| Author: |
Ruijun Hou
|
| Release at: | 2017 |
| Pages: | 277 |
| Edition: |
First Edition
|
| File Size: | 6 MB |
| File Type: | |
| Language: | English |
Description of Catalytic and Process Study of the Selective Hydrogenation of Acetylene and 1,3-Butadiene (PDF)
Catalytic and Process Study of the Selective Hydrogenation of Acetylene and 1,3-Butadiene by Ruijun Hou is a research book available in (PDF) download. The series “Catalytic and Process Study of the Selective Hydrogenation of Acetylene and 1,3-Butadiene Theses” brings together a selection of the very best Ph.D. theses from around the world and across the physical sciences. Nominated and endorsed by two recognized specialists, each published volume has been selected for its scientific excellence and the high impact of its contents for the pertinent field of research. For greater accessibility to non-specialists, the published versions include an extended introduction, as well as a foreword by the student’s supervisor explaining the special relevance of the work for the field.
As a whole, the series will provide a valuable resource both for newcomers to the research fields described, and for other scientists seeking detailed background information on special questions. Finally, it provides an accredited documentation of the valuable contributions made by today’s younger generation of scientists.
Content of Catalytic and Process Study of the Selective Hydrogenation of Acetylene and 1,3-Butadiene (PDF)
1 Introduction. 1
1.1 Background 1
1.1.1 Purification of C2–C4 Olefins. 1
1.1.2 Production of Ethylene from Acetylene 2
1.2 Properties of Selective Hydrogenation Reactions . 3
1.3 Industrial Processes 3
1.4 Progress in Catalyst Development 6
1.4.1 Reaction Mechanism on Pd Catalyst 6
1.4.2 Influencing Factors on Pd-Based Catalysts 12
1.4.3 Pd-Based Bimetallic Catalysts. 17
1.4.4 Non-Pd Catalysts 19
1.5 Thesis Outline 20
References 21
2 Experimental and Theoretical Methods 31
2.1 Chemicals and Instruments 31
2.2 Measurements of Model Surfaces. 31
2.2.1 Ultra-High Vacuum (UHV) System 31
2.2.2 Preparation of Single-Crystal Surfaces 31
2.2.3 Temperature-Programmed Desorption (TPD) . 33
2.3 Density Functional Theory (DFT) Calculations 34
2.4 Catalyst Preparation 34
2.4.1 Supported Catalyst 34
2.4.2 Mo2C-Based Catalyst . 35
2.5 Catalyst Characterization . 35
2.5.1 SEM 35
2.5.2 TEM 36
2.5.3 XRD 36
2.5.4 TG-DTA 36
2.5.5 Physisorption 36
2.5.6 CO-Chemisorption 36
2.5.7 XAFS . 37
2.6 Catalyst Evaluation 38
2.6.1 Batch Reactor . 38
2.6.2 Fixed-Bed Reactor 40
2.6.3 Slurry Reactor. 41
2.7 Measurement of Solubility 41
References 42
3 Selective Hydrogenation of 1,3-Butadiene on Pd–Ni Bimetallic
Catalyst: From Model Surfaces to Supported Catalysts 45
3.1 Introduction 45
3.2 DFT Calculation 47
3.2.1 Adsorption Energy 47
3.2.2 Activation Barrier . 47
3.3 UHV Results . 49
3.3.1 Preparation of Single-Crystal Surfaces 49
3.3.2 TPD Results 52
3.4 Characterization of Supported Catalysts 55
3.4.1 TEM 56
3.4.2 CO Chemisorption 56
3.4.3 XAFS . 56
3.5 Evaluation of Supported Catalysts 60
3.5.1 Batch Reactor . 60
3.5.2 Fixed-Bed Reactor 63
3.6 Discussion 66
3.7 Conclusion 68
References 69
4 Effect of Oxide Supports on Pd–Ni Bimetallic Catalysts
for 1,3-Butadiene Hydrogenation 73
4.1 Introduction 73
4.2 Catalyst Characterization . 74
4.2.1 TEM 74
4.2.2 CO Chemisorption 74
4.2.3 Temperature Programmed Reduction (TPR) 76
4.2.4 XAFS . 77
4.3 Catalyst Evaluation 79
4.3.1 Bimetallic Effect 79
4.3.2 Hydrogenation Activity 81
4.3.3 Selectivity . 82
4.4 Discussion 84
4.4.1 Bimetallic Effect 84
4.4.2 Support Effect . 84
4.5 Conclusion 86
References 87
5 Replacing Precious Metals with Carbide Catalysts for
Hydrogenation Reactions 89
5.1 Introduction 89
5.2 Catalyst Characterization . 90
5.3 Mo2C for the Hydrogenation of Dienes 92
5.3.1 1,3-Butadiene . 93
5.3.2 1,3-Cyclohexadiene 94
5.3.3 1,4-Cyclohexadiene 95
5.4 Ni/Mo2C for the Hydrogenation of 1,3-Butadiene 97
5.5 Discussion 98
5.5.1 Hydrogenation Activity and Stability . 98
5.5.2 Selectivity . 101
5.5.3 Potential Advantage in Cost Reduction 103
5.6 Conclusion 104
References 104
6 Selective Hydrogenation of Acetylene in Liquid Phase: A Novel
Process 107
6.1 Introduction 107
6.2 Catalyst Characterization . 109
6.3 Optimization of Operation Parameters 110
6.3.1 Effect of Temperature . 111
6.3.2 Effect of GHSV 113
6.3.3 Effect of H2/C2H2 Ratio 114
6.3.4 Comparison with Gas-Phase Reaction . 117
6.4 Solvent Effect . 118
6.4.1 Selective Solubility 118
6.4.2 Viscosity 119
6.5 Induction Period 121
6.6 Catalyst Stability 122
6.7 Solid Catalyst with Ionic Liquid Layer and Comparison (SCILL) 124
6.7.1 A General Comparison 124
6.7.2 Selectivity . 126
6.7.3 Stability 126
6.7.4 Discussion. 129
6.8 Process Optimization and Reactor Design 131
6.8.1 Two-Stage Slurry Reactor . 132
6.8.2 Pressure Effect. 132
6.8.3 Design of Multi-Stage Reactor 134
6.9 Conclusion 135
References 136
7 Conclusions . 139
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