PhD, University of Cincinnati, 2017, Engineering and Applied Science: Chemical Engineering
The present dissertation work aims at developing of the photocatalysts which have significantly higher activity as well as stability in visible light. In our early steps we have developed a series of photocatalysts based on transition metals (M' = V, Cr, Fe, Co, Mn, Mo, Ni, Cu, Y, Ce, and Zr) incorporated TiO2 (Ti/M' = 20 atomic ratio) materials synthesized by a one-step liquid flame aerosol synthesis technique. Among all the catalysts tested, Cr-doped titania demonstrated a superior catalytic performance with a rate constant about 8-19 times higher than the rest of the metal-doped catalysts. We have optimized the Cr content in TiO2, the system with Ti/Cr atomic ratio 40 proven as a highly effective catalyst. Based on the characterization of the materials and reaction analysis, we proposed plausible reaction pathway for the catalytic activity under visible light conditions.
Next, we studied the effect of leaching and stability of Cr-TiO2 nanoparticles synthesized by flame spray pyrolysis (FSP), co-precipitation, and sol-gel synthesis techniques. The leaching of the Cr into the liquid phase was found to be the primary cause of a reduction in the activity of the catalyst. We developed Si/Ti/Cr catalyst by FSP method which stabilizes and enhances the photocatalytic activity of the catalyst. Unlike the Cr/TiO2 systems, optimal flame-made Cr/Ti/Si catalyst established high efficiency under visible light, stability, and reusability without any Cr leaching even after five consecutive cycles.
In the second half of the work, we successfully developed a novel rapid and continuous process for the synthesis of nitrogen-doped TiO2 (N-TiO2) with flame spray pyrolysis (FSP) equipment. The N incorporation into TiO2 by achieved by simple modification (addition of dilute nitric acid) in the precursor for the synthesis. The N atomic % in the range of 0.09 % to 0.15 % for the primary nitrogen source (nitric acid) has enhanced to remarkable 0.97 % when secondary N source was (open full item for complete abstract)
Committee: Peter Panagiotis Smirniotis Ph.D. (Committee Chair); Anastasios Angelopoulos Ph.D. (Committee Member); Gregory Beaucage Ph.D. (Committee Member); Vesselin Shanov Ph.D. (Committee Member); Makram Suidan Ph.D. (Committee Member)
Subjects: Chemical Engineering