Aerosolization and Atmospheric Transformation of Engineered Nanoparticles

While 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.

Name thesis:degree_name

Ph. D.

Level thesis:degree_level

doctoral

Discipline thesis:degree_discipline

Civil Engineering

Department dc:contributor.department

Civil and Environmental Engineering

Grantor dc:publisher

Virginia Tech

Year dc:date.issued

2014

Author dc:creator

• Tiwari, Andrea Jean

Chair dc:contributor.committeechair

• Marr, Linsey C.

Committee members dc:contributor.committeemember

• Vikesland, Peter J.
• Hochella, Michael F. Jr.
• Morris, John R.

• Aerosol
• nanoparticle
• atmosphere

Statement dc:rights

• In Copyright

Licence dc:rights.uri

• http://rightsstatements.org/vocab/InC/1.0/

Dc Identifier Other

vt_gsexam:2544

OAI identifier oai:identifier

oai:vtechworks.lib.vt.edu:10919/56664