Section 1
486kb |
Summary |
7 |
1 |
Introduction |
14 |
|
1.1 |
Alternatives to crude oil as chemical
feedstock |
14 |
1.2 |
The use of a slurry reactor for the Fischer-Tropsch
synthesis |
15 |
1.3 |
Aim and outline of this investigation |
17 |
References |
18 |
2 |
Catalytic Performance of Potassium Promoted
Fused Iron in the Slurry Phase |
19 |
|
2.1 |
Introduction |
19 |
2.2 |
Materials and catalyst |
19 |
2.3 |
Apparatus |
20 |
2.4 |
Accumulation of hydrocarbons in a stirred
laboratory slurry reactor |
23 |
|
2.4.1 |
Introduction |
23 |
2.4.2 |
Theoretical and experimental results |
23 |
2.4.3 |
Conclusion |
28 |
2.5 |
The importance of the water-gas shift activity
for the performance of Fischer-Tropsch catalysts |
28 |
2.6 |
The water-gas shift activity of potassium
promoted fused iron |
32 |
|
2.6.1 |
Introduction |
32 |
2.6.2 |
Experimental |
32 |
2.6.3 |
Results and discussion |
33 |
2.6.4 |
Conclusion |
36 |
Section 2
413kb |
2.7 |
Product distribution |
37 |
|
2.7.1 |
Introduction |
37 |
2.7.2 |
Experimental |
41 |
2.7.3 |
Results |
42 |
2.7.4 |
Discussion |
49 |
2.7.5 |
Conclusions |
52 |
2.8 |
Kinetics of the conversion of synthesis gas |
52 |
|
2.8.1 |
Introduction |
52 |
Section 3
467kb |
2.8.2 |
Experimental |
57 |
2.8.3 |
Results and discussion |
57 |
2.8.4 |
Conclusion |
68 |
2.9 |
Olefin selectivity |
68 |
|
2.9.1 |
Introduction |
68 |
2.9.2 |
Competition model for the olefin selectivity
in a well-mixed slurry reactor |
70 |
2.9.3 |
Experimental |
73 |
2.9.4 |
Results and discussion |
73 |
Section 4
452kb |
2.9.5 |
Conclusions |
83 |
2.10 |
Isomerization |
84 |
|
2.10.1 |
Introduction |
84 |
2.10.2 |
Competition model for both hydrogenation and
isomerization |
86 |
2.10.3 |
Experimental |
88 |
2.10.4 |
Results and discussion |
88 |
2.10.5 |
Conclusions |
90 |
2.11 |
Olefin selectivity as a function of carbon
number |
91 |
2.12 |
The effect of co-feeding of ethene on the
activity and selectivity under various reaction conditions |
96 |
|
2.12.1 |
Introduction |
96 |
2.12.2 |
Experimental |
99 |
2.12.3 |
Results |
99 |
2.12.4 |
Conclusions |
105 |
Section 5
535kb |
2.13 |
Long-term performance of fused iron with 0.55
H2/CO feed ratio |
107 |
|
2.13.1 |
Introduction |
107 |
2.13.2 |
Experimental |
107 |
2.13.3 |
Results and discussion |
108 |
2.13.4 |
Conclusions |
112 |
2.14 |
Discussion |
114 |
Symbols |
116 |
References |
117 |
3 |
The Performance of RuFe/SiO2 and Ru/SiO2
at High Pressure During an Extented Run |
121 |
|
3.1 |
Introduction |
121 |
3.2 |
Experimental |
123 |
|
3.2.1 |
Catalyst preparation and apparatus |
123 |
3.2.2 |
Experiments |
124 |
3.3 |
Results |
127 |
|
3.3.1 |
The activity of RuFe/SiO2 and Ru/SiO2 |
127 |
Section 6
442kb |
3.3.2 |
Comparison of RuFe/SiO2 and Ru/SiO2 |
134 |
3.3.3 |
Comparison of RuFe/SiO2 , Ru/SiO2
and fused iron |
135 |
3.3.4 |
Kinetic model for RuFe/SiO2 |
136 |
3.3.5 |
Kinetic model for Ru/SiO2 |
142 |
3.3.6 |
Product distribution over RuFe/SiO2 |
143 |
3.3.7 |
Product distribution over Ru/SiO2
and comparison with RuFe/SiO2 |
146 |
3.3.8 |
Olefin selectivity for RuFe/SiO2 |
150 |
3.3.9 |
Olefin selectivity for Ru/SiO2 |
156 |
3.3.10 |
Comparison of the olefin selectivity over RuFe/SiO2
and fused iron |
158 |
Section 7
494kb |
3.3.11 |
The olefin selectivity observed with other
bimetallic catalysts |
160 |
3.3.12 |
Mössbauer analysis |
162 |
|
3.3.12.1 |
Introduction |
162 |
3.3.12.2 |
Experimental |
162 |
3.3.12.3 |
Results and discussion |
163 |
3.4 |
Discussion |
165 |
Appendix 1 |
167 |
References |
169 |
4 |
Gas-Liquid Mass Transfer in a Slurry Bubble
Column Reactor at Fischer-Tropsch Conditions |
171 |
|
4.1 |
Introduction |
171 |
4.2 |
The resistance in series in model |
172 |
4.3 |
Calculation of kLa from conversion
date |
177 |
4.4 |
Choice of the reactor models |
182 |
4.5 |
Choice of model reaction |
184 |
Section 8
489kb |
4.6 |
Experimental |
185 |
|
4.6.1 |
Material and catalyst |
185 |
4.6.2 |
Apparatus |
185 |
4.7 |
Results and discussion |
187 |
|
4.7.1 |
Effect of the gas distributor |
187 |
4.7.2 |
Effect of the liquid/suspension level |
192 |
4.7.3 |
The effect of solids on the gas holdup and
volumetric mass transfer. |
194 |
4.8 |
The importance of gas-liquid mass transfer
limitations to the Fischer-Tropsch slurry proces |
203 |
Symbols |
208 |
References |
209 |
Section 9
446kb |
5 |
The Effect of the Conversion Level and
Recycling of Product Gas on the Olefin Selectivity over Potassium
Promoted Fused-Iron in a Bubble Column |
212 |
|
5.1 |
Introduction |
212 |
5.2 |
Modelling of a bubble column with recycling of
product gas |
212 |
5.3 |
Experimental |
217 |
|
5.3.1 |
Materials and catalyst |
217 |
5.3.2 |
Apparatus |
217 |
5.4 |
Results and discussion |
219 |
5.5 |
Conclusions |
225 |
Symbols |
226 |
Samenvatting |
227 |
Dankwoord |
230 |
Curriculum vitae |
231 |