Monday, June 16, 2008 - 1:20 PM
Room 7b (McKimmon Conference Center)
109

Photocatalyzed Soot Oxidation on Titanium Dioxide Thin Films

Paul Chin, Christine S. Grant, and David F. Ollis. North Carolina State University, Raleigh, NC

We developed earlier1 a series/parallel kinetic model for direct photocatalytic soot oxidation by thin films of TiO2 and successfully used it to analyze the experimental CO2 generation data of Mills et al.2 and the soot mass loss data of Lee and Choi3. The model assumes two oxidation pathways: a single step yielding CO2 directly, and a serial sequence through a solid intermediate species, which is subsequently oxidized to CO2.

In the present work, laboratory studies of photocatalyzed soot oxidation are conducted using a quartz crystal microbalance (QCM). Hurricane lamp soot is deposited on TiO2-coated quartz crystals using a controlled, reproducible analytical rotator. The TiO2 film is characterized using atomic force microscopy, x-ray diffraction, and ellipsometry, whereas the soot film is described by UV-Vis spectroscopy.

Following each interval of photocatalyzed oxidation, the measured QCM frequency shifts are related to the change in adherent soot mass using the Sauerbrey equation4. The mass of TiO2 and soot are varied to determine their effects on the rate of soot photooxidation. We test our series/parallel reaction mechanism to fit our data.
 

Figure 1: Representative visual example of soot photocatalytic oxidation on TiO2 films at (a) 0 minutes and (b) 11,000 minutes of UV illumination

(a)

(b)

 

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1 Chin, P.; Roberts, G. W.; Ollis, D. F. Ind. Eng. Chem. Res. 2007, 46, 7598-7604.

2 Mills, A.; Wang, J.; Crow, M. Chemosphere 2006, 64, 1032-1035.

3 Lee, N. C.; Choi, W. Y. J. Phys. Chem. B 2002, 106, 11818-11822.

4 Sauerbrey, G. Z. Phys. 1959, 155, 206-222.