Advances and Applications of Mass Spectral Techniques for the Characterization of Atmospheric Aerosol Particles
Advances and Applications of Mass Spectral Techniques for the Characterization of Atmospheric Aerosol Particles

Author: Lindsay Erighn Hatch

Publisher:

Published: 2012

Total Pages: 172

ISBN-13: 9781267646781

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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.

Aerosol Measurement
Aerosol Measurement

Author: Pramod Kulkarni

Publisher: John Wiley & Sons

Published: 2011-07-12

Total Pages: 920

ISBN-13: 0470387416

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Aerosol Measurement: Principles, Techniques, and Applications Third Edition is the most detailed treatment available of the latest aerosol measurement methods. Drawing on the know-how of numerous expert contributors; it provides a solid grasp of measurement fundamentals and practices a wide variety of aerosol applications. This new edition is updated to address new and developing applications of aerosol measurement, including applications in environmental health, atmospheric science, climate change, air pollution, public health, nanotechnology, particle and powder technology, pharmaceutical research and development, clean room technology (integrated circuit manufacture), and nuclear waste management.

Using Mass Spectrometry and Ftir to Characterize Atmospherically-relevant Particles Generated in Laboratory Systems
Using Mass Spectrometry and Ftir to Characterize Atmospherically-relevant Particles Generated in Laboratory Systems

Author: Emily Anne Bruns

Publisher:

Published: 2011

Total Pages: 166

ISBN-13: 9781267057884

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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.

Ambient Mass Spectroscopy Techniques in Food and the Environment
Ambient Mass Spectroscopy Techniques in Food and the Environment

Author: Leo M.L. Nollet

Publisher: CRC Press

Published: 2019-01-30

Total Pages: 431

ISBN-13: 1351378481

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Ambient mass spectrometry—that is the use of mass spec but in the atmospheric environment—has been widely employed in food and environmental analysis. Ambient Mass Spectroscopy Techniques in Food and the Environment presents the theoretical underpinnings of mass spectrometry, and the benefits and pitfalls of ambient mass spectrometry, as well as the latest developments of the technique, in the analysis of food and environmental parameters. It describes methods that enable the detection of surface materials like waxes, alkaloids, flavors, or pesticides by plainly exposing the corresponding items to the ionization region of the interface, without harm to samples. Features: Explains the theoretical aspects of ambient mass spectrometry Describes how to use ambient MS techniques for food safety, authenticity, and traceability screening Lists the benefits of ambient MS in analysis of food and environmental parameters Covers recent developments of ambient MS in analysis of food and environmental parameters The specialized work provides insight to professionals practicing in food and the environment, including food scientists, food engineers, food biotechnologists, chemical engineers, and those working in research labs, universities, and government regulatory agencies.

Understanding the Chemistry of Atmospheric Particles Using Single Particle Mass Spectrometry
Understanding the Chemistry of Atmospheric Particles Using Single Particle Mass Spectrometry

Author: Maria Anna Zawadowicz

Publisher:

Published: 2017

Total Pages: 219

ISBN-13:

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This thesis explores ways in which single particle mass spectrometry can be extended, whether through hardware improvements, or through the use of advanced data processing techniques to provide new kinds of aerosol chemistry measurements. Most of this work has been carried out using the Particle Analysis by Laser Mass Spectrometry (PALMS) instrument, an aircraft deployable mass spectrometer that uses intense (~10^9 Wcm^-2 ) UV laser pulses to vaporize and ionize single particles and measures their mass spectra using a time-of-flight mass spectrometer. Near-term and long-term hardware improvements as well as advanced data analysis techniques are explored in order to extract new chemical information from the thus obtained single particle mass spectra. Hardware improvements to PALMS are explored, such as the use of a high-powered femtosecond laser to obtain single particle mass spectra and a new high resolution compact mass analyzer. Also, a new commercial mass spectrometer LAAPToF is characterized and compared to PALMS. In addition to hardware improvements, novel data analysis techniques for analysis of single particle mass spectra were developed as a part of this work. In particular, a new method to identify biologically-derived particles is presented and used to derive vertical profiles of bioaerosol from near-surface to the upper troposphere.

Novel Techniques and Applications in Single Particle Mass Spectrometry
Novel Techniques and Applications in Single Particle Mass Spectrometry

Author: John Francis Cahill

Publisher:

Published: 2014

Total Pages: 419

ISBN-13: 9781321232462

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In the environment, aerosol particles can affect climate directly though scattering and absorbing radiation and indirectly by influencing cloud formation, albedo, and lifetime. Beyond the environment, aerosols are commonly used as a delivery mechanism for a variety of products, such as inhalers and spray paints. Chemically characterizing aerosols is a difficult endeavor, and relatively few instrumental methods are capable of doing so. A unique subset of instrumentation and techniques exist to measure aerosol chemical and physical properties. Among these, the aerosol time-of-flight mass spectrometer (ATOFMS) can measure single particle chemistry and size in real time. The ATOFMS was developed for the study atmospheric aerosols, and data acquired by the ATOFMS over the years since its creation has provided significant insight into many atmospheric phenomena; however, the application of this technique into disciplines other than atmospheric chemistry has been relatively unexplored. In this dissertation the ATOFMS is used in a conventional sense, to provide insight into atmospheric particle chemistry through two field studies in California, but also in an unconventional way by using the ATOFMS to answer outstanding questions in other disciplines, including nanomaterials and biochemistry. Often the chemistry of a single unit, rather than of the bulk, is needed in these disciplines, and the ATOFMS is uniquely suited to provide this information. The ATOFMS was used to chemically characterize single particles of a unique class of nanomaterials, called metal organic frameworks (MOFs), comprised of functionalized organic linkers and metal ions or metal ion clusters. ATOFMS data was able to show the presence of MOFs with mixed functionality, and show the exchange of functional groups between materials. Cell processes can be monitored by measuring small molecules that are part of cell metabolism, which can provide insight into cell functions, environment, and disease. Using an ATOFMS with a modified aerodynamic lens inlet, single microalgae cells 4-10 μm in diameter of various types have been be characterized. Compared to other single cell mass spectrometry techniques, the modified ATOFMS has unprecedented throughput, up to 50 Hz. Time-resolved measurements of cells undergoing nitrogen deprivation further highlight the abilities of the technique for single cell analysis.

Fundamentals and Applications in Aerosol Spectroscopy
Fundamentals and Applications in Aerosol Spectroscopy

Author: Ruth Signorell

Publisher: CRC Press

Published: 2010-12-20

Total Pages: 513

ISBN-13: 142008562X

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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