Aerosolization and Atmospheric Transformation of Engineered Nanoparticles

dc.contributor.authorTiwari, Andrea Jeanen
dc.contributor.committeechairMarr, Linsey C.en
dc.contributor.committeememberVikesland, Peter J.en
dc.contributor.committeememberHochella, Michael F. Jr.en
dc.contributor.committeememberMorris, John R.en
dc.contributor.departmentCivil and Environmental Engineeringen
dc.date.accessioned2015-09-28T15:22:38Zen
dc.date.available2015-09-28T15:22:38Zen
dc.date.issued2014-04-04en
dc.description.abstractWhile research on the environmental impacts of engineered nanoparticles (ENPs) is growing, the potential for them to be chemically transformed in the atmosphere has been largely ignored. The overall objective of this work was to assess the atmospheric transformation of carbonaceous nanoparticles (CNPs). The research focuses on C₆₀ fullerene because it is an important member of the carbonaceous nanoparticle (CNP) family and is used in a wide variety of applications. The first specific objective was to review the potential of atmospheric transformations to alter the environmental impacts of CNPs. We described atmospheric processes that were likely to physically or chemically alter aerosolized CNPs and demonstrated their relevance to CNP behavior and toxicity in the aqueous and terrestrial environment. In order to investigate the transformations of CNP aerosols under controlled conditions, we developed an aerosolization technique that produces nano-scale aerosols without using solvents, which can alter the surface chemistry of the aerosols. We demonstrated the technique with carbonaceous (C₆₀) and metal oxide (TiO₂, CeO₂) nanoparticle powders. All resulting aerosols exhibited unimodal size distributions and mode particle diameters below 100 nm. We used the new aerosolization technique to investigate the reaction between aerosolized C₆₀ and atmospherically realistic levels of ozone (O₃) in terms of reaction products, reaction rate, and oxidative stress potential. We identified C₆₀O, C₆₀O2, and C₆₀O3 as products of the C₆₀-O3 reaction. We demonstrated that the oxidative stress potential of C₆₀ may be enhanced by exposure to O3. We found the pseudo-first order reaction rate to be 9 x 10⁻⁶ to 2 x 10⁻⁵ s⁻¹, which is several orders of magnitude lower than the rate for several PAH species under comparable conditions. This research has demonstrated that a thorough understanding of atmospheric chemistry of ENPs is critical for accurate prediction of their environmental impacts. It has also enabled future research in that vein by developing a novel technique to produce nanoscale aerosols from nanoparticle powders. Results of this research will help guide the formulation of appropriate environmental policy concerning the regulation of ENPs.en
dc.description.degreePh. D.en
dc.format.mediumETDen
dc.identifier.othervt_gsexam:2544en
dc.identifier.urihttp://hdl.handle.net/10919/56664en
dc.publisherVirginia Techen
dc.rightsIn Copyrighten
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/en
dc.subjectAerosolen
dc.subjectnanoparticleen
dc.subjectatmosphereen
dc.titleAerosolization and Atmospheric Transformation of Engineered Nanoparticlesen
dc.typeDissertationen
thesis.degree.disciplineCivil Engineeringen
thesis.degree.grantorVirginia Polytechnic Institute and State Universityen
thesis.degree.leveldoctoralen
thesis.degree.namePh. D.en

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