Section 1
292kb |
Acknowledgments |
ii |
Abstract |
iii |
List of Figures |
ix |
List of Tables |
xiv |
1.0 |
Introduction |
1 |
2.0 |
Background |
6 |
|
2.1 |
CO Hydrogenation |
6 |
|
2.1.1 |
Nature of the Selectivity Problem in F-T Synthesis |
6 |
Section 2
275kb |
2.1.2 |
Product Selectivity Control |
10 |
2.2 |
Zeolite-Supported Metals |
10 |
2.3 |
Zeolite Catalyzed Reactions |
16 |
2.4 |
Diffusion in Zeolites |
20 |
3.0 |
Experimental |
21 |
|
3.1 |
Materials |
21 |
|
3.1.1 |
Preparation of Fully-Exchanged Alkali Zeolites |
21 |
3.1.2 |
Preparation of Zeolite-Supported Ru Catalysts |
21 |
3.1.3 |
Preparation of FuSiO2 |
22 |
3.1.4 |
Preparation of Partially-Exchanged Alkali Y-Zeolites |
23 |
Section 3
227kb |
3.2 |
Catalyst Characterization |
24 |
|
3.2.1 |
Atomic Absorption |
24 |
3.2.2 |
Chemisorption |
26 |
3.2.3 |
X-Ray Diffraction |
29 |
3.3 |
Reaction Studies |
29
|
|
3.3.1 |
Experimental Setups and Procedures |
29 |
|
3.3.1.1 |
CO Hydrogenation |
29 |
3.3.1.2 |
Hydrocarbon Reactions |
31 |
3.3.2 |
Product Analysis |
33 |
3.3.3 |
Activity and Selectivity Determination |
34 |
|
3.3.3.1 |
CO Hydrogenation |
34 |
3.3.3.2 |
Olefin Reactions |
35 |
Section 4
374kb |
4.0 |
Characterization of Zeolite-Supported Ru
Catalysts |
37 |
|
4.1 |
Chemical Composition and Structural Character
of the Zeolites |
37 |
4.2 |
H2 and CO Chemisorption |
40 |
4.3 |
Effect of Decomposition/Reduction Conditions |
48 |
|
4.3.1 |
Introduction |
48 |
4.3.2 |
Experimental |
49 |
4.3.3 |
Results and Discussion |
50 |
4.3.4 |
Conclusion |
55 |
Section 5
451kb |
5.0 |
Effect of Group IA Cations on CO Hydrogenation
Over Ru/Y-Zeolites |
58 |
|
5.1 |
Introduction |
58 |
5.2 |
Experimental |
59 |
5.3 |
Results and Discussion |
59 |
|
5.3.1 |
Catalytic Activity |
59 |
5.3.2 |
Methane Selectivity and Chain Growth
Probability |
69 |
5.3.3 |
Olefin Fraction |
73 |
Section 6
288kb |
5.3.4 |
Structural Isomerization |
83 |
5.4 |
Conclusions |
85 |
6.0 |
Secondary Reactions During CO
Hydrogenation on Zeolite-Supported Metal Catalysts: Influence of Alkali
Cations |
87 |
|
6.1 |
Introduction |
87 |
6.2 |
Experimental |
89 |
|
6.2.1 |
Materials |
89 |
6.2.2 |
Reaction Studies |
89 |
6.3 |
Results and Discussion |
91 |
|
6.3.1 |
CO Hydrogenation |
91 |
6.3.2 |
Olefin Reactions Over Alkali
Y-Zeolites |
96 |
Section 7
332kb |
6.3.3 |
Olefin Reactions Over
Partially-Exchanged HY-Zeolites |
99 |
6.4 |
Conclusion |
116 |
Section 8
350kb |
7.0 |
Secondary Reactions During CO
Hydrogenation on Zeolite-Supported Metal Catalysts: Effect of
Si/Al Ratio |
118 |
|
7.1 |
Introduction |
118 |
7.2 |
Experimental |
119 |
|
7.2.1 |
Materials |
119 |
7.2.2 |
Reaction Studies |
119 |
7.3 |
Results and Discussion |
120 |
|
7.3.1 |
Catalyst Activites for CO
Hydrogenation |
120 |
7.3.2 |
Catalyst Selectivites in CO
Hydrogenation |
124 |
7.3.3 |
Olefin Reactions on the Zeolites
without Ru |
134 |
7.3.4 |
Deactivation Characteristics of
H-mordenite and HY-zeolite |
137 |
Section 9
178kb |
7.4 |
Conclusion |
141 |
8.0 |
Summary |
142
|
|
Appendix A 258kb |
147 |
Appendix B 182kb |
186 |
Appendix C 56kb |
197 |
Bibliography 375kb |
208 |