Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts:
Gespeichert in:
| 1. Verfasser: | |
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| Format: | Buch |
| Sprache: | English |
| Veröffentlicht: |
2005
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| Schlagworte: | |
| Online-Zugang: | Inhaltsverzeichnis |
| Beschreibung: | Hamburg-Harburg, Techn. Univ., Diss., 2005 |
| Beschreibung: | IV, 287 S. graph. Darst. |
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Datensatz im Suchindex
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| adam_text | THEORETICAL INVESTIGATION OF THE NITROUS OXIDE DECOMPOSITION OVER IRON
ZEOLITE CATALYSTS VOM PROMOTIONSAUSSCHUSS DER TECHNISCHEN UNIVERSITAT
HAMBURG-HARBURG ZUR ERLANGUNG DES AKADEMISCHEN GRADES DOKTOR-INGENIEUR
GENEHMIGTE DISSERTATION VON ANDREAS HEYDEN AUS PINNEBERG 2005 TABLE OF
CONTENTS 1 INTRODUCTION 1 2 CONTROL OF NITROUS OXIDE EMISSIONS 5 2.1
KYOTO PROCESS 5 2.2 NITROUS OXIDE EMISSIONS 6 2.3 CONTROL OF N 2 O FROM
NITRIC ACID PRODUCTION 8 3 THEORETICAL BACKGROUND 13 3.1 SCHRODINGER
EQUATION 14 3.1.1 BORN-OPPENHEIMER APPROXIMATION 16 3.1.2 VARIATIONAL
PRINCIPLE AND MOLECULAR ORBITALS 17 3.1.3 HARTREE-FOCK METHOD 19 3.2
DENSITY FUNCTIONAL THEORY 20 3.2.1 KOHN-SHAM EQUATIONS 22 3.2.2
EXCHANGE-CORRELATION FUNCTIONALS 24 3.2.3 HYBRID EXCHANGE-CORRELATION
FUNCTIONALS 27 3.2.4 BASIS SETS 29 3.2.5 BASIS SET SUPERPOSITION ERROR
31 3.3 NON-ADIABATIC EFFECTS 32 3.3.1 SPIN SURFACE CROSSING 34 3.3.2
LANDAU-ZENER FORMULA 35 3.4 STATISTICAL METHODS 38 3.4.1 POTENTIAL
ENERGY SURFACE 39 3.4.2 TRANSITION STATE THEORY 45 II TABLE OF CONTENTS
3.4.3 STATISTICAL MECHANICS AND THERMODYNAMIC FUNCTIONS 47 3.4.4 RATES
OF REACTION 50 4 ALGORITHMS FOR FINDING TRANSITION STATES IN CHEMICAL
REACTIONS 53 4.1 INTERPOLATION METHODS 55 4.1.1 STRING METHOD 57 4.1.2
GROWING STRING METHOD 60 4.2 LOCAL SADDLE POINT SEARCH ALGORITHMS 63
4.2.1 PARTITIONED RATIONAL FUNCTION OPTIMIZATION METHOD 65 4.2.2 DIMER
METHOD 67 4.2.3 IMPROVED DIMER METHOD 71 4.3 COMPARISON OF IMPROVED
DIMER AND P-RFO METHOD 77 4.3.1 DETAILS OF CALCULATIONS 78 4.3.2 RESULTS
79 4.4 ALGORITHM FOR FINDING MINIMUM ENERGY CROSSING POINTS 89 4.5
CONCLUSIONS 91 5 COMPREHENSIVE DFT STUDY OF THE NITROUS OXIDE
DECOMPOSITION OVER FE-ZSM-5 .93 5.1 N 2 O DECOMPOSITION OVER FE-ZSM-5 94
5.1.1 EXPERIMENTAL CHARACTERIZATION OF FE-ZSM-5 96 5.1.2 THEORETICAL
CHARACTERIZATION OF FE-ZSM-5 98 5.1.3 CONCLUSIONS 99 5.2 COMPUTATIONAL
MODEL OF THE ACTIVE SITE IN FE-ZSM-5 100 5.2.1 ZSM-5 101 5.2.2 CLUSTER
MODELS FOR EXTENDED SYSTEMS 102 5.2.3 LIMITATIONS OF THE CLUSTER MODEL
105 5.3 COMPUTATIONAL METHODOLOGY 107 TABLE OF CONTENTS 5.4
COMPUTATIONAL RESULTS AND DISCUSSION 109 5.4.1 CATALYTIC CYCLE ON Z [FE]
+ 110 5.4.2 CATALYTIC CYCLE ON Z [FEO] + 126 5.4.3 CATALYTIC CYCLE ON
Z[FEO 2 ] + 131 5.4.4 H 2 O ADSORPTION ON Z [FEO] + 132 5.4.5 CATALYTIC
CYCLE ON Z[FE(OH) 2 ] + 135 5.5 COMPARISON WITH EXPERIMENTAL OBSERVATION
137 5.6 CONCLUSIONS 141 6 KINETIC MODELING OF NITROUS OXIDE
DECOMPOSITION ON FE-ZSM-5 143 6.1 MECHANISM AND KINETICS OF N 2 O
DECOMPOSITION OVER FE-ZSM-5 144 6.2 EFFECTS OF WATER VAPOR ON THE
DISTRIBUTION OF FE SPECIES AND THE RATE OF N 2 O DECOMPOSITION 147 6.3
SIMULATION OF TEMPERATURE-PROGRAMMED REACTION EXPERIMENTS 149 6.4
SIMULATION OF TRANSIENT-RESPONSE EXPERIMENTS 154 6.5 OXYGEN ADSORPTION
AND DESORPTION FROM FE-ZSM-5 158 6.6 CONCLUSIONS 161 7 COMPREHENSIVE DFT
STUDY OF NO-ASSISTED N 2 O DECOMPOSITION OVER FE-ZSM-5 163 7.1
EXPERIMENTAL EVIDENCE OF NO-ASSISTED NITROUS OXIDE DECOMPOSITION 164 7.2
COMPUTATIONAL METHODOLOGY 168 7.3 COMPUTATIONAL RESULTS AND DISCUSSION
172 7.3.1 INTERACTION OF NITRIC OXIDE WITH Z [FEO] + , Z [FEO 2 ] + AND
Z[OFEO] + 186 7.3.2 CATALYTIC CYCLE ON Z[FEONO] + 192 7.3.3 CATALYTIC
CYCLE ON Z[FEO 2 N] + 197 7.3.4 CATALYTIC CYCLE ON Z[FEO 2 NO] + 201 IV
TABLE OF CONTENTS 7.3.5 ACTIVATION OF POISONED Z[FE(OH) 2 ] + SITES 206
7.3.6 CATALYTIC CYCLE ON Z [FEOH] + 207 7.3.7 FORMATION OF NITRIC OXIDE
ON SINGLE IRON SITES 212 7.4 COMPARISON WITH EXPERIMENTAL OBSERVATION
214 7.5 CONCLUSIONS 230 8 SUMMARY 233 LIST OF ACRONYMS 237 LIST OF
SYMBOLS 241 LITERATURE CITED 245 APPENDIX 269 A CONVERGENCE TESTS 271
A.I BASIS SET 272 A.2 CLUSTER SIZE 274 B APPARENT REACTION RATE CONSTANT
FOR THE N 2 O DECOMPOSITION ON FE-ZSM-5 281 B.I SYSTEM OF RATE EQUATIONS
282 B.I.I GAS SPECIES 282 B.1.2 SURFACE SPECIES 282 B.2 PSEUDO-STEADY
STATE APPROXIMATION 283 B.3 DETERMINATION OF MAIN SURFACE SITES 285 B.4
RATE OF CHANGE OF NITROGEN, OXYGEN AND NITROUS OXIDE 286
|
| adam_txt |
THEORETICAL INVESTIGATION OF THE NITROUS OXIDE DECOMPOSITION OVER IRON
ZEOLITE CATALYSTS VOM PROMOTIONSAUSSCHUSS DER TECHNISCHEN UNIVERSITAT
HAMBURG-HARBURG ZUR ERLANGUNG DES AKADEMISCHEN GRADES DOKTOR-INGENIEUR
GENEHMIGTE DISSERTATION VON ANDREAS HEYDEN AUS PINNEBERG 2005 TABLE OF
CONTENTS 1 INTRODUCTION 1 2 CONTROL OF NITROUS OXIDE EMISSIONS 5 2.1
KYOTO PROCESS 5 2.2 NITROUS OXIDE EMISSIONS 6 2.3 CONTROL OF N 2 O FROM
NITRIC ACID PRODUCTION 8 3 THEORETICAL BACKGROUND 13 3.1 SCHRODINGER
EQUATION 14 3.1.1 BORN-OPPENHEIMER APPROXIMATION 16 3.1.2 VARIATIONAL
PRINCIPLE AND MOLECULAR ORBITALS 17 3.1.3 HARTREE-FOCK METHOD 19 3.2
DENSITY FUNCTIONAL THEORY 20 3.2.1 KOHN-SHAM EQUATIONS 22 3.2.2
EXCHANGE-CORRELATION FUNCTIONALS 24 3.2.3 HYBRID EXCHANGE-CORRELATION
FUNCTIONALS 27 3.2.4 BASIS SETS 29 3.2.5 BASIS SET SUPERPOSITION ERROR
31 3.3 NON-ADIABATIC EFFECTS 32 3.3.1 SPIN SURFACE CROSSING 34 3.3.2
LANDAU-ZENER FORMULA 35 3.4 STATISTICAL METHODS 38 3.4.1 POTENTIAL
ENERGY SURFACE 39 3.4.2 TRANSITION STATE THEORY 45 II TABLE OF CONTENTS
3.4.3 STATISTICAL MECHANICS AND THERMODYNAMIC FUNCTIONS 47 3.4.4 RATES
OF REACTION 50 4 ALGORITHMS FOR FINDING TRANSITION STATES IN CHEMICAL
REACTIONS 53 4.1 INTERPOLATION METHODS 55 4.1.1 STRING METHOD 57 4.1.2
GROWING STRING METHOD 60 4.2 LOCAL SADDLE POINT SEARCH ALGORITHMS 63
4.2.1 PARTITIONED RATIONAL FUNCTION OPTIMIZATION METHOD 65 4.2.2 DIMER
METHOD 67 4.2.3 IMPROVED DIMER METHOD 71 4.3 COMPARISON OF IMPROVED
DIMER AND P-RFO METHOD 77 4.3.1 DETAILS OF CALCULATIONS 78 4.3.2 RESULTS
79 4.4 ALGORITHM FOR FINDING MINIMUM ENERGY CROSSING POINTS 89 4.5
CONCLUSIONS 91 5 COMPREHENSIVE DFT STUDY OF THE NITROUS OXIDE
DECOMPOSITION OVER FE-ZSM-5 .93 5.1 N 2 O DECOMPOSITION OVER FE-ZSM-5 94
5.1.1 EXPERIMENTAL CHARACTERIZATION OF FE-ZSM-5 96 5.1.2 THEORETICAL
CHARACTERIZATION OF FE-ZSM-5 98 5.1.3 CONCLUSIONS 99 5.2 COMPUTATIONAL
MODEL OF THE ACTIVE SITE IN FE-ZSM-5 100 5.2.1 ZSM-5 101 5.2.2 CLUSTER
MODELS FOR EXTENDED SYSTEMS 102 5.2.3 LIMITATIONS OF THE CLUSTER MODEL
105 5.3 COMPUTATIONAL METHODOLOGY 107 TABLE OF CONTENTS 5.4
COMPUTATIONAL RESULTS AND DISCUSSION 109 5.4.1 CATALYTIC CYCLE ON Z"[FE]
+ 110 5.4.2 CATALYTIC CYCLE ON Z"[FEO] + 126 5.4.3 CATALYTIC CYCLE ON
Z[FEO 2 ] + 131 5.4.4 H 2 O ADSORPTION ON Z"[FEO] + 132 5.4.5 CATALYTIC
CYCLE ON Z[FE(OH) 2 ] + 135 5.5 COMPARISON WITH EXPERIMENTAL OBSERVATION
137 5.6 CONCLUSIONS 141 6 KINETIC MODELING OF NITROUS OXIDE
DECOMPOSITION ON FE-ZSM-5 143 6.1 MECHANISM AND KINETICS OF N 2 O
DECOMPOSITION OVER FE-ZSM-5 144 6.2 EFFECTS OF WATER VAPOR ON THE
DISTRIBUTION OF FE SPECIES AND THE RATE OF N 2 O DECOMPOSITION 147 6.3
SIMULATION OF TEMPERATURE-PROGRAMMED REACTION EXPERIMENTS 149 6.4
SIMULATION OF TRANSIENT-RESPONSE EXPERIMENTS 154 6.5 OXYGEN ADSORPTION
AND DESORPTION FROM FE-ZSM-5 158 6.6 CONCLUSIONS 161 7 COMPREHENSIVE DFT
STUDY OF NO-ASSISTED N 2 O DECOMPOSITION OVER FE-ZSM-5 163 7.1
EXPERIMENTAL EVIDENCE OF NO-ASSISTED NITROUS OXIDE DECOMPOSITION 164 7.2
COMPUTATIONAL METHODOLOGY 168 7.3 COMPUTATIONAL RESULTS AND DISCUSSION
172 7.3.1 INTERACTION OF NITRIC OXIDE WITH Z"[FEO] + , Z"[FEO 2 ] + AND
Z[OFEO] + 186 7.3.2 CATALYTIC CYCLE ON Z[FEONO] + 192 7.3.3 CATALYTIC
CYCLE ON Z[FEO 2 N] + 197 7.3.4 CATALYTIC CYCLE ON Z[FEO 2 NO] + 201 IV
TABLE OF CONTENTS 7.3.5 ACTIVATION OF POISONED Z[FE(OH) 2 ] + SITES 206
7.3.6 CATALYTIC CYCLE ON Z"[FEOH] + 207 7.3.7 FORMATION OF NITRIC OXIDE
ON SINGLE IRON SITES 212 7.4 COMPARISON WITH EXPERIMENTAL OBSERVATION
214 7.5 CONCLUSIONS 230 8 SUMMARY 233 LIST OF ACRONYMS 237 LIST OF
SYMBOLS 241 LITERATURE CITED 245 APPENDIX 269 A CONVERGENCE TESTS 271
A.I BASIS SET 272 A.2 CLUSTER SIZE 274 B APPARENT REACTION RATE CONSTANT
FOR THE N 2 O DECOMPOSITION ON FE-ZSM-5 281 B.I SYSTEM OF RATE EQUATIONS
282 B.I.I GAS SPECIES 282 B.1.2 SURFACE SPECIES 282 B.2 PSEUDO-STEADY
STATE APPROXIMATION 283 B.3 DETERMINATION OF MAIN SURFACE SITES 285 B.4
RATE OF CHANGE OF NITROGEN, OXYGEN AND NITROUS OXIDE 286 |
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| index_date | 2024-07-02T14:30:24Z |
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| spelling | Heyden, Andreas 1975- Verfasser (DE-588)131381121 aut Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts von Andreas Heyden 2005 IV, 287 S. graph. Darst. txt rdacontent n rdamedia nc rdacarrier Hamburg-Harburg, Techn. Univ., Diss., 2005 Zersetzung (DE-588)4190752-8 gnd rswk-swf Stickstoffoxide (DE-588)4057516-0 gnd rswk-swf Zeolith (DE-588)4067660-2 gnd rswk-swf Katalysator (DE-588)4029919-3 gnd rswk-swf (DE-588)4113937-9 Hochschulschrift gnd-content Stickstoffoxide (DE-588)4057516-0 s Zersetzung (DE-588)4190752-8 s Katalysator (DE-588)4029919-3 s Zeolith (DE-588)4067660-2 s DE-604 HEBIS Datenaustausch Darmstadt application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=014763852&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis |
| spellingShingle | Heyden, Andreas 1975- Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts Zersetzung (DE-588)4190752-8 gnd Stickstoffoxide (DE-588)4057516-0 gnd Zeolith (DE-588)4067660-2 gnd Katalysator (DE-588)4029919-3 gnd |
| subject_GND | (DE-588)4190752-8 (DE-588)4057516-0 (DE-588)4067660-2 (DE-588)4029919-3 (DE-588)4113937-9 |
| title | Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts |
| title_auth | Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts |
| title_exact_search | Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts |
| title_exact_search_txtP | Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts |
| title_full | Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts von Andreas Heyden |
| title_fullStr | Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts von Andreas Heyden |
| title_full_unstemmed | Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts von Andreas Heyden |
| title_short | Theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts |
| title_sort | theoretical investigation of the nitrous oxide decomposition over iron zeolite catalysts |
| topic | Zersetzung (DE-588)4190752-8 gnd Stickstoffoxide (DE-588)4057516-0 gnd Zeolith (DE-588)4067660-2 gnd Katalysator (DE-588)4029919-3 gnd |
| topic_facet | Zersetzung Stickstoffoxide Zeolith Katalysator Hochschulschrift |
| url | http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=014763852&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
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