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Application Of Soft Ionization Aerosol Mass Spectrometry To Analysis Of Complex Organic Aerosol
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Book Synopsis Application of Soft Ionization Aerosol Mass Spectrometry to Analysis of Complex Organic Aerosol by : Scott Robertson Geddes
Download or read book Application of Soft Ionization Aerosol Mass Spectrometry to Analysis of Complex Organic Aerosol written by Scott Robertson Geddes and published by . This book was released on 2011 with total page 30 pages. Available in PDF, EPUB and Kindle. Book excerpt: The advantages of soft ionization AMS techniques of high sensitivity such as NIR-LDI-AMS are exemplified by an analysis of limonene ozonolysis SOA whereby first generation homogeneous oxidation products are delineated from second generation heterogeneous oxidation products. Future development of NIR-LDI-AMS and potential applications of high sensitivity soft ionization AMS systems are also discussed.
Book Synopsis Soft Ionization Aerosol Mass Spectrometry of Complex Organics by : Scott Geddes
Download or read book Soft Ionization Aerosol Mass Spectrometry of Complex Organics written by Scott Geddes and published by LAP Lambert Academic Publishing. This book was released on 2011-09 with total page 248 pages. Available in PDF, EPUB and Kindle. Book excerpt: Aerosol Mass Spectrometry (AMS) has emerged as the principal tool for aerosol analysis and soft ionization techniques are an important subset particularly suited for chemical speciation investigations. This dissertation presents the use of soft ionization AMS for the analysis of complex organic aerosols in laboratory studies, both as models for Primary and Secondary Organic Aerosol (POA and SOA). An established technique (PERCI-AMS) is used to identify the resonance capture mechanisms for cysteine containing peptide residues. This technique is then applied to investigate the ozonolysis of mixed particles representative of biogenic rich organic aerosol as is common for marine aerosols. In order to apply soft ionization AMS to lower concentrations of particle mass more representative of ambient aerosol loadings and thus allow SOA investigations, an entirely new AMS technique was developed and is presented utilizing Near-Infrared Laser-Desorption-Ionization (NIR-LDI-AMS). The advantages this technique are exemplified by an analysis of limonene ozonolysis SOA whereby first generation homogeneous oxidation products are delineated from second generation heterogeneous oxidation products.
Book Synopsis Development of Soft Ionization for Particulate Organic Detection with the Aerodyne Aerosol Mass Spectrometer by :
Download or read book Development of Soft Ionization for Particulate Organic Detection with the Aerodyne Aerosol Mass Spectrometer written by and published by . This book was released on 2008 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: During this DOE SBIR Phase II project, we have successfully developed several soft ionization techniques, i.e., ionization schemes which involve less fragmentation of the ions, for use with the Aerodyne time-of-flight aerosol mass spectrometer (ToF-AMS). Vacuum ultraviolet single photon ionization was demonstrated in the laboratory and deployed in field campaigns. Vacuum ultraviolet single photon ionization allows better identification of organic species in aerosol particles as shown in laboratory experiments on single component particles, and in field measurements on complex multi-component particles. Dissociative electron attachment with lower energy electrons (less than 30 eV) was demonstrated in the measurement of particulate organics in chamber experiments in Switzerland, and is now a routine approach with AMS systems configured for bipolar, negative ion detection. This technique is particularly powerful for detection of acidic and other highly oxygenated secondary organic aerosol (SOA) chemical functionality. Low energy electron ionization (10 to 12 eV) is also a softer ionization approach routinely available to AMS users. Finally, Lithium ion attachment has been shown to be sensitive to more alkyl-like chemical functionality in SOA. Results from Mexico City are particularly exciting in observing changes in SOA molecular composition under different photochemical/meteorological conditions. More recent results detecting biomass burns at the Montana fire lab have demonstrated quantitative and selective detection of levoglucosan. These soft ionization techniques provide the ToF-AMS with better capability for identifying organic species in ambient atmospheric aerosol particles. This, in turn, will allow more detailed study of the sources, transformations and fate of organic-containing aerosol.
Book Synopsis Further Development and Application of Laser Desorption Ionization (LDI) Using Aerosol Time-of-flight Mass Spectrometry (ATOFMS) by : Ryan Jay Wenzel
Download or read book Further Development and Application of Laser Desorption Ionization (LDI) Using Aerosol Time-of-flight Mass Spectrometry (ATOFMS) written by Ryan Jay Wenzel and published by . This book was released on 2004 with total page 454 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Molecular Characterization of Organic Aerosol by Mass Spectrometry by : Yuqian Gao
Download or read book Molecular Characterization of Organic Aerosol by Mass Spectrometry written by Yuqian Gao and published by . This book was released on 2011 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: Organic aerosol is a major constituent of atmospheric fine particles, especially over continental regions. These particles adversely affect human health and global climate. A significant fraction of organic aerosol is considered to be from the oxidation products of ozone and volatile organic compounds, which are called secondary organic aerosol (SOA). To study the formation mechanisms of secondary organic aerosol, it is important to characterize their molecular composition. The composition of secondary organic aerosol is very complex including thousands of species with molecular weight up to over a thousand Dalton. Methods utilized for the identification of these oxidation products involve advanced mass spectrometry techniques. In this dissertation, three mass spectrometry techniques were developed to study the molecular composition of organic aerosol. Firstly, online nano-aerosol sample deposition methods for matrix-assisted laser desorption/ionization (MALDI) mass spectrometry was developed to incorporate matrix particles directly with analyte particles onto a conventional MALDI plate. Secondly, a microsampling and analysis technique was developed in order to collect microgram samples and analyze them with high performance mass spectrometry. With this technique, the molecular composition of particle phase SOA at a low mass loading can be elucidated, which provides information about SOA formation at the early stages. A species with the (neutral molecule) formula C 17 H 26 O 8 (MW 358) increased substantially in intensity relative to other products as the mass loading decreased. Tandem mass spectrometry (MS n) of this species showed it to be a dimer of C 9 H 14 O 4 and C 8 H 12 O 4, most likely pinic acid and terpenylic acid, respectively. This species is likely to be critical at the early stages of SOA formation. Thirdly, ambient secondary electrospray ionization (ESI) source was designed to characterize the molecular composition of both gas and particle phases SOA online. This ion source was demonstrated to be applicable to a wide range of mass spectrometers having an ambient inlet. This technique provides a tool to acquire detailed information about possible SOA nucleation agents. A species with the (neutral molecule) formula C 20 H 36 O 6 (MW 372) was found in the gas-phase products of SOA, which could be critical for the new particle formation of SOA. Tandem mass spectrometry (MS n) of this species showed it to be a dimer of an organic hydroperoxide C 10 H 18 O 3, which is likely formed via OH-initiated oxidation pathway.
Book Synopsis Enabling the Identification, Quantification, and Characterization of Organics in Complex Mixtures to Understand Atmospheric Aerosols by : Gabriel Avram Isaacman
Download or read book Enabling the Identification, Quantification, and Characterization of Organics in Complex Mixtures to Understand Atmospheric Aerosols written by Gabriel Avram Isaacman and published by . This book was released on 2014 with total page 167 pages. Available in PDF, EPUB and Kindle. Book excerpt: Particles in the atmosphere are known to have negative health effects and important but highly uncertain impacts on global and regional climate. A majority of this particulate matter is formed through atmospheric oxidation of naturally and anthropogenically emitted gases to yield highly oxygenated secondary organic aerosol (SOA), an amalgamation of thousands of individual chemical compounds. However, comprehensive analysis of SOA composition has been stymied by its complexity and lack of available measurement techniques. In this work, novel instrumentation, analysis methods, and conceptual frameworks are introduced for chemically characterizing atmospherically relevant mixtures and ambient aerosols, providing a fundamentally new level of detailed knowledge on their structures, chemical properties, and identification of their components. This chemical information is used to gain insights into the formation, transformation and oxidation of organic aerosols. Biogenic and anthropogenic mixtures are observed in this work to yield incredible complexity upon oxidation, producing over 100 separable compounds from a single precursor. As a first step toward unraveling this complexity, a method was developed for measuring the polarity and volatility of individual compounds in a complex mixture using two-dimensional gas chromatography, which is demonstrated in Chapter 2 for describing the oxidation of SOA formed from a biogenic compound (longifolene: C15H24). Several major products and tens of substantial minor products were produced, but none could be identified by traditional methods or have ever been isolated and studied in the laboratory. A major realization of this work was that soft ionization mass spectrometry could be used to identify the molecular mass and formula of these unidentified compounds, a major step toward a comprehensive description of complex mixtures. This was achieved by coupling gas chromatography to high resolution time-of-flight mass spectrometry with vacuum ultraviolet (VUV) photo-ionization. Chapters 3 and 4 describe this new analytical technique and its initial application to determine the structures of unknown compounds and formerly unresolvable mixtures, including a complete description of the chemical composition of two common petroleum products related to anthropogenic emissions: diesel fuel and motor oil. The distribution of hydrocarbon isomers in these mixtures - found to be mostly of branched, cyclic, and saturated - is described with unprecedented detail. Instead of measuring average bulk aerosol properties, the methods developed and applied in this work directly measure the polarity, volatility, and structure of individual components to allow a mechanistic understanding of oxidation processes. Novel characterizations of these complex mixtures are used to elucidate the role of structure and functionality in particle-phase oxidation, including in Chapter 4 the first measurements of relative reaction rates in a complex hydrocarbon particle. Molecular structure is observed to influence particle-phase oxidation in unexpected and important ways, with cyclization decreasing reaction rates by ~30% and branching increasing reaction rates by ~20-50%. The observed structural dependence is proposed to result in compositional changes in anthropogenic organic aerosol downwind of urban areas, which has been confirmed in subsequent work by applying the techniques described here. Measurement of organic aerosol components is extended to ambient environments through the development of instrumentation with the unprecedented capability to measure hourly concentrations and gas/particle partitioning of individual highly oxygenated organic compounds in the atmosphere. Chapters 5 and 6 describe development of new procedures and hardware for the calibration and analysis of oxygenates using the Semi-Volatile Thermal desorption Aerosol Gas chromatograph (SV-TAG), a custom instrument for in situ quantification of gas- and particle-phase organic compounds in the atmosphere. High time resolution measurement of oxygenated compounds is achieved through a reproducible and quantitative methodology for in situ "derivatization"--Replacing highly polar functional groups that cannot be analyzed by traditional gas chromatography with less polar groups. Implementation of a two-channel sampling system for the simultaneous collection of particle-phase and total gas-plus-particle phase samples allows for the first direct measurements of gas/particle partitioning in the atmosphere, significantly advancing the study of atmospheric composition and variability, as well as the processes governing condensation and re-volatilization. This work presents the first in situ measurements of a large suite of highly oxygenated biogenic oxidation products in both the gas- and particle-phase. Isoprene, the most ubiquitous biogenic emission, oxidizes to form 2-methyltetrols and C5 alkene triols, while [alpha]-pinene, the most common monoterpene, forms pinic, pinonic, hydroxyglutaric, and other acids. These compounds are reported in Chapter 7 with unprecedented time resolution and are shown for the first time to have a large gas-phase component, contrary to typical assumptions. Hourly comparisons of these products with anthropogenic aerosol components elucidate the interaction of human and natural emissions at two rural sites: the southeastern, U.S. and Amazonia, Brazil. Anthropogenic influence on SOA formation is proposed to occur through the increase in liquid water caused by anthropogenic sulfate. Furthermore, these unparalleled observations of gas/particle partitioning of biogenic oxidation products demonstrate that partitioning of oxygenates is unexpectedly independent of volatility: many volatile, highly oxygenated compounds have a large particle-phase component that is poorly described by traditional models. These novel conclusions are reached in part by applying the new frameworks developed in previous chapters to understand the properties of unidentified compounds, demonstrating the importance of detailed characterization of atmospheric organic mixtures. Comprehensive analysis of anthropogenic and biogenic emissions and oxidation product mixtures is coupled in this work with high time-resolution measurement of individual organic components to yield significant insights into the transformations of organic aerosols. Oxidation chemistry is observed in both laboratory and field settings to depend on molecular properties, volatility, and atmospheric composition. However, this work demonstrates that these complex processes can be understood through the quantification of individual known and unidentified compounds, combined with their classification into descriptive frameworks.
Book Synopsis Fundamentals and Applications in Aerosol Spectroscopy by : Ruth Signorell
Download or read book Fundamentals and Applications in Aerosol Spectroscopy written by Ruth Signorell and published by CRC Press. This book was released on 2010-12-20 with total page 513 pages. Available in PDF, EPUB and Kindle. Book excerpt: Helping you better understand the processes, instruments, and methods of aerosol spectroscopy, Fundamentals and Applications in Aerosol Spectroscopy provides an overview of the state of the art in this rapidly developing field. It covers fundamental aspects of aerosol spectroscopy, applications to atmospherically and astronomically relevant problem
Book Synopsis Advances and Applications of Mass Spectral Techniques for the Characterization of Atmospheric Aerosol Particles by : Lindsay Erighn Hatch
Download or read book Advances and Applications of Mass Spectral Techniques for the Characterization of Atmospheric Aerosol Particles written by Lindsay Erighn Hatch and published by . This book was released on 2012 with total page 172 pages. Available in PDF, EPUB and Kindle. Book excerpt: Aerosol particles are ubiquitous in the atmosphere and induce significant impacts on human health and climate that depend on their physical and chemical properties, such as size, composition, and mixing state (chemical associations). Measurements of aerosol composition at the single-particle level are necessary to better understand these effects. Aerosol time-of-flight mass spectrometry (ATOFMS) is able to monitor the size and chemical composition of individual particles in real time. In this doctoral research, ATOFMS analysis was extended to identify new mass spectral markers and improve the potential for quantitative measurements. Development of novel instrumentation was also undertaken. Ion markers indicative of organosulfate compounds were identified in ATOFMS mass spectra collected in Atlanta, GA. In this study, the mixing state and temporal behavior of particulate organosulfate compounds were observed for the first time. Organosulfates were overwhelmingly detected in carbonaceous submicron particles and the temporal trends indicated that they likely formed by the daytime oxidation of isoprene followed by aqueous reaction with sulfate overnight. These results highlight the roles of mixing state and multi-phase reactivity on the formation of secondary organic aerosols. ATOFMS measurements of thermally-conditioned aerosol residuals obtained during the 2005 Study of Organic Aerosols in Riverside, CA were analyzed to determine the impacts of atmospheric aging on the laser desorption/ionization process. Coatings of secondary species suppressed the ionization efficiency, thereby impacting the mass spectral peak areas; however, a novel analysis method was found to correct these artifacts and produced strong agreement with collocated quantitative instrumentation. This new analysis technique was then applied to investigate the mixing-state dependence of aerosol volatility observed in Riverside. It was observed that particulate nitrate evaporated at different temperatures from different particle types (e.g., organic vs. biomass burning), which may influence the regional transport of nitrate species. ATOFMS provides important insights into size-resolved particle sources; however it heavily fragments most organic species, resulting in loss of the molecular information. Therefore, a novel chemical ionization mass spectrometer was developed to better characterize the molecular organic aerosol constituents. In particular, an ion funnel was incorporated into a home-built proton-transfer-reaction mass spectrometer. Initial characterization studies and ion simulations indicated that the ion funnel can provide high-efficiency ion transfer from the ionization region to the mass spectrometer. These results demonstrate the potential for this instrument to ultimately achieve highly sensitive analyses of organic aerosols.
Book Synopsis Development and Characterization of Two Versions of a New Single Particle Mass Spectrometer for Organic Aerosol Analysis that Incorporate a 3D Ion Trap by :
Download or read book Development and Characterization of Two Versions of a New Single Particle Mass Spectrometer for Organic Aerosol Analysis that Incorporate a 3D Ion Trap written by and published by . This book was released on 2001 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: Aerosol particles are ubiquitous throughout the atmosphere and play an important role in human health, climate, and the chemistry of the atmosphere. A significant mass fraction of these particles is composed of organic species, which remain poorly characterized due to the number and diversity of species present. This thesis describes the development and characterization of two versions of a new single particle mass spectrometer with a 3D ion trap for organic aerosol studies. Version I combines CO2 laser desorption and electron impact ionization in an ion trap. Mass spectra obtained for four species are comparable to NIST EI spectra. Tandem mass spectrometry studies are also demonstrated. The effects of vaporization energy, ionization delay time, and electron pulse width on the mass spectra and fragmentation patterns are examined. The detection limit of the instrument is found to be ~1x108 molecules (350 nm diameter particle) for 2,4-dihydroxybenzoic acid. Version II integrates CO2 laser desorption and tunable VUV ionization in an ion trap and was used for a detailed study of oleyl alcohol, oleic acid and mixtures thereof. Both the degree of fragmentation in the mass spectra and the translational energy of the vaporized molecules are found to vary as a function of desorption energy in the pure particles and as a function of composition in the mixed particles. These changes can be described by the energy absorbed per particle during desorption. We show that these effects hinder the quantitative response of the instrument and have important implications for other two step laser desorption/ionization systems. The final part of this thesis presents preliminary results from atmospherically relevant particles. Mass spectra of cigarette sidestream smoke, fulvic acid, meat cooking, and ammonium bisulfate aerosols are collected using both versions of the instrument. The two step desorption/ionization process only worked for two types of aerosols, while CO2 only mass spectra w.
Book Synopsis Elemental Ratio Measurements of Organic Compounds Using Aerosol Mass Spectrometry by :
Download or read book Elemental Ratio Measurements of Organic Compounds Using Aerosol Mass Spectrometry written by and published by . This book was released on 2015 with total page 20 pages. Available in PDF, EPUB and Kindle. Book excerpt: Elemental compositions of organic aerosol (OA) particles provide useful constraints on OA sources, chemical evolution, and effects. The Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is widely used to measure OA elemental composition. This study evaluates AMS measurements of atomic oxygen-to-carbon (O : C), hydrogen-to-carbon (H : C), and organic mass-to-organic carbon (OM : OC) ratios, and of carbon oxidation state (span style="border-top: 1px solid
Book Synopsis Characterizing Single Particle Ionization Using Bio-aerosol Mass Spectrometry by : Erica Lynne McJimpsey
Download or read book Characterizing Single Particle Ionization Using Bio-aerosol Mass Spectrometry written by Erica Lynne McJimpsey and published by . This book was released on 2008 with total page 342 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Characterization of Biogenic Secondary Organic Aerosol Using Mass Spectrometry by : Katherine J. Heaton
Download or read book Characterization of Biogenic Secondary Organic Aerosol Using Mass Spectrometry written by Katherine J. Heaton and published by . This book was released on 2010 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: Secondary Organic Aerosol (SOA) forms in the atmosphere from the oxidation of biogenic emissions. Even though SOA has been linked to health and climate effects, the chemical mechanism of SOA formation is not well understood. Through the use of mass spectrometry, this work characterizes SOA during the early stages of growth from the reaction of ozone with monoterpenes, a major biogenic emission. In this thesis, three types of studies are described for analyzing SOA formation: (1) the molecular composition of SOA is studied using the photoionization aerosol mass spectrometer, (2) the atomic composition is studied with the nanometer aerosol mass spectrometer and (3) high resolution mass spectrometry is used to help reconcile atomic and molecular composition data. The monoterpene ozonolysis reactions were performed in a flow tube reactor, where the reaction period could vary from 3s to 22s. The Photoionization Aerosol Mass Spectrometer (PIAMS) detected the formation of oligomers within seconds of the onset of the reaction. Ions that were detected were mapped to dimers that could form via the stabilized Criegee intermediate channel or the hydroperoxy channel. The Nanometer Aerosol Mass Spectrometer (NAMS) analyzed the elemental composition of the SOA which showed the formation of highly polar compounds during the early stages of SOA growth. NAMS also analyzed the changes in the composition of SOA when it formed in the presence of atmospheric species (water vapor, nitric acid vapor and sodium chloride seed particles). The data collected indicated that there is not as much change for endocyclic compounds as there is for exocyclic compounds. Finally, a new off-line analysis technique was created to micro-extract SOA deposited on a plate from the flow tube reactor. The samples were analyzed with the Fourier Transform Ion Cyclotron Resonance Mass Spectrometer (FTICR-MS). The FTICR-MS was used to collect molecular and elemental data simultaneously. The FTICR-MS produced accurate mass data that could be used to calculate molecular formulas. This provided a direct comparison of the data acquired with PIAMS and NAMS.
Book Synopsis Analytical Chemistry of Aerosols by : Kvetoslav R. Spurny
Download or read book Analytical Chemistry of Aerosols written by Kvetoslav R. Spurny and published by Routledge. This book was released on 2017-11-22 with total page 504 pages. Available in PDF, EPUB and Kindle. Book excerpt: Until the 1980s, researchers studied and measured only the physical properties of aerosols. Since the 80s, however, interest in the physicochemcal properties of aerosols has grown tremendously. Scientists in environmental hygiene, medicine, and toxicology have recognized the importance held by the chemical composition and properties of aerosols and the interactions of inhaled, "bad" aerosols. This book offers the first comprehensive treatment of modern aerosol analytical methods, sampling and separation procedures, and environmental applications, and offers critical reviews of the latest literature. This important field has developed rapidly in the last 15 years, but until now, no book effectively summarized or analyzed the existing research. Analytical Chemistry of Aerosols reviews procedures, techniques, and trends in the measurement and analysis of atmospheric aerosols. With contributions from acknowledged, international experts, the book discusses various methods of bulk analysis, single particle analysis, and the analysis of special aerosol systems, including fibrous and bacterial aerosols.
Book Synopsis Using Mass Spectrometry and Ftir to Characterize Atmospherically-relevant Particles Generated in Laboratory Systems by : Emily Anne Bruns
Download or read book Using Mass Spectrometry and Ftir to Characterize Atmospherically-relevant Particles Generated in Laboratory Systems written by Emily Anne Bruns and published by . This book was released on 2011 with total page 166 pages. Available in PDF, EPUB and Kindle. Book excerpt: Atmospheric aerosols are known to have multifaceted effects on human health, visibility and climate. To understand these effects, characterization of aerosol properties is necessary. This dissertation focuses on several specific topics with the overall goal of improving our understanding of aerosols in the atmosphere. One area of importance is particulate organic nitrates, which are known to be ubiquitous in the atmosphere; however, there is a lack of proven analytical techniques for their measurement. The qualitative and quantitative response of a high resolution time of flight aerosol mass spectrometer to particulate organic nitrates was studied by analyzing secondary organic aerosol (SOA) from NO3 radical reactions with [Alpha]- and [Beta]-pinene, 3-carene, limonene, and isoprene. Extensive fragmentation of the organic nitrate products was observed in the mass spectra, which precluded molecular speciation. Another area of interest is the recent development of a number of ambient ionization techniques, which are promising for aerosol characterization. One such technique, atmospheric solids analysis probe mass spectrometry (ASAP-MS), was applied for the first time to the identification of organics in SOA, which was generated in the laboratory from the ozonolysis of & alpha;-pinene and isoprene, and from the NO3 oxidation of & alpha;-pinene. Also, ambient samples were collected from a forested and a suburban location. ASAP-MS data for the laboratory-generated samples showed peaks corresponding to well-known products of these reactions, and higher molecular weight oligomers were present in all samples. This is consistent with previously published studies of similar systems and shows that ASAP-MS should have wide applicability in both laboratory and field studies. Vapor pressures of low volatility compounds are important parameters in several atmospheric processes, including the formation of new particles and the partitioning of compounds between the gas-phase and particles. However, vapor pressures of low volatility compounds are challenging to measure and reported values vary significantly, illustrating the need for new approaches. ASAP-MS was applied for the first time to the measurement of vapor pressures and heats of sublimation. The measured heats of sublimation were in good agreement with published values. The vapor pressures were typically within a factor of three of published values made at similar temperatures. This study establishes that ASAP-MS is a promising new technique for vapor pressure and heat of sublimation measurements of low volatility compounds. To further understand new particle formation, laboratory and field measurements were made to identify gas-phase amines, which could play a role in new particle formation, from previously unknown sources using proton transfer reaction mass spectrometry. The work presented in this dissertation advances our understanding of aerosols and explores novel methods for their characterization.
Book Synopsis Establishing Chemical Mechanisms and Estimating Phase State of Secondary Organic Aerosol From Atmospherically Relevant Organic Precursors by : Shashank Jain
Download or read book Establishing Chemical Mechanisms and Estimating Phase State of Secondary Organic Aerosol From Atmospherically Relevant Organic Precursors written by Shashank Jain and published by . This book was released on 2016 with total page 352 pages. Available in PDF, EPUB and Kindle. Book excerpt: Organic aerosol (OA) is a ubiquitous component of atmospheric particulate that influences both human health and global climate. A large fraction of OA is secondary in nature (SOA), being produced by oxidation of volatile organic compounds (VOCs) emitted by biogenic and anthropogenic sources. Despite the integral role of SOA in atmospheric processes, there remains a limited scientific understanding of the chemical and physical changes induced in SOA as it ages in the atmosphere. This thesis describes work done to increase the knowledge of processes and properties of atmospherically relevant SOA. In the work presented in this thesis, I have worked on improving an existing innovative, soft ionization aerosol mass spectrometer and utilized it to establish chemical mechanisms for oxidation of atmospherically relevant organic precursors (i.e., Green Leaf Volatiles). I discovered that SOA formation from cis-3-hexen-1-ol is dominated by oligomer and higher molecular weight products, whereas the acetate functionality in cis-3-hexenylacetate inhibited oligomer formation, resulting in SOA that is dominated by low molecular weight products. One of the most important factors contributing to uncertainties in our estimations of SOA mass in the atmosphere, remains our basic assumption that atmospheric SOA is liquid-like, which we have found to be untrue. Hence, I developed a methodology to estimate the phase state of SOA and identified new parameters that can have significant influence on the phase state of atmospheric aerosol. This simplified method eliminates the need for a Scanning Mobility Particle Sizer (SMPS) and directly measures Bounce Factor (BF) of polydisperse SOA using only one multi-stage cascade Electrostatic Low Pressure Impactor (ELPI). The novel method allows for the real time determination of SOA phase state, permitting studies of the relationship between SOA phase, oxidative formation and chemical aging in the atmosphere. I demonstrated that SOA mass loading (CSOA) influences the phase state significantly. Results show that under nominally identical conditions, the maximum BF decreases by approximately 30% at higher CSOA and suggests that extrapolation of experiments not conducted at atmospherically relevant SOA levels to simulate the chemical properties may not yield results that are relevant to our natural environment. My work has provided a better understanding of the mechanisms of aerosol formation at atmospheric concentrations, which is necessary to understand its physical properties. This improved understanding is fundamental to accurately model aerosol formation in the atmosphere, and subsequently evaluate their large-scale effect on human health and environment.
Book Synopsis Analysis of Atmospheric Aerosol Processes Using Single Particle Mass Spectrometry by : Jeffrey Robert Whiteaker
Download or read book Analysis of Atmospheric Aerosol Processes Using Single Particle Mass Spectrometry written by Jeffrey Robert Whiteaker and published by . This book was released on 2002 with total page 644 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Composition and Photochemistry of Anthropogenic and Biogenic Organic Aerosols by : Sandra Louise Blair
Download or read book Composition and Photochemistry of Anthropogenic and Biogenic Organic Aerosols written by Sandra Louise Blair and published by . This book was released on 2016 with total page 228 pages. Available in PDF, EPUB and Kindle. Book excerpt: Aerosols can substantially impact human health, atmospheric chemistry, and climate. The composition and photochemistry of a variety of anthropogenic and biogenic primary and secondary organic aerosols (POA and SOA) have yet to be fully characterized. The composition of organic aerosols is extremely complex - they contain a variety of highly oxidized, multifunctional, low vapor pressure organic compounds. The primary focus of this thesis is on the molecular characterization of organic aerosols that are not well understood or have not been studied before, such as primary emissions from electronic cigarettes, iron (III) mediated SOA, and photooxidized biodiesel and diesel fuel SOA. Another focus of this dissertation is the effect of direct photochemical aging on the composition of organic aerosol. Direct photolysis experiments were first applied to a system that is known to have a photolabile composition, alpha-pinene ozonolysis SOA, such that characterization of a photochemical effect would be possible to quantify. Photolysis of more complex SOA that have not been studied before, photooxidized biodiesel and diesel fuel SOA, were also investigated in this thesis. Advanced high resolution mass spectrometry techniques were used in the molecular characterization of organic aerosols, including nano-Desorption Electrospray Ionization Mass Spectrometry (nano-DESI) and Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR). An additional suite of online instrumentation was used to measure gas-phase composition, particle-phase composition, particle size and concentration, and absorption properties: Proton Transfer Reaction Time-of-Flight Mass Spectrometry (PTR-ToF-MS), Aerosol Mass Spectrometry (ToF-AMS), Scanning Mobility Particle Sizing (SMPS), and UV-vis spectroscopy. The molecular analysis of these aerosols provides valuable insight to the formation and photochemical behavior of unexpected, polymeric, light absorbing, and unique organosulfur species.
