FT-ICR studies of transition metal cluster ions [Elektronische Ressource] / Iulia Balteanu

Informations

• Publié par: technische_universitat_munchen
• Publié le: 01 janvier 2005
• Nombre de lectures: 14
• Langue: Deutsch
• Poids de l'ouvrage: 2 Mo

Extrait

FT-ICR Studies of
Transition Metal Cluster Ions

Iulia Balteanu






Dissertation
Technische Universität München








Technische Universität München
Fakultät für Chemie
- Lehrstuhl II für Physikalische Chemie -


FT-ICR Studies of Transition Metal Cluster Ions

Iulia Balteanu


Vollständiger Abdruck der von der Fakultät für Chemie der Technischen Universität
München zur Erlangung des akademischen Grades eines

Doktors der Naturwissenschaften

genehmigten Dissertation.



Vorsitzender: Univ.-Prof. Dr. U. K. Heiz

Prüfer der Dissertation:

1. Univ.-Prof. V. E. Bondybey, Ph.D. (Univ. of California, Berkeley, USA)
2. Univ.-Prof. Dr. K. Köhler



Die Dissertation wurde am 11.01.2005 bei der Technischen Universität München
eingereicht und durch die Fakultät für Chemie am 11.02.2005 angenommen.









For Buni
In memory of my grandmother, Mémé









































Contents 5


Contents

1. Introduction 9

2. Experimental and Theoretical Methods 15
2.1. Fourier Transform Ion Cyclotron Resonance Mass Spectrometry 15
2.1.1. General 15
2.1.2. The Garching FT-ICR Mass Spectrometer Garching FTICR 19
2.1.3. The Laser Vaporization Molecular Beam Ion Source 22
2.2. Ion-molecule Reactions 24
2.3. References 25

3. CO Adsorption on Anionic Gold Clusters: Implications for Catalytic Activity 29
3.1. Introduction 29
3.2. Experimental Details 31
3.3. Results and Discussion 33
3.4. Conclusions 47
3.5. References 48

4. Size and Charge-state Dependent Reactivity of Azidoacetonitrile with
+/-
Anionic and Cationic Rhodium Clusters Rh 51 n
4.1. Introduction 51
4.2. Experimental Details 54 6 Contents

4.3. Results and Discussion 55
4.3.1. Reactions of Anionic Clusters 56
4.3.2. Reactions of Cationic Clusters 61
4.3.3. Comparison of Cationic and Anionic Clusters 70
4.4. Conclusions 72
4.5. References 73

5. Reactions of Rhodium Cationic Clusters with Ethane 77
5.1. Introduction 77
5.2. Experimental Details 78
5.3. Computational Details 79
5.4. Results and Discussion 79
5.5. Conclusions 93
5.6. References 93

6. Isotopically Enriched Platinum Cluster Studies.
195 ±Reactions of Platinum Clusters Pt , n=1-23, with N O and CO 97 n 2
6.1. Introduction 97
6.2. Experimental Details 99
6.3. Results and Discussion 100
195 ±
6.3.1. Reactions of Platinum Clusters Pt , n = 1 - 23, n
with NO 101 2
195 +/- 6.3.2. Saturation Reactions of Platinum Clusters Pt , n
n = 1 - 24, with CO 108
6.3.3. Catalytic Oxidation of CO on Gas Phase Platinum Clusters 120 Contents 7

6.4. Conclusions 126
6.5. References

7. Methane and Deuterated Methane Activation by Platinum Cluster Ions 131
7.1. Introduction 131
7.2. Experimental Details 132
7.3. Results 133
7.3.1. Reactions of Cationic Clusters 133
7.3.2. Reactions of Anionic Clusters 139
7.4. Discussion 141
7.5. Conclusions 143
7.6. References 144

8. Summary 147

Appendix
A List ofPublications 153
B List of Presentations at Scientific Workshops and Conferences 157

Acknowledgements 161




8 Contents