of ambient SOA concentrations in atmospheric models.
Author: Aristeidis Voliotis
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ISBN:
Category :
Languages : en
Pages :
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Author: Arthur W. H. Chan
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ISBN:
Category : Atmospheric aerosols
Languages : en
Pages : 726
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Author: Nga Lee Ng
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ISBN:
Category : Electronic dissertations
Languages : en
Pages : 972
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Author: Axel Metzger
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Category :
Languages : en
Pages : 140
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Author: Yingdi Liu
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Category : Air
Languages : en
Pages : 65
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This thesis is only a part of my research work. For more information about my other work, including cavity ring down spectroscopy studies for peroxy radical, aerosol optical extinction, transparent thin and time of flight mass spectrometry studies for the initial steps of ozone and alkenes reaactions, please refer to my PhD thesis in Chemistry department, UC-Riverside.
Author: Crystal Glen
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Category :
Languages : en
Pages :
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Secondary organic aerosols (SOA) comprise a substantial fraction of the total global aerosol budget. While laboratory studies involving smog chambers have advanced our understanding of the formation mechanisms responsible for SOA, our knowledge of the processes leading to SOA production under ambient gaseous and particulate concentrations as well as the impact these aerosol types have on climate is poorly understood. Although the majority of atmospheric aerosols scatter radiation either directly or indirectly by serving as cloud condensation nuclei, soot is thought to have a significant warming effect through absorption. Like inorganic salts, soot may undergo atmospheric transformation through the vapor condensation of non-volatile gaseous species which will alter both its chemical and physical properties. Typical smog chamber studies investigating the formation and growth of SOA as well as the soot aging process are temporally limited by the initial gaseous concentrations injected into the chamber environment. Furthermore, data interpretation from such experiments is generally restricted to the singular gaseous species under investigation. This dissertation discusses the use of a new aerosol chamber designed to study the formation and growth of SOA and soot aging under atmospherically relevant conditions. The Ambient Aerosol Chamber for Evolution Studies (AACES) was deployed at three field sites where size and hygroscopic growth factor (HGF) of ammonium sulfate seed particles was monitored over time to examine the formation and growth of SOA. Similar studies investigating the soot aging process were also conducted in Houston, TX. It is shown that during the ambient growth of ammonium sulfate seed particles, as particle size increases, hygroscopic growth factors decrease considerably resulting in a significant organic mass fraction in the particle phase concluding an experiment. Observations of soot aging show an increase in measured size, HGF, mass and single scattering albedo. Ambient growth rate comparisons with chamber growth yielded similar trends verifying the use of AACES to study aerosol aging. Based on the results from this study, it is recommended that AACES be employed in future studies involving the production and growth of SOA and soot aging under ambient conditions in order to bridge the gaps in our current scientific knowledge.
Author:
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Category :
Languages : en
Pages : 15
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