Catalytic and Process Study of the Selective Hydrogenation of Acetylene and 1,3-Butadiene (PDF)

Catalytic Process Study

Author:
Ruijun Hou
Release at: 2017
Pages: 277
Edition:
First Edition
File Size: 6 MB
File Type: pdf
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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