Modeling and simulation of heterogeneous catalytic reactions: from the molecular process to the technical system
Gespeichert in:
| Weitere beteiligte Personen: | |
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| Format: | Buch |
| Sprache: | Englisch |
| Veröffentlicht: |
Weinheim
Wiley-VCH
2012
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| Links: | http://deposit.dnb.de/cgi-bin/dokserv?id=3718049&prov=M&dok_var=1&dok_ext=htm http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=024493680&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
| Umfang: | XVI, 354 S. Ill., graph. Darst. 240 mm x 170 mm |
| ISBN: | 9783527321209 3527321209 |
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CONTENTS
PREFACE XI LIST OF CONTRIBUTORS XV
1 MODELING CATALYTIC REACTIONS ON SURFACES WITH DENSITY FUNCTIONAL
THEORY 1 JOHN A. KEITH, JOSEF ANTON, PAYAM KAGHAZCHI, AND TIMO JACOB 1.1
INTRODUCTION 1
1.2 THEORETICAL BACKGROUND 2
1.2.1 THE MANY-BODY PROBLEM 2 1.2.2 BORN-OPPENHEIMER APPROXIMATION 3
1.2.3 WAVE FUNCTION-BASED METHODS 4 1.2.3.1 HARTREE-FOCK APPROXIMATION 4
1.2.3.2 POST HARTREE-FOCK METHODS 5
1.2.4 DENSITY-BASED METHODS 6 1.2.4.1 THE THOMAS-FERMI MODEL 7 1.2.4.2
THE HOHENBERG-KOHN THEOREMS 7 1.2.4.3 THE KOHN-SHAM EQUATIONS 9 1.2 A A
EXCHANGE-CORRELATION FUNCTIONALS 10 1.2.5 TECHNICAL ASPECTS OF MODELING
CATALYTIC REACTIONS 13
1.2.5.1 GEOMETRY OPTIMIZATIONS 13 1.2.5.2 TRANSITION-STATE OPTIMIZATIONS
14 1.2.5.3 VIBRATIONAL FREQUENCIES 14 1.2.5.4 THERMODYNAMIC TREATMENTS
OF MOLECULES 16 1.2.5.5 CONSIDERING SOLVATION 17 1.2.6 MODEL
REPRESENTATION 19 1.2.6.1 SLAB/SUPERCELL APPROACH 39
1.2.6.2 CLUSTER APPROACH 21 1.3 THE ELECTROCATALYTIC OXYGEN REDUCTION
REACTION ON PT(LLL) 22 1.3.1 WATER FORMATION FROM GASEOUS O 2 AND H 2 24
1.3.1.1 O 2 DISSOCIATION 25 1.3.1.2 OOH FORMATION 27
1.3.1.3 HOOH FORMATION 28 1.3.2 SIMULATIONS INCLUDING WATER SOLVATION 28
BIBLIOGRAFISCHE INFORMATIONEN HTTP://D-NB.INFO/1011200112
DIGITALISIERT DURCH
IMAGE 2
VI CONTENTS
1.3.2.1 LANGMUIR-HINSHELWOOD MECHANISMS 30
1.3.2.2 ELEY-RIDEAL REACTIONS 31 1.3.3 INCLUDING THERMODYNAMICAL
QUANTITIES 32 1.3.3.1 LANGMUIR-HINSHELWOOD AND ELEY-RIDEAL MECHANISMS 33
1.3.4 INCLUDING AN ELECTRODE POTENTIAL 35 1.4 CONCLUSIONS 36
REFERENCES 37
2 DYNAMICS OF REACTIONS AT SURFACES 39 AXEL GROSS 2.1 INTRODUCTION 39
2.2 THEORETICAL AND COMPUTATIONAL FOUNDATIONS OF DYNAMICAL SIMULATIONS
41 2.3 INTERPOLATION OF POTENTIAL ENERGY SURFACES 43 2.4 QUANTUM
DYNAMICS OF REACTIONS AT SURFACES 45 2.5 NONDISSOCIATIVE MOLECULAR
ADSORPTION DYNAMICS 49 2.6 ADSORPTION DYNAMICS ON PRECOVERED SURFACES 55
2.7 RELAXATION DYNAMICS OF DISSOCIATED H 2 MOLECULES 59 2.8
ELECTRONICALLY NONADIABATIC REACTION DYNAMICS 62 2.9 CONCLUSIONS 66
REFERENCES 67
3 FIRST-PRINCIPLES KINETIC MONTE CARLO SIMULATIONS FOR HETEROGENEOUS
CATALYSIS: CONCEPTS, STATUS, AND FRONTIERS 71 KARSTEN REUTER 3.1
INTRODUCTION 71
3.2 CONCEPTS AND METHODOLOGY 73 3.2.1 THE PROBLEM OF A RARE EVENT
DYNAMICS 73 3.2.2 STATE-TO-STATE DYNAMICS AND KMC TRAJECTORIES 75 3.2.3
KMC ALGORITHMS: FROM BASICS TO EFFICIENCY 77 3.2.4 TRANSITION STATE
THEORY 80
3.2.5 FIRST-PRINCIPLES RATE CONSTANTS AND THE LATTICE APPROXIMATION 84
3.3 A SHOWCASE 88
3.3.1 SETTING UP THE MODEL: LATTICE, ENERGETICS, AND RATE CONSTANT
CATALOG 3.3.2 STEADY-STATE SURFACE STRUCTURE AND COMPOSITION 90 3.3.3
PARAMETER-FREE TURNOVER FREQUENCIES 95
3.3.4 TEMPERATURE-PROGRAMMED REACTION SPECTROSCOPY 99 3.4 FRONTIERS 102
3.5 CONCLUSIONS 107
REFERENCES 208
4 MODELING THE RATE OF HETEROGENEOUS REACTIONS 113 LOTHAR KUNZ, LUBOW
MALER, STEFFEN TISCHER, AND OLAF DEUTSCHMANN 4.1 INTRODUCTION 113
4.2 MODELING THE RATES OF CHEMICAL REACTIONS IN THE GAS PHASE 115 4.3
COMPUTATION OF SURFACE REACTION RATES ON A MOLECULAR BASIS 116
IMAGE 3
CONTENTS VII
4.3.1 KINETIC MONTE CARLO SIMULATIONS 116
4.3.2 EXTENSION OF MC SIMULATIONS TO NANOPARTIDES 120 4.3.3 REACTION
RATES DERIVED FROM MC SIMULATIONS 124 4.3.4 PARTIDE-SUPPORT INTERACTION
AND SPILLOVER 125 4.3.5 POTENTIALS AND LIMITATIONS OF MC SIMULATIONS FOR
DERIVATION
OF OVERALL REACTION RATES 125 4.4 MODELS APPLICABLE FOR NUMERICAL
SIMULATION OF TECHNICAL CATALYTIC REACTORS 128 4A.I MEAN FIELD
APPROXIMATION AND REACTION KINETICS 129 4.4.2 THERMODYNAMIC CONSISTENCY
131 4.4.3 PRACTICABLE METHOD FOR DEVELOPMENT OF MULTISTEP SURFACE
REACTION MECHANISMS 134 4.4 A POTENTIALS AND LIMITATIONS OF THE MEAN
FIELD APPROXIMATION 139 4.5 SIMPLIFYING COMPLEX KINETIC SCHEMES 141 4.6
SUMMARY AND OUTLOOK 142
REFERENCES 143
5 MODELING REACTIONS IN POROUS MEDIA 149 FRERICHJ. KEIL 5.1 INTRODUCTION
149
5.2 MODELING POROUS STRUCTURES AND SURFACE ROUGHNESS 152 5.3 DIFFUSION
158
5.4 DIFFUSION AND REACTION 163
5.5 PORE STRUCTURE OPTIMIZATION: SYNTHESIS 173 5.6 CONCLUSION 275
REFERENCES 175
6 MODELING POROUS MEDIA TRANSPORT, HETEROGENEOUS THERMAL CHEMISTRY, AND
ELECTROCHEMICAL CHARGE TRANSFER 287 ROBERT J. KEE AND HUAYANG ZHU
6.1 INTRODUCTION 187
6.2 QUALITATIVE ILLUSTRATION 189 6.3 GAS-PHASE CONSERVATION EQUATIONS
190 6.3.1 GAS-PHASE TRANSPORT 292
6.3.2 CHEMICAL REACTION RATES 292 6.3.3 BOUNDARY CONDITIONS 192 6.4 ION
AND ELECTRON TRANSPORT 192
6.5 CHARGE CONSERVATION 194
6.5.1 EFFECTIVE PROPERTIES 195 6.5.2 BOUNDARY CONDITIONS 295 6.5.3
CURRENT DENSITY AND CELL POTENTIAL 296 6.6 THERMAL ENERGY 296
6.7 CHEMICAL KINETICS 296
6.7.1 THERMAL HETEROGENEOUS KINETICS 297 6.7.2 CHARGE TRANSFER KINETICS
298
IMAGE 4
VIII CONTENTS
6.7.3 BUTLER-VOLMER FORMULATION 204
6.7 A ELEMENTARY AND BUTLER-VOLMER FORMULATIONS 206 6.8 COMPUTATIONAL
ALGORITHM 207 6.9 BUTTON CELL EXAMPLE 207
6.9.1 POLARIZATION CHARACTERISTICS 208 6.9.2 ELECTRIC POTENTIALS AND
CHARGED SPECIES FLUXES 208 6.9.3 ANODE GAS-PHASE PROFILES 222 6.9.4
ANODE SURFACE SPECIES PROFILES 213
6.9.5 APPLICABILITY AND EXTENSIBILITY 224 6.10 SUMMARY AND CONDUSIONS
224 6.10.1 GREEK LETTERS 227 REFERENCES 228
7 EVALUATION OF MODELS FOR HETEROGENEOUS CATALYSIS 222 JOHN MANTZARAS
7.1 INTRODUCTION 222
7.2 SURFACE AND GAS-PHASE DIAGNOSTIC METHODS 222 7.2.1 SURFACE SCIENCE
DIAGNOSTICS 222 7.2.2 IN SITU GAS-PHASE DIAGNOSTICS 223 7.3 EVALUATION
OF HETERO/HOMOGENEOUS CHEMICAL REACTION SCHEMES 225
7.3.1 FUEL-LEAN COMBUSTION OF METHANE/AIR ON PLATINUM 225 7.3.1.1
HETEROGENEOUS KINETICS 225 7.3.1.2 GAS-PHASE KINETICS 228 7.3.2
FUEL-LEAN COMBUSTION OF PROPANE/AIR ON PLATINUM 231 7.3.3 FUEL-LEAN
COMBUSTION OF HYDROGEN/AIR ON PLATINUM 234 7.3.4 FUEL-RICH COMBUSTION OF
METHANE/AIR ON RHODIUM 238 7.3.5 APPLICATION OF KINETIC SCHEMES IN
MODELS FOR TECHNICAL SYSTEMS 240 7.4 EVALUATION OF TRANSPORT 242
7A.I TURBULENT TRANSPORT IN CATALYTIC SYSTEMS 243 7.4.2 MODELING
DIRECTIONS IN INTRAPHASE TRANSPORT 245 7.5 CONDUSIONS 246
REFERENCES 248
8 COMPUTATIONAL FLUID DYNAMICS OF CATALYTIC REACTORS 252 VINOD
M.JANARDHANAN AND OLAF DEUTSCHMANN 8.1 INTRODUCTION 252
8.2 MODELING OF REACTIVE FLOWS 253 8.2.1 GOVERNING EQUATIONS OF
MULTICOMPONENT FLOWS 253 8.2.2 TURBULENT FLOWS 256 8.2.3 THREE-PHASE
FLOW 256 8.2.4 MOMENTUM AND ENERGY EQUATIONS FOR POROUS MEDIA 257
8.3 COUPLING OF THE FLOW FIELD WITH HETEROGENEOUS CHEMICAL REACTIONS 258
8.3.1 GIVEN SPATIAL RESOLUTION OF CATALYST STRUCTURE 258 8.3.2 SIMPLE
APPROACH FOR MODELING THE CATALYST STRUCTURE 259
IMAGE 5
CONTENTS IX
8.3.3 REACTION DIFFUSION EQUATIONS 260
8.3.4 DUSTY GAS MODEL 262 8.4 NUMERICAL METHODS AND COMPUTATIONAL TOOLS
262 8.4.1 NUMERICAL METHODS FOR THE SOLUTION OF THE GOVERNING EQUATIONS
263 8.4.2 CFD SOFTWARE 264
8.4.3 SOLVERS FOR STIFF ODE AND DAE SYSTEMS 264 8.5 REACTOR SIMULATIONS
264
8.5.1 FLOW THROUGH CHANNELS 265 8.5.2 MONOLITHIC REACTORS 268 8.5.3
FIXED BED REACTORS 272 8.5.4 WIRE GAUZES 273
8.5.5 CATALYTIC REACTORS WITH MULTIPHASE FLUIDS 273 8.5.6 MATERIAL
SYNTHESIS 275 8.5.7 ELECTROCATALYTIC DEVICES 277 8.6 SUMMARY AND OUTLOOK
278
REFERENCES 279
9 PERSPECTIVE OF INDUSTRY ON MODELING CATALYSIS 283 JENS R.
ROSTRUP-NIELSEN 9.1 THE INDUSTRIAL CHALLENGE 283
9.2 THE DUAL APPROACH 285
9.3 THE ROLE OF MODELING 287
9.3.1 REACTOR MODELS 287 9.3.2 SURFACE SCIENCE AND BREAKDOWN OF THE
SIMPLIFIED APPROACH 288 9.3.3 THEORETICAL METHODS 290
9.4 EXAMPLES OF MODELING AND SCALE-UP OF INDUSTRIAL PROCESSES 292 9.4.1
AMMONIA SYNTHESIS 292 9.4.2 SYNGAS MANUFACTURE 294 9.4.2.1 STEAM
REFORMING 294 9.4.2.2 AUTOTHERMAL REFORMING 297 9.5 CONDUSIONS 298
REFERENCES 300
10 PERSPECTIVES OF THE AUTOMOTIVE INDUSTRY ON THE MODELING OF EXHAUST
GAS AFTERTREATMENT CATALYSTS 303 DANIEL CHATTERJEE, VOLKER SCHMEISSER,
MARCUS FREY, AND MICHEL WEIBEL 10.1 INTRODUCTION 303
10.2 EMISSION LEGISLATION 304 10.3 EXHAUST GAS AFTERTREATMENT
TECHNOLOGIES 306 10.4 MODELING OF CATALYTIC MONOLITHS 308 10.5 MODELING
OF DIESEL PARTICULATE FILTERS 323 10.6 SELECTIVE CATALYTIC REDUCTION BY
NH 3 (UREA-SCR) MODELING 315
10.6.1 KINETIC ANALYSIS AND CHEMICAL REACTION MODELING 316 10.6.1.1 NH 3
ADSORPTION, DESORPTION, AND OXIDATION 326 10.6.1.2 NO-SCR REACTION 316
IMAGE 6
X CONTENTS
10.6.1.3 NH 3 -NO-NO 2 REACTIONS 327
10.6.2 INFLUENCE OF WASHCOAT DIFFUSION 329 10.7 DIESEL OXIDATION
CATALYST, THREE-WAY CATALYST, AND NO X STORAGE AND REDUCTION CATALYST
MODELING 329 10.7.1 DIESEL OXIDATION CATALYST 320 10.7.2 THREE-WAY
CATALYST 321 10.7.3 NO* STORAGE AND REDUCTION CATALYST 322 10.7.3.1
SPECIES TRANSPORT EFFECTS RELATED TO NSCR: SHRINKING CORE MODEL 326
10.7.3.2 NH 3 FORMATION DURING RICH OPERATION WITHIN A NSRC 327 10.8
MODELING CATALYTIC EFFECTS IN DIESEL PARTICULATE FILTERS 328 10.9
DETERMINATION OF GLOBAL KINETIC PARAMETERS 329 10.10 CHALLENGES FOR
GLOBAL KINETIC MODELS 330 10.11 SYSTEM MODELING OF COMBINED EXHAUST
AFTERTREATMENT SYSTEMS 332
10.12 CONCLUSION 335
REFERENCES 339
INDEX 345
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| record_format | marc |
| spellingShingle | Modeling and simulation of heterogeneous catalytic reactions from the molecular process to the technical system Katalyse (DE-588)4029921-1 gnd Heterogene Reaktion (DE-588)4261131-3 gnd |
| subject_GND | (DE-588)4029921-1 (DE-588)4261131-3 (DE-588)4143413-4 |
| title | Modeling and simulation of heterogeneous catalytic reactions from the molecular process to the technical system |
| title_auth | Modeling and simulation of heterogeneous catalytic reactions from the molecular process to the technical system |
| title_exact_search | Modeling and simulation of heterogeneous catalytic reactions from the molecular process to the technical system |
| title_full | Modeling and simulation of heterogeneous catalytic reactions from the molecular process to the technical system ed. by Olaf Deutschmann |
| title_fullStr | Modeling and simulation of heterogeneous catalytic reactions from the molecular process to the technical system ed. by Olaf Deutschmann |
| title_full_unstemmed | Modeling and simulation of heterogeneous catalytic reactions from the molecular process to the technical system ed. by Olaf Deutschmann |
| title_short | Modeling and simulation of heterogeneous catalytic reactions |
| title_sort | modeling and simulation of heterogeneous catalytic reactions from the molecular process to the technical system |
| title_sub | from the molecular process to the technical system |
| topic | Katalyse (DE-588)4029921-1 gnd Heterogene Reaktion (DE-588)4261131-3 gnd |
| topic_facet | Katalyse Heterogene Reaktion Aufsatzsammlung |
| url | http://deposit.dnb.de/cgi-bin/dokserv?id=3718049&prov=M&dok_var=1&dok_ext=htm http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=024493680&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
| work_keys_str_mv | AT deutschmannolaf modelingandsimulationofheterogeneouscatalyticreactionsfromthemolecularprocesstothetechnicalsystem |
Inhaltsverzeichnis
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Teilbibliothek Chemie
| Signatur: |
0302 CHE 026f 2011 A 8250
Lageplan 0304 CHE 026f 2011 A 8250 Lageplan |
|---|---|
| Exemplar 1 | Ausleihbar Am Standort |
| Exemplar 1 | Nicht ausleihbar Am Standort |