Date of Award

2-1-2009

Degree Type

Thesis

University or Center

Clark Atlanta University(CAU)

School

School of Arts and Sciences

Degree Name

M.S.

Department of Chemistry

First Advisor

Dr. Conrad W. Ingram

Second Advisor

Dr. Issifu L. Harruna

Third Advisor

Dr. Cass D. Parker

Abstract

Following the methodology used in sol—gel chemistry to functionalize amorphous silica, organic functionalized mesoporous silica were prepared by the co-condensation of tetraethoxysilane and organoalkoxysilanes in the presence of surfactant templates. A series of titanium catalysts containing Ti-MCM-41 with different bridging and pendant organic functional groups (such as methyl triethoxysilane (MTEOS), phenyl triethoxysilane (PTEOS), diphenyl triethoxysilane (DPTEOS), bis (triethoxysilyl) ethane (BTSE), 1,4 bis(triethoxysiyl) benzene (BTSB), bis( triethoxysilyl) biphenyl (BTSDP) and two catalysts with different organic-inorganic ratios (90% TEOS with 10% phenyl, 70% TEOS with 30% phenyl) were synthesized. The catalysts were characterized by elemental analysis, XRD, FTIR, UVDRS, by solid state 13C and 29Si MAS NMR, and BET surface area analysis. The catalytic activities of the synthesized materials were evaluated for epoxidation of cyclohexene with TBIIP. The materials yielded improved conversion compared to the conversion results obtained from the traditional titanium containing mesoporous silica (Ti-MCM-41). The hydrophobic character of the synthesized catalysts was tested in the epoxidation of cyclohexene by using wet TBIIP.

Ti-MCM41 with bridged organosilane showed almost the same conversion in the presence of water, while for Ti-MCM-41 with organosilane pendant groups. conversion decreased almost 36%. This implies that the silylation of the surface ofTi-MCM4I protected the active sites. The effect of substrate: oxidant molar ratio in these reactions were studied and high conversion, high selectivity were achieved at 1:1 molar ratio.


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