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Implications of the Use of Cerium Oxide Nanoparticle Diesel Fuel-Borne Catalysts: From Transformation During Combustion Through Exposure to Plants and Soils
Dale, James G
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The fate of nanoparticulate cerium oxide from the diesel fuel catalyst Envirox was studied from its presence in the additive to its transformations during combustion through its exposure to plants and soils using a broad range of analytical techniques. Envirox is a fuel-borne catalyst comprised of nanoparticles of cerium oxide suspended in kerosene. The particles suspended in Envirox were confirmed by synchrotron X-ray diffraction, dynamic light scattering, and electron microscopy to be 5-7 nm crystals of CeO2 present as 15 nm aggregates. Significant changes to the particles were induced by the combustion process, resulting in 50-300 nm euhedral crystals of CeO2 in the exhaust as discovered using high resolution transmission electron microscopy. Single particle electron diffraction of the emitted cerium oxide particles showed evidence of ordered oxygen vacancies, indicative of a superstructure. Variations in the engine operating load resulted in no significant differences in the emitted cerium oxide particles. The mobility through soils and impacts on the plant Brassica napus (dwarf essex rape) of the emitted cerium oxide were compared to small and large CeO2 nanoparticles as well as diesel particulate matter emissions with very low cerium. The small CeO2 nanoparticles exhibited high mobility through soils and significant uptake and translocation in the plants. The large CeO2 nanoparticles showed extremely low mobility in soils and no significant increase in cerium anywhere in the plants. Cerium emissions from a diesel engine utilizing Envirox was found to have moderate mobility through the soils as well as an increased association with the roots of the plants, though translocation of the cerium into the aboveground biomass was not statistically significant. Despite uptake and translocation of some materials by B. napus, exposure to these cerium sources at 100 ppm Ce in the topsoil showed no significant impacts on the growth or overall health of the plants when compared to unexposed control samples. This dissertation shows that CeO2 nanoparticles employed as catalysts suspended in diesel fuel are altered during their use resulting in changes to their mobility and interaction upon entering the environment. This dissertation lays the groundwork for a new approach to nanotoxicology.
- Doctoral Dissertations