ISOTOPES IN HETEROGENEOUS CATALYSIS (V4)

By: JUSTIN S J HARGREAVES

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Hardcover | 12 April 2006

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306 Pages

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The purpose of this book is to review the current, state-of-the-art application of isotopic methods to the field of heterogeneous catalysis. Isotopic studies are arguably the ultimate technique in in situ methods for heterogeneous catalysis. In this review volume, chapters have been contributed by experts in the field and the coverage includes both the application of specific isotopes - Deuterium, Tritium, Carbon-14, Sulfur-35 and Oxygen-18 - as well as isotopic techniques - determination of surface mobility, steady state transient isotope kinetic analysis, and positron emission profiling.

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Non-Fiction Science Chemistry Physical Chemistry Nuclear Chemistry Analytical Chemistry Biographies & True Stories Biographies Engineering & Technology Biochemical Engineering Booktopia Publisher Services World Scientific Publishing

Contributors	p. xi
Preface	p. xiii
Deuterium-Labelling in Mechanistic Studies on Heterogeneous Acid-Base Catalysts	p. 1
Introduction	p. 1
H/D Exchange in the Strongest Liquid Superacids	p. 2
H/D Exchange between Alkanes and Solid Acid Catalysts	p. 5
The number of exchangeable acid sites on the catalyst	p. 5
H/D exchange with methane and ethane	p. 10
H/D exchange with alkanes having more than 2 carbon atoms	p. 13
The case of propane	p. 19
Competitive reactions evidenced by H/D exchange	p. 23
Molecular rearrangement	p. 23
Deactivation of acidic catalysts	p. 23
The inhibiting effect of CO	p. 25
Conclusion	p. 25
Application of [superscript 14]C Radiotracer for the Study of Heterogeneous Catalytic Reactions	p. 31
Introduction	p. 31
Investigation of Reaction Pathways by Using Mixtures Containing Labelled Reactant	p. 32
Hydrocarbon cracking and isomerisation over acidic catalysts	p. 32
Formation and rupture of C[subscript 5]-cyclic hydrocarbons	p. 39
Aromatisation of branched alkanes	p. 40
Study of Reaction Kinetics by Isotope Tracer	p. 44
Benzene hydrogenation	p. 45
The kinetic isotope method	p. 46
Reaction Pathway Studies by the Determination of the Position of the Label	p. 48
Dehydrocyclisation	p. 50
Skeletal transformations of cyclic hydrocarbons	p. 51
Fischer-Tropsch synthesis	p. 53
[superscript 14]C Tracers - Past or Future?	p. 58
Use of [superscript 35]S Radiotracer in Catalytic Studies	p. 63
Catalyst Sulfur Uptake	p. 66
Single crystals	p. 66
Non-supported catalysts	p. 67
Supported catalysts	p. 69
Catalysts' Sulfur Mobility	p. 74
Catalyst sulfur exchange with hydrogen sulphide	p. 75
Sulfur exchange via thiophene HDS	p. 79
Sulfur exchange via HDS of thioaromatic compounds	p. 83
On the Role of Catalyst Sulfur in Catalytic Hydrodesulfurisation: Some Conclusions from Tracer Studies	p. 86
On the mechanism of sulfur exchange	p. 87
On the reaction mechanism of desulfurisation	p. 88
Tritium in Catalysis	p. 97
Introduction	p. 97
Radiochemical Facilities	p. 98
Tritiation Procedures	p. 106
Discussion	p. 107
Conclusion	p. 111
Acknowledgements	p. 112
Isotopic Exchange of Oxygen Over Oxide Surfaces	p. 115
Introduction	p. 115
Activity Patterns	p. 118
Nature of the Exchange Site	p. 126
Conclusion	p. 130
Oxygen and Hydrogen Surface Mobility in Supported Metal Catalysts. Study by [superscript 18]O/[superscript 16]O and [superscript 2]H/[superscript 1]H Exchange	p. 133
Introduction	p. 134
Measurement of Surface Diffusion by Isotopic Exchange	p. 135
Overview	p. 135
Mechanisms of isotopic exchange of oxygen on oxides	p. 136
Definitions	p. 136
Kinetics of the exchange between a gas and a monophasic solid	p. 137
Mechanisms of isotopic exchange of oxygen on oxide-supported catalysts	p. 138
Isotopic heteroexchange on supported metal catalysts general parameters	p. 139
Mechanism and kinetic conditions	p. 139
Determination of the rate of exchange	p. 141
Initial rates of exchange	p. 142
Numbers of exchanged and of exchangeable atoms	p. 143
Isotopic heteroexchange on supported metal catalysts kinetics	p. 144
Exchange is controlled by adsorption-desorption of X[subscript 2] on the metal	p. 144
Exchange is controlled by the metal to support transfer	p. 145
Exchange is controlled by the surface diffusion on the support	p. 147
Exchange is controlled by bulk diffusion into the support	p. 148
Isotopic homoexchange on supported metal catalysts	p. 149
Mechanisms	p. 150
Kinetics	p. 151
Surface Diffusion of Hydrogen and Oxygen	p. 153
Overview	p. 153
[superscript 1]H[subscript 2]/[superscript 2]H[subscript 2] and [superscript 16]O[subscript 2]/[superscript 18]O[subscript 2] homoexchange on metals	p. 154
[superscript 1]H[subscript 2]/[superscript 2]H[subscript 2] equilibration	p. 154
[superscript 16]O[subscript 2]/[superscript 18]O[subscript 2] equilibration	p. 156
[superscript 2]H[subscript 2]/[superscript 1]H[subscript S] and [superscript 18]O[subscript 2]/[superscript 16]O[subscript S] heteroexchange on supports	p. 159
[superscript 2]H[subscript 2] exchange with [superscript 1]H[subscript S] species of oxides	p. 159
[superscript 18]O[subscript 2] exchange with [superscript 16]O[subscript S] species of oxides	p. 163
Surface diffusion of hydrogen species on supported metal catalysts	p. 166
[superscript 2]H[subscript 2] heteroexchange with [superscript 1]H species of alumina in the presence of metals	p. 166
Hydrogen exchange on other supports	p. 169
Surface diffusion of oxygen species on supported metal catalysts	p. 170
Comparison between H and O surface diffusion	p. 172
Recent Developments of [superscript 16]O/[superscript 18]O Isotopic Exchange: Case of Oxides with Very High Oxygen Mobility	p. 174
Investigation of Reaction at the Site Level Using SSITKA	p. 183
Introduction	p. 183
Theory	p. 184
Advanced Mathematical Analysis	p. 190
Deconvolution	p. 190
Convolution	p. 191
Experimental Limitations and Corrective Techniques	p. 193
H[subscript 2]-D[subscript 2]	p. 193
O[subscript 2]	p. 194
Readsorption	p. 194
Steady-state versus non-steady-state analysis	p. 196
Applications	p. 197
TOF on metals	p. 197
Cause of deactivation	p. 198
Effects of promotion	p. 199
Effect of alloying	p. 200
Acid catalysis	p. 201
High temperature reaction	p. 203
Effect of temperature	p. 204
Effect of partial pressure of reactant	p. 206
Summary	p. 206
Positron Emission Profiling - The Ammonia Oxidation Reaction as a Case Study	p. 213
Introduction	p. 213
Positron emission and positron-electron annihilation	p. 214
Positron emission detection methods	p. 216
Positron Emission Tomography (PET), Particle Tracking (PEPT) and Profiling (PEP)	p. 217
The TU/e PEP detector	p. 219
Synthesis of Radio-labelled Molecules	p. 222
[superscript 13]NH[subscript 3] production	p. 223
Positron Emission Profiling Study on the Catalytic Ammonia Oxidation	p. 224
Activation of ammonia dissociation on Pt	p. 225
Experimental details	p. 226
Activation of ammonia adsorption by oxygen	p. 226
Influence of temperature on the ammonia dissociation on pre-oxidised Pt	p. 228
Determination of adsorbed species by temperature programmed desorption	p. 230
Determination of adsorbed species by temperature programmed oxidation	p. 232
Reaction of adsorbed N species with H[subscript 2], NH[subscript 3], and NO	p. 234
Conclusions	p. 239
Low temperature ammonia oxidation on Pt	p. 240
Experimental details	p. 241
Ammonia oxidation at 323-473 K	p. 241
Characterisation of the adsorbed nitrogen and oxygen species	p. 244
Conversion and selectivity on pre-oxidised platinum	p. 248
Desorption of water	p. 249
Reaction mechanism	p. 251
Conclusion	p. 253
Ammonia adsorption on alumina	p. 254
Experimental details	p. 254
[superscript 13 N]-NH[subscript 3] equilibrium pulse experiments	p. 255
[superscript 13 N]-NH[subscript 3] Adsorption Assisted Desorption pulse experiments	p. 255
Conclusions	p. 256
Low temperature ammonia oxidation on Pt/alumina	p. 257
Index	p. 261
Table of Contents provided by Ingram. All Rights Reserved.

ISOTOPES IN HETEROGENEOUS CATALYSIS (V4)

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