Document Type

PhD diss.

Date of Degree

2010

Degree Name

PhD (Doctor of Philosophy)

Department

Chemical and Biochemical Engineering

First Advisor

Vicki H. Grassian

Abstract

As commercially manufactured nanomaterials become more commonplace, they have the potential to enter ecological and biological environments sometime during their lifecycle of production, distribution, use or disposal. Despite rapid advances in the production and application of nanomaterials, little is known about how nanomaterials may interact with the environment or affect human health. This research investigates an environmental application of nanomaterials and characterizes the physicochemical properties of commonly manufactured nanomaterials in environmental health and safety studies.

Characterization of nanomaterials for applications and environmental health and safety studies is essential in order to understand how physicochemical properties correlate with chemical, ecological, or biological response or lack of response. Full characterization includes determining the bulk and surface properties of nanomaterials. Bulk characterization methods examine the shape, size, phase, electronic structure and crystallinity, and surface characterization methods include surface area, arrangement of surface atoms, surface electronic structure, surface composition and functionality.

This work investigates the selective catalytic reduction (SCR) of NO2 to N2 and O2 with ammonia on nanocrystalline NaY, Aldrich NaY and nanocrystalline CuY using in situ Fourier transform infrared (FTIR) spectroscopy. It was determined that the kinetics of SCR were 30% faster on nanocrystalline NaY compared to commercial NaY due to an increase in external surface area and external surface reactivity. Copper-cation exchanged nanocrystalline Y resulted in an additional increase in the rate of SCR as well as distinct NO2 and NH3 adsorption sites associated with the copper cation. These superior materials for reducing NOx could contribute to a cleaner environment.

This work consists of characterization of commonly manufactured or synthesized nanomaterials and studies of nanomaterials in specific environmental conditions. Bulk and surface characterization techniques were used to examine carbon nanotubes, titanium dioxide nanoparticles, bare silver nanoparticles and polymer-coated silver nanoparticles, and copper nanoparticles. Lithium titanate nanomaterial was collected from a manufacturing facility was also characterized to identify occupational health risks. Particle size distribution measurements and chemical composition data showed the lithium titanate nanomaterial forms larger micrometer agglomerates, while the nanoparticles present were due to incidental processes.

A unique approach was applied to study particle size during dissolution of nanoparticles in aqueous and acidic conditions. An electrospray coupled to a scanning mobility particle sizer (ES-SMPS) was used to determine the particle size distribution (PSD) of bare silver nanoparticles in nitric acid and copper nanoparticles in hydrochloric acid. The results show unique, size-dependent dissolution behavior for the nanoparticles relative to their micrometer sized counterparts.

This research shows size-dependent properties of nanomaterials can influence how they will be transported and transformed in specific environments, and the behavior of larger sized materials cannot be used to predict nanomaterial behavior. The type of nanomaterial and the media it enters are important factors for determining the fate of the nanomaterial. These studies will be important when considering measures for exposure control and environmental remediation of nanomaterials.

Pages

xiv, 174

Bibliography

160-174

Comments

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Copyright

Copyright 2010 Sherrie Renee Elzey