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A Kinetic Study on the Adsorption and Reaction of Hydrogen over Silica-supported Ruthenium and Silver-ruthenium Catalysts during the Hydrogenation of Carbon Monoxide - 1999

VanderWiel, David

Iowa State University

Table of Contents

  List of Figures vi
List of Tables viii
Section 1
814kb

1

 Research Objectives 1

2

 Introduction 4

3

 Hydrogenation of Carbon Monoxide 7
 

3.1

 Mechanism and Kinetics 9
  3.1.1 Fischer-Tropsch Synthesis 9
3.1.2 Methanation 12
3.1.3 Transition State Theory 15
3.2 Adsorption of Carbon Monoxide 16
3.3 Adsorption of Hydrogen 18
3.4 Coadsorption of Hydrogenation and Carbon Monoxide 19
Section 2
728kb		 3.5 Surface Structure Sensitivity 20
  3.5.1 Reaction Sensitivity 20
3.5.2 Adsorption Sensitivity 21

3.6

 Bimetallic Ruthenium Catalysts 21

4

 Experimental Techniques 25
  4.1 Preadsorbed CO Reaction Techniques 25
4.2 Catalyst Preparation 27
4.3 Dispersion Measurements 28
4.4 H-NMR Experimentation 29
4.5 Catalyst Pretreatment 29
4.6 Experimental Apparatus 30
4.7 Experimental Reaction Methods 32
4.8 Data Anaylsis 33
Section 3
381kb

5

 Results 36
 

5.1

 Results for Ru/SiO2 Catalysts 36
  5.1.1 Preliminary Experimentation 36
5.1.2 Methanation Reactions 37
5.1.3 Kinetic Parameters 40
5.1.4 H-NMR Experimentation 42

5.2

 Results for Ag-Ru/SiO2 Catalysts 47
  5.2.1 Methanation Reactions 47
5.2.2 Kinetic Parameters 50
Section 4
702kb

6

 Discussion of Results 53
 

6.1

 Discussion of Results for Ru/SiO2 Catalysts 53
  6.1.1 Preliminary Experimentation 53
6.1.2 Methanation Reactions 54
6.1.3 Kinetic Parameters 55
6.1.4 H-NMR Experimentation 55

6.2

 Discussion of Results for Ag-Ru/SiO2 Catalysts 57
  6.2.1 Methanation Reactions 57
6.2.2 Kinetic Parameters 58

7

 Portal Site Mediated Hydrogen Adsorption 64
Section 5
277kb

8

 Summary and Conclusions 69
Appendix 71
Section 6
339kb		 References 87
Acknowledgements 94
Biographical Sketch 95