Novel ruthenium dihydrogen complexes and their application in catalysis:
Gespeichert in:
| 1. Verfasser: | |
|---|---|
| Format: | Buch |
| Sprache: | English |
| Veröffentlicht: |
Duisburg [u.a.]
WiKu-Verl.
2007
|
| Schriftenreihe: | Wissenschaftliche Monographie der MPG und der RWTH Aachen
|
| Schlagworte: | |
| Online-Zugang: | Inhaltsverzeichnis |
| Beschreibung: | Zugl.: Aachen, Techn. Hochsch., Diss., 2007 |
| Beschreibung: | XIII, 152 S. graph. Darst. |
| ISBN: | 9783865532299 |
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| 245 | 1 | 0 | |a Novel ruthenium dihydrogen complexes and their application in catalysis |c vorgelegt von Martin H. G. Prechtl |
| 264 | 1 | |a Duisburg [u.a.] |b WiKu-Verl. |c 2007 | |
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| 490 | 0 | |a Wissenschaftliche Monographie der MPG und der RWTH Aachen | |
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| 650 | 7 | |a Hydridokomplexe |2 swd | |
| 650 | 7 | |a Katalyse |2 swd | |
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Datensatz im Suchindex
| _version_ | 1804137609527558144 |
|---|---|
| adam_text | 1. Introduction 1
1.1. Background and Motivation 1
1.2. State ofthe Art and Objectives 2
1.2.1. Ruthenium Dihydrogen Complexes 2
1.2.2. Characterisation of Nonclassical Hydride Complexes 6
1.2.3. Catalysis 9
1.2.3.1. CH-Activation and H/D-Exchange Reactions 9
1.2.3.2. Ruthenium Hydrides in Hydrogen Transfer Processes 11
2. Results and Discussion 15
2.1. The Ruthenium Dihydrogen Complex [Ru(dtbpmp)(H2)H2] 15
2.1.1. Synthesis 15
2.1.2. Characterisation 17
2.1.3 Reactivity 23
2.1.3.1. H2 / N2 Exchange 23
2.1.3.2. H / D Exchange 26
2.1.3.3. Treatment with carbon monoxide 31
2.1.3.4. Reaction with pinacolborane 34
2.1.3.5. Reaction with CO2 36
2.1.4. Other PNP pincer ligands for ruthenium hydride complexes 40
2.2. The Ruthenium Dihydrogen Complex [Ru(dtbpoet)(H2)H2] 42
2.2.1. Synthesis 42
2.2.2. Characterisation 43
2.2.3. Reactivity 49
2.3. Catalysis 50
2.3.1. Catalytic ///D-Exchange between Aromatic Hydfocarbons and Deuterated
Solvents 50
2.3.1.1. D2O as Deuterium Source 50
2.3.1.2. C6D6as Deuterium Source 58
2.3.2. Catalytic Dehydrogenation of Alcohol and Tandem Reactions 67
2.3.2.1. Dehydrogenative Coupling of Primary Alcohols 67
2.3.2.2. Dehydrogenation of Secondary Alcohols 77
3. Summary 82
3.1. Ruthenium Dihydrogen Complexes 82
3.2. Catalysis g4
4 Experimental Section gg
4.1. General og
4.2. Analytic Methods g(
4.2.1. Nuclear Magnetic Resonance Spectroscopy (NMR) 86
4.2.2. Mrared Spectroscopy (1R) gg
4.2.3. Mass Spectrometry gg
42A X ^y gg
4.2.5. Microanalysis 88
4.2.6. Autoclaves for High-Pressure Experiments 89
4.2.6.1. Typ I (glass autoclave, 50 mL) 89
4.2.6.2. Typ II (autoclave, 36 mL) 89
4-3. Synthetic Procedures 90
43.1. Uterature Compounds 90
4-3.2. Chelating Diphosphine Nitrogen Ligands (PNP-pincer) 91
43.3. Ruthenium Dihydrogen Complexes 92
4.3.3.1. Preparation of[Ru( M,pmp)H2(H2)] 4 92
43.3.2. Preparation of the complex [D,HRu( M,pm/?)H2(H2)] [D,]-4 94
43.3.3. Reaction of [Ru(d,bpmp)H2(H2)} 4 with C6D6 to highly deuterated [D,]-4 95
43.3.4. Reaction of RU(d,bpmp)H2(H2) 4 with D2O in C6DI2 to |D6|-4 / 26 95
43.3.5. Reaction of lRu(dtbpmp)H2(H2) 4 with N2 to RU(d,bpmp)H2(N2)] 20 96
4.3.3.6. Reaction of [Ru(dtbpmp)H2(H2)} 4 with carbon monoxide and hydrogen gas to
[Ru(dtbpmp)(CO)H] 28 97
43.3.7. Reaction of [Ru(dtbpmp)H2(H2)] 4 with pinacolborane 97
43.3.8. Solid State Structure: Reaction with CO2 99
43.3.9. Preparation of lRu(,dtbpoet)H2(H2)} 5 104
4.3.3.10. Reaction of [Ru(dtbpoet)H2(H2)] 5 with N2 to [Ru(d,bpoe,)H2(N2)] 52 106
4.33.11. Reaction of [Ru(A^o«)H2(H2)l 5 with D2 to
|DxHRu(rf/^oe,)H2(H2)l[Dx]-5 106
4-3.4. Catalysis ]07
4.3.4.1 Catalytic tf/D-exchange with D2O as Deuterium Source 107
4.3.4.2. Catalytic tf/D-exchange with [D6]benze„e as Deuterium Source 113
43.4.3. CatalyticDehydrogenationofAlcohols 119
5 Figure Index 126
6 Scheme Index 129
7 Table Index 132
8 Abbreviation Index 133
9 Compound Name Index 135
10 Compound Structure Index 138
11 Literature 146
|
| adam_txt |
1. Introduction 1
1.1. Background and Motivation 1
1.2. State ofthe Art and Objectives 2
1.2.1. Ruthenium Dihydrogen Complexes 2
1.2.2. Characterisation of Nonclassical Hydride Complexes 6
1.2.3. Catalysis 9
1.2.3.1. CH-Activation and H/D-Exchange Reactions 9
1.2.3.2. Ruthenium Hydrides in Hydrogen Transfer Processes 11
2. Results and Discussion 15
2.1. The Ruthenium Dihydrogen Complex [Ru(dtbpmp)(H2)H2] 15
2.1.1. Synthesis 15
2.1.2. Characterisation 17
2.1.3 Reactivity 23
2.1.3.1. H2 / N2 Exchange 23
2.1.3.2. H / D Exchange 26
2.1.3.3. Treatment with carbon monoxide 31
2.1.3.4. Reaction with pinacolborane 34
2.1.3.5. Reaction with CO2 36
2.1.4. Other PNP pincer ligands for ruthenium hydride complexes 40
2.2. The Ruthenium Dihydrogen Complex [Ru(dtbpoet)(H2)H2] 42
2.2.1. Synthesis 42
2.2.2. Characterisation 43
2.2.3. Reactivity 49
2.3. Catalysis 50
2.3.1. Catalytic ///D-Exchange between Aromatic Hydfocarbons and Deuterated
Solvents 50
2.3.1.1. D2O as Deuterium Source 50
2.3.1.2. C6D6as Deuterium Source 58
2.3.2. Catalytic Dehydrogenation of Alcohol and Tandem Reactions 67
2.3.2.1. Dehydrogenative Coupling of Primary Alcohols 67
2.3.2.2. Dehydrogenation of Secondary Alcohols 77
3. Summary 82
3.1. Ruthenium Dihydrogen Complexes 82
3.2. Catalysis g4
4 Experimental Section gg
4.1. General og
4.2. Analytic Methods g(
4.2.1. Nuclear Magnetic Resonance Spectroscopy (NMR) 86
4.2.2. Mrared Spectroscopy (1R) gg
4.2.3. Mass Spectrometry gg
42A X"^y ' gg
4.2.5. Microanalysis 88
4.2.6. Autoclaves for High-Pressure Experiments 89
4.2.6.1. Typ I (glass autoclave, 50 mL) 89
4.2.6.2. Typ II (autoclave, 36 mL) 89
4-3. Synthetic Procedures 90
43.1. Uterature Compounds 90
4-3.2. Chelating Diphosphine Nitrogen Ligands (PNP-pincer) 91
43.3. Ruthenium Dihydrogen Complexes 92
4.3.3.1. Preparation of[Ru( M,pmp)H2(H2)] 4 92
43.3.2. Preparation of the complex [D,HRu( M,pm/?)H2(H2)] [D,]-4 94
43.3.3. Reaction of [Ru(d,bpmp)H2(H2)} 4 with C6D6 to highly deuterated [D,]-4 95
43.3.4. Reaction of \RU(d,bpmp)H2(H2)\ 4 with D2O in C6DI2 to |D6|-4 / 26 95
43.3.5. Reaction of lRu(dtbpmp)H2(H2)\ 4 with N2 to \RU(d,bpmp)H2(N2)] 20 96
4.3.3.6. Reaction of [Ru(dtbpmp)H2(H2)} 4 with carbon monoxide and hydrogen gas to
[Ru(dtbpmp)(CO)H] 28 97
43.3.7. Reaction of [Ru(dtbpmp)H2(H2)] 4 with pinacolborane 97
43.3.8. Solid State Structure: Reaction with CO2 99
43.3.9. Preparation of lRu(,dtbpoet)H2(H2)} 5 104
4.3.3.10. Reaction of [Ru(dtbpoet)H2(H2)] 5 with N2 to [Ru(d,bpoe,)H2(N2)] 52 106
4.33.11. Reaction of [Ru(A^o«)H2(H2)l 5 with D2 to
|DxHRu(rf/^oe,)H2(H2)l[Dx]-5 106
4-3.4. Catalysis ]07
4.3.4.1 Catalytic tf/D-exchange with D2O as Deuterium Source 107
4.3.4.2. Catalytic tf/D-exchange with [D6]benze„e as Deuterium Source 113
43.4.3. CatalyticDehydrogenationofAlcohols 119
5 Figure Index 126
6 Scheme Index 129
7 Table Index 132
8 Abbreviation Index 133
9 Compound Name Index 135
10 Compound Structure Index 138
11 Literature 146 |
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| author | Prechtl, Martin 1978- |
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| index_date | 2024-07-02T20:42:12Z |
| indexdate | 2024-07-09T21:15:01Z |
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| isbn | 9783865532299 |
| language | English |
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| physical | XIII, 152 S. graph. Darst. |
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| spelling | Prechtl, Martin 1978- Verfasser (DE-588)131737368 aut Novel ruthenium dihydrogen complexes and their application in catalysis vorgelegt von Martin H. G. Prechtl Duisburg [u.a.] WiKu-Verl. 2007 XIII, 152 S. graph. Darst. txt rdacontent n rdamedia nc rdacarrier Wissenschaftliche Monographie der MPG und der RWTH Aachen Zugl.: Aachen, Techn. Hochsch., Diss., 2007 Hydridokomplexe swd Katalyse swd Rutheniumkomplexe swd (DE-588)4113937-9 Hochschulschrift gnd-content HBZ Datenaustausch application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=016472431&sequence=000002&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis |
| spellingShingle | Prechtl, Martin 1978- Novel ruthenium dihydrogen complexes and their application in catalysis Hydridokomplexe swd Katalyse swd Rutheniumkomplexe swd |
| subject_GND | (DE-588)4113937-9 |
| title | Novel ruthenium dihydrogen complexes and their application in catalysis |
| title_auth | Novel ruthenium dihydrogen complexes and their application in catalysis |
| title_exact_search | Novel ruthenium dihydrogen complexes and their application in catalysis |
| title_exact_search_txtP | Novel ruthenium dihydrogen complexes and their application in catalysis |
| title_full | Novel ruthenium dihydrogen complexes and their application in catalysis vorgelegt von Martin H. G. Prechtl |
| title_fullStr | Novel ruthenium dihydrogen complexes and their application in catalysis vorgelegt von Martin H. G. Prechtl |
| title_full_unstemmed | Novel ruthenium dihydrogen complexes and their application in catalysis vorgelegt von Martin H. G. Prechtl |
| title_short | Novel ruthenium dihydrogen complexes and their application in catalysis |
| title_sort | novel ruthenium dihydrogen complexes and their application in catalysis |
| topic | Hydridokomplexe swd Katalyse swd Rutheniumkomplexe swd |
| topic_facet | Hydridokomplexe Katalyse Rutheniumkomplexe Hochschulschrift |
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