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The Fischer-Tropsch Synthesis in Slurry Phase Reactors - Kinetics and Mass Transfer - 1988

Boelee, J. H.

Technische Universiteit Eindhoven

Table of Contents 161kb

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