Principles and practice of heterogeneous catalysis:
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| Language: | English |
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2015
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| Edition: | 2., completely rev. ed. |
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| ISBN: | 352731458X 9783527314584 |
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| 245 | 1 | 0 | |a Principles and practice of heterogeneous catalysis |c J. M. Thomas and W. J. Thomas |
| 250 | |a 2., completely rev. ed. | ||
| 264 | 1 | |a Weinheim |b Wiley-VCH |c 2015 | |
| 300 | |a XX, 744 S. |b Ill., graph. Darst. | ||
| 336 | |b txt |2 rdacontent | ||
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CONTENTS
PREFACE XVII
1
SETTING THE SCENE 1
1.1
PROLOGUE: ADVANCES SINCE THE EARLY 1990S 1
1.2 INTRODUCTION 13
1.2.1
SELECTIVITY OF CATALYSTS 14
1.3 PERSPECTIVES IN CATALYSIS: PAST, PRESENT AND FUTURE 16
1.3.1 APPLIED CATALYSIS SINCE THE 1940S 19
1.3.2 SOME CURRENT TRENDS IN APPLIED CATALYSIS 23
1.3.2.1
AUTO-EXHAUST CATALYSTS 23
1.3.2.2 CATALYSTS IN ELECTROCHEMISTRY AND PHOTOELECTROCHEMISTRY 25
1.3.2.3 IMMOBILIZED METALS 26
1.3.2.4 IMMOBILIZED ENZYMES AND CELLS: PRESENT AND FUTURE 29
1.3.2.5 RIBOZYMES 31
1.4
DEFINITION OF CATALYTIC ACTIVITY 32
1.4.1 MAGNITUDE OF TURNOVER FREQUENCIES AND ACTIVE SITE
CONCENTRATIONS 33
1.4.2 VOLCANO PLOTS 35
1.4.3
EVOLUTION OF IMPORTANT CONCEPTS AND TECHNIQUES IN HETEROGENEOUS
CATALYSIS 36
1.4.3.1 MECHANISTIC INSIGHTS FROM ISOTOPIC LABELLING 47
1.4.3.2 CONCEPTS FROM ORGANOMETALLIC CHEMISTRY 48
1.5 KEY ADVANCES IN RECENT THEORETICAL TREATMENTS: UNIVERSABILITY
IN HETEROGENEOUS CATALYSIS
52
1.5.1 SOME MAJOR CURRENT DEVELOPMENTS IN HETEROGENEOUS
CATALYSIS 53
1.6 MILESTONES REACHED IN INDUSTRIAL CATALYSIS IN THE TWENTIETH CENTURY,
AND SOME
CONSEQUENTIAL CHALLENGES 54
PROBLEMS 61
REFERENCES 64
FURTHER READING 66
HTTP://D-NB.INFO/1050180941
V
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2
THE FUNDAMENTALS OF ADSORPTION: STRUCTURAL AND DYNAMICAL
CONSIDERATIONS, ISOTHERMS AND ENERGETICS 67
2.1 CATALYSIS MUST ALWAYS BE PRECEDED BY ADSORPTION 67
2.1.1 PHYSICAL ADSORPTION, CHEMISORPTION AND PRECURSOR STATES 67
2.2
THE SURFACES OF CLEAN SOLIDS ARE SOMETIMES RECONSTRUCTED 71
2.3 THERE ARE MANY WELL-DEFINED KINDS OF ORDERED ADLAYERS 74
2.4 ADSORPTION ISOTHERMS AND ISOBARS 79
2.4.1 THE EMPIRICAL FACTS 80
2.4.2 INFORMATION THAT CAN BE GLEANED FROM ISOTHERMS 80
2.4.3 ADSORPTION IS ALMOST INVARIABLY EXOTHERMIC 85
2.5 DYNAMICAL CONSIDERATIONS 86
2.5.1 RESIDENCE TIMES 87
2.5.2 RATES OF ADSORPTION 88
2.5.3 APPLYING STATISTICAL MECHANICS TO ADSORPTION 91
2.5.4
ADSORPTION KINETICS CAN OFTEN BE REPRESENTED BY THE ELOVICH
EQUATION 93
2.5.5 RATES OF DESORPTION 96
2.5.6 APPLYING STATISTICAL MECHANICS TO DESORPTION 98
2.5.7
INFLUENCE OF A PRECURSOR STATE ON THE KINETICS OF DESORPTION 99
2.6 RELATING THE ACTIVATION ENERGY TO THE ENERGY OF CHEMISORPTION.
UNIVERSALITY IN HETEROGENEOUS CATALYSIS AND THE
BRANSTED- EVANS -POLANYI (BEP) RELATION 101
2.6.1
PARETO-OPTIMAL CATALYSTS 104
2.7 DERIVING ADSORPTION ISOTHERMS FROM KINETIC PRINCIPLES 105
2.7.1 USING THE LANGMUIR ISOTHERM TO ESTIMATE THE PROPORTIONS OF
NON-DISSOCIATIVE AND ASSOCIATIVE ADSORPTION 106
2.7.2
OTHER ADSORPTION ISOTHERMS 109
2.7.2.1 HENRY'S ADSORPTION ISOTHERM 109
2.7.2.2 FREUNDLICH ISOTHERM 109
2.7.2.3 TEMKIN ISOTHERM 110
2.7.2A
BRUNAUER-EMMETT- TELLER ISOTHERM 110
2.7.2.5 DEVELOPMENTS FROM POLANYI'S ADSORPTION THEORY 110
2.7.2.6 KAGANER'S ISOTHERM AND THE DKR EQUATION 112
2.7.2.7 VIRIAL EQUATION OF STATE 112
2.8
ENERGETICS OF ADSORPTION 113
2.8.1 ESTIMATING THE BINDING ENERGIES OF PHYSICALLY ADSORBED SPECIES 114
2.8.2 BINDING ENERGIES OF CHEMISORBED SPECIES 118
2.8.3 ESTIMATING HEATS OF ADSORPTION FROM THERMODYNAMIC DATA 121
2.8.4
DECLINE OF THE HEAT OF ADSORPTION WITH INCREASING COVERAGE 123
. 2.9 MOBILITY AT SURFACES 126
2.10
KINETICS OF SURFACE REACTIONS 127
2.10.1 THE INFLUENCES OF PRECURSOR STATES ON THE KINETICS AND ENERGY
DISTRIBUTION OF CATALYSED REACTIONS 130
2.10.2 COMPARING THE RATES OF HETEROGENEOUS AND HOMOGENEOUS
REACTIONS
131
CONTENTS
| VII
2.11
AUTOCATALYTIC, OSCILLATORY AND COMPLEX HETEROGENEOUS
REACTIONS 132
2.11.1 AN OUTLINE OF AUTOCATALYSIS 133
2.11.2 BACKGROUND TO OSCILLATING REACTIONS 134
2.11.3 INSTABILITIES AND TRANSIENT PHENOMENA IN HETEROGENEOUS
CATALYSIS
136
2.11.4
MULTIPLE STEADY STATES 137
2.11.5 TRANSIENT PHENOMENA 139
2.11.6 RECENT THOUGHTS ON SPATIO-TEMPORAL BEHAVIOUR AND TURBULENCE
AT CATALYST SURFACES 145
2.12
MICROKINETICS: A SUMMARY 147
2.12.1 BUILDING KINETIC MODELS 149
2.12.2 FORMULATION OF KINETIC MODELS IN TERMS OF TRANSITION STATES 154
2.12.3 DEGREE OF RATE CONTROL 154
PROBLEMS
155
REFERENCES 161
FURTHER READING 162
3
THE CHARACTERIZATION OF INDUSTRIAL AND MODEL SOLID CATALYSTS 163
PART 1: CHARACTERIZATION OF INDUSTRIAL SOLID CATALYSTS 163
3.1 NON-INVASIVE METHODS SUITABLE FOR STUDIES INVOLVING CATALYTIC
REACTORS 164
3.1.1 MAGNETIC RESONANCE IMAGING (MRI) 165
3.1.1.1 VISUALIZING THE SPATIAL VARIATION OF ESTERIFICATION,
ETHERIFICATION AND
HYDROGENATION WITHIN FIXED-BED AND TRICKLE-BED REACTORS WITH
MRI
166
3.1.2
POSITRON EMISSION METHODS 170
3.1.3 USE OF SPATIALLY-RESOLVED X-RAY ABSORPTION TO PROBE SUPPORTED
NOBEL METAL CATALYSTS DURING OPERATING CONDITIONS 170
PART II: LABORATORY CHARACTERIZATION OF SOLID CATALYSTS 172
3.2 A PORTFOLIO OF MODERN METHODS: INTRODUCING THE ACRONYMS 172
3.3 WHICH ELEMENTS AND WHICH PHASES ARE PRESENT? 175
3.3.1 X-RAY FLUORESCENCE (XRF), X-RAY EMISSION (XRE) AND
PROTON-INDUCED X-RAY EMISSION (PIXE) 175
3.3.2
DEVELOPING TECHNIQUES: ICPMS 177
3.3.3 X-RAY DIFFRACTION (XRD) AND SMALL-ANGLE X-RAY SCATTERING 177
3.3.3.1 MEAN SIZE, SURFACE AREA AND PARTICLE-SIZE DISTRIBUTION FROM
SAXS 180
3.3.3.2 IN SITU STUDIES BY X-RAY DIFFRACTION 181
3.3.3.3
EXPERIMENTAL ASPECTS 183
3.4 PROBING SURFACES WITH IR, HREELS, AES AND XPS 184
3.4.1 INFRARED SPECTROSCOPY (IR): A NON-DESTRUCTIVE TECHNIQUE USABLE ON
CATALYSTS EXPOSED TO HIGH PRESSURE 184
3.4.2
HIGH-RESOLUTION ELECTRON-ENERGY LOSS SPECTROSCOPY (HREELS): THE
MOST SENSITIVE TOOL FOR IDENTIFYING SURFACE VIBRATIONAL MODES 189
VIII | CONTENTS
3.4.3
MERITS AND LIMITATIONS OF ELECTRON SPECTROSCOPY 190
3.5 ULTRAVIOLET-VISIBLE AND PHOTOLUMINESCENCE SPECTROSCOPY 191
3.6 STRUCTURE AND CRYSTALLOGRAPHY OF SURFACES: NATURE OF ORDERED AND
RECONSTRUCTED SURFACES 193
3.6.1 TWO- AND THREE-DIMENSIONAL SURFACE CRYSTALLOGRAPHY 193
3.6.2 NOTATIONS FOR DESCRIBING ORDERED STRUCTURES AT SURFACES 198
3.6.3 HOW DO BOND DISTANCES AT SURFACES COMPARE WITH THOSE OF BULK
SOLIDS? WHAT OF DISPLACIVE RECONSTRUCTIONS? 199
3.6.4 EXAFS, SEXAFS, XANES AND NEXAFS: PROBING BOND DISTANCES AND
SITE ENVIRONMENTS EVEN WHEN THERE IS NO LONG-RANGE ORDER 200
3.6.4.1 ORIGIN OF EXAFS AND HOW IT IS USED 200
3.6.4.2 APPLICATIONS OF EXAFS TO THE STUDY OF CATALYSTS 206
3.6.4.3 SEXAFS 209
3.6.4.4 XANES AND PRE-EDGE STRUCTURE: DEDUCING SITE SYMMETRY AND
OXIDATION STATES
210
3.6.4.5
NEXAFS 211
3.7 OTHER STRUCTURAL TECHNIQUES FOR CHARACTERIZING BULK AND SURFACES OF
CATALYSTS 214
3.7.1 ELECTRON SPIN RESONANCE (ESR): PROBING THE NATURE OF CATALYTICALLY
ACTIVE SITES AND THE CONCENTRATION OF PARAMAGNETIC INTERMEDIATES
ON SURFACES AND IN THE GAS PHASE 214
3.7.1.1 EXAMPLES OF THE USE OF ESR IN HETEROGENEOUS CATALYSIS 215
3.7.2 NUCLEAR MAGNETIC RESONANCE (NMR): A TECHNIQUE APPLICABLE,
AT HIGH RESOLUTION, TO SOLIDS
AND THEIR SURFACES 216
3.7.2.1 BASIC PRINCIPLES 216
3.7.2.2 NMR SPECTRA OF SOLIDS 219
3.7.2.3 APPLICATIONS OF NMR TO THE STUDY OF CATALYSTS, ADSORBENTS AND
ADSORBATES
220
3.7.2.4
FUTURE PROSPECTS FOR THE STUDY OF CATALYSTS BY SOLID-STATE NMR 224
3.7.3 SUM FREQUENCY GENERATION (SFG) AND INFRARED REFLECTION
ABSORPTION SPECTROSCOPY (IRAS OR IRRAS) 225
3.7.3.1 ESSENTIAL BACKGROUND AND MODE OF OPERATION 225
3.7.4 SCANNING TUNNELLING MICROSCOPY (STM) AND CLUES FOR THE DESIGN
OF NEW CATALYSTS
229
3.7.4.1 SCANNING TUNNELLING SPECTROSCOPY (STS) 238
3.7.4.2 ATOMIC FORCE MICROSCOPY (AFM) AND FLUORESCENCE MICROSCOPY
(FM) 239
3.7.5 ELECTRON MICROSCOPY 240
3.7.5.1 ELECTRON CRYSTALLOGRAPHY 245
3.7.5.2 ELECTRON TOMOGRAPHY (ET) 246
3.7.5.3 A FEW ILLUSTRATIVE EXAMPLES OF STATIC EM IMAGES 247
3.7.5.4 IN SITU (ENVIRONMENTAL) TEM 248
3.7.5.5 4D ELECTRON MICROSCOPY 248
3.7.6 OPTICAL MICROSCOPY AND ELLIPSOMETRY (NON-INVASIVE
TECHNIQUES)
250
CONTENTS
| IX
3.7.7
NEUTRON SCATTERING: A TECHNIQUE OF GROWING IMPORTANCE IN THE
STUDY OF CATALYSTS 252
3.7.7.1 DETERMINING THE ATOMIC STRUCTURE AND TEXTURE OF MICROCRYSTALLINE
CATALYSTS, THE NATURE OF THE ACTIVE SITES AND THE DISPOSITION OF
BOUND REACTANTS
256
3.7.7.2 DETERMINING THE STRUCTURE OF, AND IDENTIFYING FUNCTIONAL GROUPS
IN,
CHEMISORBED LAYERS AT CATALYST SURFACES 257
3.8 A MISCELLANY OF OTHER PROCEDURES 258
3.9
DETERMINING THE STRENGTH OF SURFACE BONDS: THERMAL AND OTHER
TEMPERATURE-PROGRAMMED METHODS 259
3.9.1 TEMPERATURE-PROGRAMMED DESORPTION (TPD) OR FLASH DESORPTION
SPECTROSCOPY (FDS) 260
3.9.2
TEMPERATURE-PROGRAMMED REACTION SPECTROSCOPY (TPRS) 262
3.9.3 MAGNITUDE OF THE HEAT AND ENTROPY OF ADSORPTION 263
3.10 REFLECTIONS ON THE CURRENT SCENE PERTAINING IN SITU METHODS OF
STUDYING CATALYSTS 265
3.10.1 ISOTOPIC LABELLING AND TRANSIENT RESPONSE 269
3.10.2 FROM TEMPORAL ANALYSIS OF PRODUCTS (TAP) TO STEADY-STATE ISOTOPIC
TRANSIENT KINETIC ANALYSIS (SSITKA) 272
3.10.3 INFRARED, RAMAN, NMR, AND X-RAY ABSORPTION SPECTROSCOPY FOR
IN SITU
STUDIES 273
3.10.4 IN SITU X-RAY, ELECTRON AND NEUTRON DIFFRACTION STUDIES 275
3.10.5 COMBINED X-RAY ABSORPTION AND X-RAY DIFFRACTION AND OTHER
TECHNIQUES FOR IN SITU STUDIES OF CATALYSTS 278
PROBLEMS 281
REFERENCES
288
FURTHER READING 29J
GENERAL 291
ADDITIONAL 291
IN SITU TECHNIQUES
291
4
POROUS CATALYSTS: THEIR NATURE AND IMPORTANCE 293
4.1 DEFINITIONS AND INTRODUCTION 293
4.2 DETERMINATION OF SURFACE AREA 296
4.2.1 ASSESSMENT OF POROSITY 298
4.2.1.1 CAPILLARY CONDENSATION; THE KELVIN EQUATION AND THE
BARRETT
- JOYNER - HALENDA METHOD 300
4.2.2 EVALUATION OF BOTH MICROPORE AND MESOPORE SIZE USING DENSITY
FUNCTIONAL THEORY AND GRAND CANONICAL MONTE CARLO METHODS 300
4.2.2.1 AN EXPLANATORY NOTE ABOUT DENSITY FUNCTIONAL THEORY (DFT) IN THE
CONTEXT OF ADSORPTION
302
4.2.2.2 HOW DOES ONE TACKLE A 'BREATHING' MOF NANOPOROUS
STRUCTURE? 303
4.2.3 THE FRACTAL APPROACH 304
4.2.4
PRACTICAL CONSIDERATIONS 305
X
I CONTENTS
4.3
MERCURY POROSIMETRY 306
4.4 WHEELER'S SEMI-EMPIRICAL PORE MODEL 308
4.4.1 MATHEMATICAL MODELS OF POROUS STRUCTURES 310
4.4.1.1 THE DUSTY GAS MODEL 310
4.4.1.2 RANDOM PORE MODEL 311
4.4.1.3
STOCHASTIC PORE NETWORKS AND FRACTALS 311
4.5 DIFFUSION IN POROUS CATALYSTS 314
4.5.1 THE EFFECTIVE DIFFUSIVITY 314
4.5.1.1
MOLECULAR (MAXWELLIAN) DIFFUSION OR BULK DIFFUSION 316
4.5.1.2 KNUDSEN DIFFUSION 317
4.5.1.3 THE TRANSITION REGION OF DIFFUSION 318
4.5.1.4 FORCED FLOW IN PORES 318
4.6
CHEMICAL REACTION IN POROUS CATALYST PELLETS 319
4.6.1 EFFECT OF INTRAPARTICLE DIFFUSION ON EXPERIMENTAL
PARAMETERS 326
4.6.2
NON-ISOTHERMAL REACTIONS IN POROUS CATALYST PELLETS 328
4.6.3 CRITERIA FOR DIFFUSION CONTROL 331
4.6.4 EXPERIMENTAL METHODS OF ASSESSING THE EFFECT OF DIFFUSION ON
REACTION 334
PROBLEMS
337
REFERENCES 340
FURTHER READING 341
SPECIFIC BOOKS 342
GENERAL 342
5
SOLID STATE CHEMICAL ASPECTS OF HETEROGENEOUS CATALYSTS 343
5.1 RECENT ADVANCES IN OUR KNOWLEDGE OF SOME METAL CATALYSTS: IN
THEIR EXTENDED, CLUSTER OR NANOPARTICLE STATES 34S
5.1.1 SURFACE AND SUB-SURFACE CHEMISTRY OF AG PARTICLES 345
5.1.2 ACTIVE SITE OF METHANOL SYNTHESIS OVER CU/ZNO/AL
2
O
S
CATALYSTS
347
5.1.3 PLATINUM AS A HYDROGENERATION CATALYST 349
5.1.4 AN EARLY REPORT THAT MONOATOMIC PT FUNCTIONS AS AN ACTIVE
HETEROGENEOUS CATALYST 350
5.1.5 AN EXCEPTIONALLY ACTIVE, ATOMICALLY DISPERSED PT-BASED CATALYST
FOR
GENERATING HYDROGEN FROM WATER
350
5.2 COMMENTS ON THE CATALYTIC BEHAVIOUR OF NANOGOLD 352
5.2.1 WHAT A SINGLE ATOM OF PALLADIUM CAN DO IN THE APPROPRIATE
ENVIRONMENT 358
5.3 RECENT ADVANCES IN THE ELUCIDATION OF CERTAIN METAL-OXIDE
CATALYSTS
359
5.3.1
AN ILLUSTRATIVE INVESTIGATION; COUPLING STM, IR, THERMAL REACTION
SPECTROSCOPY AND DFT OF FORMALDEHYDE FORMATION ON VANADIUM
OXIDE SURFACES
362
CONTENTS
| XI
5.4 ATOMIC-SCALE EDGE STRUCTURES IN INDUSTRIAL-STYLE MOS
2
NANOCATALYSTS 363
5.5 OPEN-STRUCTURE CATALYSTS: FROM 2D TO 3D 364
5.5.1 A BRIEF GUIDE TO THE STRUCTURE OF ZEOLITIC AND CLOSELY-RELATED
SOLID
CATALYSTS
365
5.5.1.1
NOTION OF FRAMEWORK DENSITY 369
5.5.2 NEW FAMILIES OF NANOPOROUS CATALYSTS 370
5.5.2.1 THE PRINCIPAL CATALYTIC SIGNIFICANCE OF NEW FAMILIES OF
NANOPOROUS
SOLIDS 375
5.6 COMPUTATIONAL APPROACHES 376
5.6.1
RESUME OF AVAILABLE METHODOLOGIES 376
5.6.1.1 SELECTED APPLICATIONS 382
5.7 A CHEMIST'S GUIDE TO THE ELECTRONIC STRUCTURE OF SOLIDS AND THEIR
SURFACES 389
5.7.1
ENERGY BANDS 390
5.7.1.1 BANDS IN ID AND 3D CRYSTALS 393
5.7.1.2 ENERGY BANDS IN IONIC SOLIDS 395
5.7.1.3 ENERGY BANDS IN TRANSITION-METAL OXIDES: UNDERSTANDING THE
ELECTRONIC STRUCTURE OF THE MONOXIDES OF TI, V, MN AND NI 398
5.7.2
FERMI LEVELS IN INSULATORS AND SEMICONDUCTORS 399
5.7.3 SURFACE ELECTRONIC STATES AND THE OCCURRENCE OF ENERGY LEVELS
WITHIN
THE BAND GAP 402
5.7.4 BAND BENDING AND METAL-SEMICONDUCTOR JUNCTIONS: SCHOTTKY
BARRIERS
403
5.7.4.1
DEPLETIVE CHEMISORPTION ON SEMICONDUCTORS 405
5.7.4.2 THE BENDING OF BANDS WHEN SEMICONDUCTORS ARE IMMERSED IN
ELECTROLYTES 406
5.7.5
QUANTUM CHEMICAL APPROACHES TO THE ELECTRONIC PROPERTIES OF
SOLIDS 407
5.7.6 A BRIEF SELECTION OF QUANTUM CHEMICAL STUDIES 408
5.7.6.1 BAND WIDTHS, DOS AND FERMI LEVELS OF THE TRANSITION METALS 408
5.7.6.2 DISSOCIATIVE CHEMISORPTION OF CO 410
5.7.6.3 INSIGHT FROM AB INITIO COMPUTATIONS: METHANOL SYNTHESIS AND
OLEFIN
METATHESIS
411
5.7.7
RECENT ADVANCES IN THE STUDY OF METATHESIS 413
5.8 KEY ADVANCES IN RECENT THEORETICAL TREATMENTS OF HETEROGENEOUS
CATALYSIS 415
5.8.1 FURTHER COMMENTS ON DENSITY FUNCTIONAL THEORY (DFT) 416
5.9 SELECTED APPLICATIONS OF DFT TO CATALYSIS 419
5.9.1
CATAPP: A WEB APPLICATION FOR SURFACE CHEMISTRY AND
HETEROGENEOUS CATALYSIS 421
5.9.2 TI
LV
CENTRED CATALYTIC EPOXIDATION OF C-HEXENE 423
5.9.3 MECHANISM OF THE AEROBIC TERMINAL OXIDATION OF LINEAR ALKANES AT
MN-DOPED ALUMINOPHOSPHATE CATALYSTS
424
5.9.4 RATE CONTROL AND REACTION ENGINEERING 425
XII
| CONTENTS
5.10
CONCLUDING REMARKS CONCERNING DFT CALCULATIONS IN
HETEROGENEOUS CATALYSIS 429
PROBLEMS 430
REFERENCES 433
KEY REFERENCES PUBLISHED SINCE THE FIRST EDITION 436
SEMINAL BOOKS 436
MONOGRAPHS
437
BOOK CHAPTERS 437
FURTHER READING 437
6
POISONING, PROMOTION, DEACTIVATION AND SELECTIVITY OF CATALYSTS 439
6.1 BACKGROUND 439
6.1.1
EFFECT OF MASS TRANSFER ON CATALYTIC SELECTIVITY 440
6.1.1.1 EFFECT OF INTRAPARTICLE DIFFUSION 440
6.1.1.2 NON-ISOTHERMAL CONDITIONS 445
6.1.1.3 EFFECT OF INTERPARTICLE MASS AND HEAT TRANSFER 448
6.1.2 BIFUNCTIONAL CATALYSTS (OR DUAL-FUNCTION CATALYSTS) 449
6.2 CATALYST DEACTIVATION 452
6.2.1 DEACTIVATION PROCESSES 452
6.2.2 DEACTIVATION MODELS 455
6.2.2.1 STEADY-STATE MODEL 455
6.2.2.2
A DYNAMIC MODEL 459
6.2.3 OPERATIONAL CONSEQUENCES OF POISONING 462
6.3 SOME MODERN THEORIES OF POISONING AND PROMOTION 463
6.3.1
GENERAL THEORETICAL CONSIDERATIONS 464
6.3.2 THEORETICAL INTERPRETATION OF POISONING AND PROMOTION 466
6.3.2.1 THE ELECTRONEGATIVITY OF A POISON SEEMS TO BE OF SECONDARY
IMPORTANCE 469
6.3.2.2
OTHER FACTORS RESPONSIBLE FOR PROMOTION AND POISONING 471
6.3.2.3 INFLUENCE OF SURFACE CARBON AND SUB-SURFACE HYDROGEN IN
HYDROGENATIONS ON PALLADIUM 473
6.3.2.4 CONCLUDING REMARKS 473
PROBLEMS
474
REFERENCES 477
FURTHER READING 477
GENERAL 477
STUDIES OF MODEL SURFACES 477
THEORY OF POISONING AND PROMOTION 478
7
CATALYTIC PROCESS ENGINEERING 479
PART I: RECENT ADVANCES IN REACTOR DESIGN 479
7.1 NOVEL OPERATING STRATEGIES 482
7.1.1 FIXED-BED REACTORS 482
7.1.1.1 PERIODIC OPERATION 483
7.1.1.2 CONCURRENT FLOW 485
CONTENTS
| XFLL
7.1.2
MICROCHANNEL REACTORS 485
7.1.3 MULTIFUNCTIONAL REACTORS 492
7.1.3.1 INTEGRATING EXOTHERMIC AND ENDOTHERMIC REACTIONS 492
7.1.3.2 INTEGRATING HEAT TRANSFER AND REACTION 494
7.1.3.3 INTEGRATING REACTION AND SEPARATION 495
PART II: TRADITIONAL METHODS
OF CATALYTIC PROCESS ENGINEERING 499
7.2 TRADITIONAL CATALYTIC REACTORS 499
7.2.1 EXPERIMENTAL LABORATORY REACTORS 499
7.2.1.1 BATCH REACTORS 500
7.2.1.2
TUBULAR REACTORS 501
7.2.1.3 CONTINUOUS STIRRED-TANK REACTOR 504
7.2.1.4 RECYCLE REACTOR 506
7.2.1.5 FLOWING-SOLIDS REACTORS 507
7.2.1.6
SLURRY REACTORS 507
7.2.2 INDUSTRIAL CHEMICAL REACTORS 510
7.2.2.1 BATCH REACTORS 511
7.2.2.2 CONTINUOUS TUBULAR REACTORS S13
7.2.2.3 FLUIDIZED-BED REACTOR 522
7.2.2.4 TRICKLE-BED REACTOR 525
7.2.2.5 METAL GAUZE REACTORS 527
7.2.3 THERMAL CHARACTERISTICS OF A CATALYTIC REACTOR 528
PROBLEMS 534
REFERENCES 538
GENERAL REFERENCES FOR PART II S39
GENERAL 539
KINETIC MODELS
539
EXPERIMENTAL CHEMICAL REACTOR CONFIGURATIONS 540
SLURRY REACTORS 540
FURTHER READING 540
8
HETEROGENEOUS CATALYSIS: EXAMPLES, CASE HISTORIES AND CURRENT
TRENDS 541
8.1 SYNTHESIS OF METHANOL 541
8.1.1 THE NATURE OF THE CATALYST 543
8.1.2 INSIGHT INTO THE MECHANISM OF FORMATION OF CH
3
OH 544
8.1.3 ASPECTS OF METHANOL SYNTHESIS TECHNOLOGY 545
8.2
FISCHER-TROPSCH CATALYSIS 546
8.2.1 MECHANISTIC CONSIDERATIONS 549
8.2.1.1 DOES SYNTHESIS PROCEED VIA HYDROXYMETHYLENE INTERMEDIATES? 550
8.2.1.2 SCHULTZ-FLORY STATISTICS 554
8.2.2 FINE-TUNING THE FISCHER-TROPSCH PROCESS 555
8.2.3 PRACTICAL FISCHER-TROPSCH CATALYSTS AND PROCESS CONDITIONS 556
8.2.4
COMMERCIAL FISCHER-TROPSCH PLANTS 559
8.2.5 METHANATION, STEAM REFORMING AND WATER-GAS SHIFT REACTIONS 559
8.2.5.1 METHANATION 559
XIV
I
CONTENTS
8.2.5.2
STEAM REFORMING: THE MOST EXTENSIVELY USED MEANS OF
MANUFACTURING HYDROGEN 563
8.3 SYNTHESIS OF AMMONIA 568
8.3.1 CATALYST PROMOTERS ARE OF TWO KINDS 570
8.3.2
KINETICS OF THE OVERALL REACTION: THE TEMKIN-PYZHEV
DESCRIPTION 5 71
8.3.3 THE SURFACE OF IRON CATALYSTS FOR AMMONIA SYNTHESIS CONTAIN
SEVERAL OTHER ELEMENTS: BUT IS THE IRON CRYSTALLINE? 573
8.3.3.1 DOES AMMONIA SYNTHESIS PROCEED VIA ATOMICALLY OR MOLECULARLY
ADSORBED NITROGEN?
575
8.3.3.2 HOW AND WHERE ARE THE REACTANT GASES ADSORBED AT THE CATALYST
SURFACE? 576
8.3.3.3 A POTENTIAL-ENERGY DIAGRAM ILLUSTRATING HOW THE OVERALL REACTION
LEADING TO AMMONIA
SYNTHESIS CAN BE CONSTRUCTED 580
8.3.3.4 HOW POTASSIUM SERVES AS AN ELECTRONIC PROMOTER 582
8.3.4 THE TECHNOLOGY OF AMMONIA SYNTHESIS 583
8.3.4.1 REACTOR CONFIGURATIONS ARE IMPORTANT INDUSTRIALLY 585
8.4 OXIDATION OF AMMONIA: STEPPING TOWARD THE FERTILIZER
INDUSTRY
588
8.4.1
AMMONIA OXIDATION AT SURFACES CONTAINING PRE-ADSORBED OXYGEN:
HOT AD-PARTICLES 592
8.5 IN SITU CATALYTIC REACTION AND SEPARATION 592
8.5.1 CATALYTIC DISTILLATION 592
8.5.2 CATALYTIC MEMBRANE PROCESSES 596
8.6
AUTOMOBILE EXHAUST CATALYSTS AND THE CATALYTIC MONOLITH 601
8.6.1 THE ARCHITECTURE OF THE THREE-WAY CATALYST 603
8.6.2 THE CATALYTIC MONOLITH 604
8.6.3 CATALYTIC MONOLITHS MAY BE USED IN SEVERAL APPLICATIONS 605
8.6.4
RATE CHARACTERISTICS OF CATALYTIC COMBUSTION PROCESSES 606
8.6.5 COMBUSTION REACTIONS IN A CATALYTIC MONOLITH DIFFER FROM THOSE
OCCURRING IN A HOMOGENEOUSLY OPERATED COMBUSTOR 607
8.6.6 SIMULATION OF THE BEHAVIOUR OF A CATALYTIC MONOLITH IS IMPORTANT
FOR
DESIGN PURPOSES 609
8.7 PHOTOCATALYTIC BREAKDOWN OF WATER AND THE HARNESSING OF SOLAR
ENERGY 614
8.7.1 PROLOGUE 614
8.7.2 ARTIFICIAL PHOTOSYNTHESIS 615
8.7.3 THE FUNDAMENTAL ENERGIES INVOLVED 618
8.7.3.1 OXYGEN GENERATION BY PHOTO-INDUCED OXIDATION OF WATER 619
8.7.3.2 HYDROGEN GENERATION BY PHOTO-INDUCED REDUCTION OF WATER 620
8.7.3.3 SIMULTANEOUS GENERATION OF HYDROGEN AND OXYGEN BY CATALYSED
PHOTOLYSIS OF WATER 621
8.7.4 SOME SELECTED PRACTICAL EXAMPLES 624
8.7.4.1 "THE GRATZEL CELL AND ITS INFLUENCE 626
8.7.4.2
TANDEM CELLS FOR WATER SPLITTING BY VISIBLE LIGHT 628
CONTENTS
I XV
8.8
CATALYTIC PROCESSES IN THE PETROLEUM INDUSTRY 629
8.8.1 CATALYTIC REFORMING 631
8.8.2 CATALYTIC CRACKING 633
8.8.2.1 CRACKING REACTIONS 636
8.8.2.2
CRACKING CATALYSTS 638
8.8.2.3 THE CATALYTIC CRACKING (FCC) REACTOR 638
8.8.3 HYDROTREATING 640
8.8.3.1 TOTAL CONVERSION OF HEAVY OILS INTO GOOD QUALITY DISTILLATES 644
PROBLEMS
645
REFERENCES 6S1
FURTHER READING 653
9
POWERING THE PLANET IN A SUSTAINABLE MANNER: SOME OF TOMORROW'S
CATALYSTS (ACTUAL AND DESIRED) AND KEY CATALYTIC FEATURES PERTAINING
TO RENEWABLE FEEDSTOCKS, GREEN CHEMISTRY AND CLEAN
TECHNOLOGY 655
9.1 INTRODUCTION 655
PART I:
PROSPECTS, PRACTICES AND PRINCIPLES OF GENERATING SOLAR
FUELS 658
9.2 POWERING THE PLANET WITH SOLAR FUEL 658
9.3 SOME SIGNIFICANT ADVANCES IN PHOTO-ASSISTED WATER SPLITTING AND
ALLIED PHENOMENA 659
9.3.1 STRATEGIES FOR SOLAR ENERGY CONVERSION 660
9.3.2 THE ARTIFICIAL LEAF 661
9.3.3 EARTH-ABUNDANT H
2
-EVOIUTION PHOTOCATALYSTS 664
9.3.4 EARTH-ABUNDANT 0
2
-EVOLUTION PHOTOCATALYSTS 665
9.3.5 LESSONS FROM ENZYMES
666
9.3.6 A SELECTIVE SURVEY AND FUTURE CHALLENGES
666
9.3.7 AN INTERIM STATUS REPORT ON WATER OXIDATION PHOTOCATALYSIS 669
9.3.8 CORE-SHELL CO-CATALYSTS IN THE PHOTOCATALYTIC CONVERSION OF C0
2
WITH WATER INTO METHANE
669
9.3.9 MODIFYING THE NATURE OF TI0
2
SO AS TO IMPROVE ITS PHOTOCATALYTIC
PERFORMANCE 670
9.3.9.1 BAND STRUCTURE ENGINEERING OF SEMICONDUCTORS FOR ENHANCED
PHOTOELECTROCHEMICAL WATER SPLITTING,
WITH SPECIAL REFERENCE TO
TI0
2
AND FE
2
0
3
674
9.3.10 METAL-ORGANIC FRAMEWORKS (MOFS) AND THEIR PHOTOCATALYTIC
POSSIBILITIES 675
9.3.11
PHOTOCATALYTIC SOLIDS FOR THE DESTRUCTION OF TOXIC POLLUTANTS AND
OTHERWISE UNWANTED MOLECULES 676
9.4 THE HYDROGEN ECONOMY 677
9.4.1 THE METHANOL ECONOMY 682
PART II:
CURRENT PRACTICES IN POWERING THE PLANET AND PRODUCING
CHEMICALS 685
9.5 SOME OF TOMORROW'S CATALYSTS: ACTUAL AND DESIRED 685
XVI
| CONTENTS
9.5.1 SOME EXISTING INDUSTRIAL CATALYSTS LIKELY TO BE DIFFICULT TO
REPLACE IN
THE NEAR FUTURE 687
9.5.2 AMMOXIDATION: ACROLEIN AND ACRYLIC ACID 687
9.5.3 POLY(ETHYLENE TEREPHTHALATE) (PET) 692
9.5.4 FISCHER-TROPSCH SYNTHESES (FTS) 696
9.5.4.1 FTS USING C0
2
TO GENERATE HYDROCARBON FUELS 696
9.5.5 ADIPIC ACID; NYLON 6,6; NYLON 6 AND TEREPHTHALIC ACID 697
9.5.5.1 THE PRACTICAL IMPORTANCE OF CASCADE CATALYTIC REACTIONS 700
9.5.6 CATALYTIC CRACKING AND REFINING: THE IMPACT OF MESOSTRUCTURED
Y ZEOLITE
701
9.5.6.1
ECOFINING: THE ROAD TO GREEN REFINERIES 705
9.6 A BIOREFINERY CAPABLE OF PRODUCING TRANSPORTATION FUELS
AND COMMODITY CHEMICALS THAT STARTS WITH METABOLIC ENGINEERING
AND ENDS WITH INORGANIC SOLID CATALYSTS 707
9.6.1
RENEWABLES TO PARA-XYLENE AND OTHER AROMATICS 709
9.6.2 BIOREFINERY FOR INTEGRATED METHODS OF PREPARING RENEWABLE
CHEMICALS 711
9.6.3 THREE ADVANCED BIOFUELS FROM SWITCHGRASS USING ENGINEERED
ESCHERICHIA COLI
711
9.7
NON-ENZYMATIC CATALYTIC PROCESSING OF BIOMASS-DERIVED RAW
MATERIALS TO SELECTED CHEMICAL PRODUCTS 711
9.7.1 SUSTAINABLE CHEMISTRY BY UPGRADING PYROLYSIS OIL 714
9.7.2 CATALYTIC CONVERSION OF MICROALGAE INTO GREEN HYDROCARBONS AND
ETHANOL
716
9.7.2.1
MICROALGAE TO DIESEL 717
9.7.2.2 MICROALGAE TO BIOETHANOL USING C0
2
AND SUNLIGHT 718
9.8 STRATEGIES FOR THE DESIGN OF NEW CATALYSTS 719
9.8.1 THE MERITS AND LIMITATIONS OF SINGLE-SITE HETEROGENEOUS
CATALYSIS
720
PART III: THERMOCHEMICAL CYCLES AND HIGH-FLUX, SOLAR-DRIVEN
CONVERSIONS 724
9.9 SOLAR-DRIVEN, CATALYSED THERMOCHEMICAL REACTIONS AS ALTERNATIVES
TO FOSSIL-FUEL-BASED ENERGY AND CHEMICAL ECONOMIES
724
ACKNOWLEDGEMENTS 726
PROBLEMS 726
REFERENCES 729
FURTHER READING
732
INDEX
733 |
| any_adam_object | 1 |
| author | Thomas, John M. 1932-2020 Thomas, W. J. |
| author_GND | (DE-588)134006143 (DE-588)106476245X |
| author_facet | Thomas, John M. 1932-2020 Thomas, W. J. |
| author_role | aut aut |
| author_sort | Thomas, John M. 1932-2020 |
| author_variant | j m t jm jmt w j t wj wjt |
| building | Verbundindex |
| bvnumber | BV041886368 |
| classification_rvk | VE 7040 |
| ctrlnum | (OCoLC)878979257 (DE-599)DNB1050180941 |
| dewey-full | 541.395 |
| dewey-hundreds | 500 - Natural sciences and mathematics |
| dewey-ones | 541 - Physical chemistry |
| dewey-raw | 541.395 |
| dewey-search | 541.395 |
| dewey-sort | 3541.395 |
| dewey-tens | 540 - Chemistry and allied sciences |
| discipline | Chemie / Pharmazie |
| edition | 2., completely rev. ed. |
| format | Book |
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| genre_facet | Aufsatzsammlung |
| id | DE-604.BV041886368 |
| illustrated | Illustrated |
| indexdate | 2025-03-10T13:01:13Z |
| institution | BVB |
| isbn | 352731458X 9783527314584 |
| language | English |
| oai_aleph_id | oai:aleph.bib-bvb.de:BVB01-027330382 |
| oclc_num | 878979257 |
| open_access_boolean | |
| owner | DE-703 DE-20 DE-29T DE-11 DE-634 DE-19 DE-BY-UBM DE-355 DE-BY-UBR DE-83 |
| owner_facet | DE-703 DE-20 DE-29T DE-11 DE-634 DE-19 DE-BY-UBM DE-355 DE-BY-UBR DE-83 |
| physical | XX, 744 S. Ill., graph. Darst. |
| publishDate | 2015 |
| publishDateSearch | 2015 |
| publishDateSort | 2015 |
| publisher | Wiley-VCH |
| record_format | marc |
| spelling | Thomas, John M. 1932-2020 Verfasser (DE-588)134006143 aut Principles and practice of heterogeneous catalysis J. M. Thomas and W. J. Thomas 2., completely rev. ed. Weinheim Wiley-VCH 2015 XX, 744 S. Ill., graph. Darst. txt rdacontent n rdamedia nc rdacarrier Heterogene Katalyse (DE-588)4123377-3 gnd rswk-swf 1\p (DE-588)4143413-4 Aufsatzsammlung gnd-content Heterogene Katalyse (DE-588)4123377-3 s DE-604 Thomas, W. J. Verfasser (DE-588)106476245X aut Erscheint auch als Online-Ausgabe, EPUB 978-3-527-68378-9 Erscheint auch als Online-Ausgabe, MOBI 978-3-527-68379-6 Erscheint auch als Online-Ausgabe, PDF 978-3-527-68380-2 X:MVB text/html http://deposit.dnb.de/cgi-bin/dokserv?id=4642517&prov=M&dok_var=1&dok_ext=htm Inhaltstext DNB Datenaustausch application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=027330382&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis 1\p cgwrk 20201028 DE-101 https://d-nb.info/provenance/plan#cgwrk |
| spellingShingle | Thomas, John M. 1932-2020 Thomas, W. J. Principles and practice of heterogeneous catalysis Heterogene Katalyse (DE-588)4123377-3 gnd |
| subject_GND | (DE-588)4123377-3 (DE-588)4143413-4 |
| title | Principles and practice of heterogeneous catalysis |
| title_auth | Principles and practice of heterogeneous catalysis |
| title_exact_search | Principles and practice of heterogeneous catalysis |
| title_full | Principles and practice of heterogeneous catalysis J. M. Thomas and W. J. Thomas |
| title_fullStr | Principles and practice of heterogeneous catalysis J. M. Thomas and W. J. Thomas |
| title_full_unstemmed | Principles and practice of heterogeneous catalysis J. M. Thomas and W. J. Thomas |
| title_short | Principles and practice of heterogeneous catalysis |
| title_sort | principles and practice of heterogeneous catalysis |
| topic | Heterogene Katalyse (DE-588)4123377-3 gnd |
| topic_facet | Heterogene Katalyse Aufsatzsammlung |
| url | http://deposit.dnb.de/cgi-bin/dokserv?id=4642517&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=027330382&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
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