Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas:
Gespeichert in:
| 1. Verfasser: | |
|---|---|
| Format: | Abschlussarbeit Buch |
| Sprache: | English |
| Veröffentlicht: |
Berlin
mvb, Mensch-und-Buch-Verl.
2012
|
| Schriftenreihe: | Engineering
|
| Schlagworte: | |
| Online-Zugang: | Inhaltsverzeichnis |
| Beschreibung: | 156 S. Ill., graph. Darst. |
| ISBN: | 9783863871864 |
Internformat
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| 245 | 1 | 0 | |a Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas |c vorgelegt von Claudia Berger-Karin |
| 264 | 1 | |a Berlin |b mvb, Mensch-und-Buch-Verl. |c 2012 | |
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Datensatz im Suchindex
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| adam_text | IMAGE 1
TABLE OF CONTENTS
1. INTRODUCTION 9
1.1 TECHNICAL BACKGROUND 9
1.2 PRODUCTION O F SYNTHESIS GAS 9
1.3 P O M CATALYSTS 10
1.4 THERMODYNAMIC AND MECHANISTIC ASPECTS 15
1.5 OBJECTIVES 17
1.6 STRATEGY AND OUTLINE 18
2. EXPERIMENTAL PART 20
2.1 CATALYST PREPARATION 20
2.2 NOBLE METAL COLLOIDS: PREPARATION AND CHARACTERIZATION 22
2.2.1 NANOPARTICLE PREPARATION AND LOADING ONTO Y-AI2O3 22
2.2.2 SMALL ANGLE X-RAY SCATTERING (SAXS) 25
2.3 PHYSICO-CHEMICAL CHARACTERIZATION 26
2.4 T EMPERATURE-PROGRAMMED METHODS 28
2.5 CATALYTIC TESTING 28
2.6 TRANSIENT EXPERIMENTS 32
2.6.1 DURATION O F TAP EXPERIMENTS 35
2.6.2 KINETIC MODELING O F TRANSIENT RESPONSES 36
3. TUNING REDUCIBILITY O F SUPPORTED NICKEL OXIDE SPECIES 40
3.1 CELLULOSE-TEMPLATED NI(10 WT.%)0 X-AL203 CATALYSTS 41
3.1.1 MORPHOLOGY O F MOX-AI2O3 MATERIALS 42
3.1.2 REDOX- AND CATALYTIC PROPERTIES 46
3.2 CE02-TI02-SUPPORTED NI(3 WT.%) CATALYSTS 52
3.2.1 C E 0 2 - T I 0 2 SUPPORT MATERIALS 52
3.2.2 NI(3 WT.%)0 X-CE02-TI02 CATALYSTS 60
3.2.3 NI(3 WT.%)0 X/Y-AL203 CATALYSTS PROMOTED BY TRACE AMOUNTS O F RH
68
3.3 PROOF O F PRINCIPLES 77
3.4 CONCLUSION 78
4. MECHANISTIC ANALYSIS O F THE NI-RH SYNERGISTIC EFFECT IN THE P O M
REACTION 80
4.1 MECHANISTIC ORIGINS O F THE NI-RH SYNERGISTIC EFFECT 81
4.2 CORRELATION O F CATALYST CHARACTERIZATION AND MECHANISTIC ANALYSIS
87
4.3 CONCLUSION 89
5. IMPROVING RHODIUM S FEASIBILITY 90
5.1 HIGHLY REDUCIBLE CE02-TI02-SUPPORTED RH(0.005 WT.%) CATALYSTS 91
5.1.1 PHYSICO-CHEMICAL PROPERTIES AS A FUNCTION O F PREPARATION METHOD
91
5.1.2 CATALYTIC PERFORMANCE IN PARTIAL OXIDATION O F METHANE TO SYNGAS
95
5.2 SUPPORTED, COLLOIDALLY PREPARED R H NANOPARTICLES 98
5.2.1 COMPARING P O M PERFORMANCE O F VARIOUS NOBLE METALS 99
5.2.2 EFFECT O F RH NP-LOADING ON P O M PERFORMANCE AND STABILITY 101
5.2.3 TAILORED, DIFFERENTLY SIZED RH N P 106
5.3 CONCLUSION 111
HTTP://D-NB.INFO/1025016009
IMAGE 2
8
TABLE O F CONTENTS
6. KINETIC ANALYSIS O F THE SIZE DEPENDENCE O F THE POM REACTION OVER
SUPPORTED
RHODIUM NANOPARTICLES 113
6.1 FUNDAMENTALS O F KINETIC MODELING 114
6.2 MODEL-FREE ANALYSIS O F THE O2, CH4, AND CO2 INTERACTION 116
6.3 KINETIC MODELING O F TRANSIENT EXPERIMENTS 119
6.4 KINETIC ORIGINS O F THE DEPENDENCE O F THE STEADY-STATE P O M
PERFORMANCE ON THE SIZE O F SUPPORTED R H NP 125
6.5 CONCLUSION 126
7. SUMMARY 127
8. OUTLOOK 130
9. REFERENCES 131
10. NOTATION 137
APPENDIX 138
A-1 TEST O F KNUDSEN FLOW ASSUMPTION 138
A-2 VALIDATION O F THE STANDARD DIFFUSION CURVE 138
A-3 TEMPERATURE PROFILE O F THE TAP MICRO-REACTOR 139
A-4 IMPACT O F MOLECULAR MASS ON TRANSIENT RESPONSES 140
A-5 CAST-TO-MOLD STRUCTURE O F CELLULOSE-TEMPLATED NI(10 WT.%)O X-AL203
140
A-6 CRYSTALLITE GROWTH OVER N I ( L 0 WT.%)0 X-AL203 CATALYSTS 141
A-7 FORMATION O F C2-HYDROCARBONS OVER NI_CT_EXO 141
A-8 EDX MAPPING O F BI-METALLIC, IW-IMPREGNATED NI-RH/Y-AHOS CATALYSTS
142
A-9 EDX SPECTROSCOPIC ANALYSIS O F BI-METALLIC INCIPIENT
WETNESS-IMPREGNATED NI-RH/Y- AI2O3 CATALYSTS 144
A-10 SIMULATION O F TWO-ZONE DIFFUSION FROM EXPERIMENTALLY DERIVED
THREE-ZONE AR TRANSIENTS 147
A - L 1 NOMINAL AND ACTUAL METAL-LOADINGS O F COLLOIDALLY PREPARED N P
CATALYSTS 149
A-12 EDX SPECTROSCOPIC ANALYSIS O F FRESH RH(0.2 WT.%)/Y-AL 203 149
A-13 PARTIAL DIFFERENTIAL EQUATIONS IMPLEMENTED IN THE PROGRAM FOR
NUMERICAL ANALYSIS AND SIMULATION O F EXPERIMENTAL DATA 150
A-14 MODEL DISCRIMINATION FOR CTU-AR EXPERIMENTS 151
A - L 5 RESIDUALS FROM NUMERICAL FITTING O F TRANSIENT RESPONSES OVER
DIFFERENTLY SIZED COLLOIDALLY PREPARED RH-NP/Y-A^OS CATALYSTS 152
A-L 6 SENSITIVITY ANALYSIS O F THE RESULTS O F THE SIMULATION O F
TRANSIENTS IN 02-AR, CFI 4-AR, CFLR02-AR, AND CH4-C02-AR EXPERIMENTS 153
A - L 7 CORRELATION ANALYSIS O F THE RESULTS O F THE SIMULATION O F 0 2
TRANSIENTS IN 02-AR EXPERIMENTS 155
LIST O F PUBLICATIONS 156
|
| any_adam_object | 1 |
| author | Berger-Karin, Claudia |
| author_GND | (DE-588)1026299489 |
| author_facet | Berger-Karin, Claudia |
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| bvnumber | BV040484090 |
| ctrlnum | (OCoLC)821213691 (DE-599)BVBBV040484090 |
| dewey-full | 665.77 |
| dewey-hundreds | 600 - Technology (Applied sciences) |
| dewey-ones | 665 - Industrial oils, fats, waxes & gases |
| dewey-raw | 665.77 |
| dewey-search | 665.77 |
| dewey-sort | 3665.77 |
| dewey-tens | 660 - Chemical engineering |
| discipline | Chemie / Pharmazie |
| format | Thesis Book |
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| indexdate | 2024-07-10T00:24:43Z |
| institution | BVB |
| isbn | 9783863871864 |
| language | English |
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| physical | 156 S. Ill., graph. Darst. |
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| spelling | Berger-Karin, Claudia Verfasser (DE-588)1026299489 aut Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas vorgelegt von Claudia Berger-Karin Berlin mvb, Mensch-und-Buch-Verl. 2012 156 S. Ill., graph. Darst. txt rdacontent n rdamedia nc rdacarrier Engineering Zugl.: Berlin, Techn. Univ., Diss., 2012 Synthesegas (DE-588)4058782-4 gnd rswk-swf Trägerkatalysator (DE-588)4185817-7 gnd rswk-swf Katalytische Oxidation (DE-588)4163425-1 gnd rswk-swf Selektive Oxidation (DE-588)4444728-0 gnd rswk-swf Methan (DE-588)4169678-5 gnd rswk-swf Herstellung (DE-588)4159653-5 gnd rswk-swf Rhodium (DE-588)4178038-3 gnd rswk-swf (DE-588)4113937-9 Hochschulschrift gnd-content Methan (DE-588)4169678-5 s Selektive Oxidation (DE-588)4444728-0 s Katalytische Oxidation (DE-588)4163425-1 s Trägerkatalysator (DE-588)4185817-7 s Rhodium (DE-588)4178038-3 s Synthesegas (DE-588)4058782-4 s Herstellung (DE-588)4159653-5 s DE-604 DNB Datenaustausch application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=025331250&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis |
| spellingShingle | Berger-Karin, Claudia Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas Synthesegas (DE-588)4058782-4 gnd Trägerkatalysator (DE-588)4185817-7 gnd Katalytische Oxidation (DE-588)4163425-1 gnd Selektive Oxidation (DE-588)4444728-0 gnd Methan (DE-588)4169678-5 gnd Herstellung (DE-588)4159653-5 gnd Rhodium (DE-588)4178038-3 gnd |
| subject_GND | (DE-588)4058782-4 (DE-588)4185817-7 (DE-588)4163425-1 (DE-588)4444728-0 (DE-588)4169678-5 (DE-588)4159653-5 (DE-588)4178038-3 (DE-588)4113937-9 |
| title | Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas |
| title_auth | Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas |
| title_exact_search | Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas |
| title_full | Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas vorgelegt von Claudia Berger-Karin |
| title_fullStr | Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas vorgelegt von Claudia Berger-Karin |
| title_full_unstemmed | Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas vorgelegt von Claudia Berger-Karin |
| title_short | Mechanistic and kinetic insights into origins governing activity and selectivity of the Ni- and Rh-catalyzed partial oxidation of methane to syngas |
| title_sort | mechanistic and kinetic insights into origins governing activity and selectivity of the ni and rh catalyzed partial oxidation of methane to syngas |
| topic | Synthesegas (DE-588)4058782-4 gnd Trägerkatalysator (DE-588)4185817-7 gnd Katalytische Oxidation (DE-588)4163425-1 gnd Selektive Oxidation (DE-588)4444728-0 gnd Methan (DE-588)4169678-5 gnd Herstellung (DE-588)4159653-5 gnd Rhodium (DE-588)4178038-3 gnd |
| topic_facet | Synthesegas Trägerkatalysator Katalytische Oxidation Selektive Oxidation Methan Herstellung Rhodium Hochschulschrift |
| url | http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=025331250&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
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