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

Catalytic Process Study
 
Author:
Ruijun Hou
Publisher:
Springer
ISBN No: 978-981-10-0773-6
Release at: 2017
Pages: 277
Edition:
First Edition
File Size: 6 MB
File Type: pdf
Language: English



Content of Catalytic Process Study



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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