Synthesis of Mixed Transition Metal Clusters of Osmium and Rhenium Via Metal Hydride Coupling Reactions PDF Download
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Author: Gregory Alan Pearson
Publisher:
ISBN:
Category :
Languages : en
Pages : 262
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Author: Gregory Alan Pearson
Publisher:
ISBN:
Category :
Languages : en
Pages : 262
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Author: Po-Kwan Jasmine Lau
Publisher: Open Dissertation Press
ISBN: 9781361426876
Category :
Languages : en
Pages :
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This dissertation, "The Chemistry of Mixed-metal Clusters of Osmium and Rhodium" by Po-kwan, Jasmine, Lau, 劉寶君, was obtained from The University of Hong Kong (Pokfulam, Hong Kong) and is being sold pursuant to Creative Commons: Attribution 3.0 Hong Kong License. The content of this dissertation has not been altered in any way. We have altered the formatting in order to facilitate the ease of printing and reading of the dissertation. All rights not granted by the above license are retained by the author. Abstract: Abstract of thesis entitled THE CHEMISTRY OF MIXED-METAL CLUSTERS OF OSMIUM AND RHODIUM Submitted by LAU PO KWAN JASMINE for the degree of Doctor of Philosophy at The University of Hong Kong in December 2005 The general background of metal clusters, the chemistry of osmium-rhodium mixed-metal clusters, and their potential catalytic applications are reviewed. The work in the synthesis, characterizations, and reactivity studies of different series of osmium-rhodium mixed-metal clusters help us to understand the properties and reactivities of new clusters as compared to the bulk metal surface. 1 1 1 A novel face-capping mode of toluene was observed in [Os Rh (μ -η η η - 3 4 3 C H CH )(CO) ] 1. Cluster 1, together with [Os Rh(-H)(η -C H CH )(CO) ] 2 6 5 3 13 4 6 5 3 12 and a known compound [Os Rh (η -C H CH )(-CO)(CO) ], were obtained from 5 2 6 5 3 16 the reaction of [Os Rh(μ-H) (CO) ] with toluene in the presence of an excess 3 3 12amount of 4-vinylphenol. The reaction of [Os Rh(-H) (CO) ] with an excess 3 3 12 amount of 4-vinylphenol (as a hydride acceptor) in refluxing m-xylene, chlorobenzene, or benzene yielded three new clusters [Os Rh {η -C H (CH ) } 5 2 6 4 3 2 6 6 (-CO)(CO) ] 3, [Os Rh (η -C H Cl)(-CO)(CO) ] 4, and [Os Rh (η -C H ) 16 5 2 6 5 16 5 2 6 6 (-CO)(CO) ] 5, respectively. 16 The hydrogenation of [Os Rh (η -C H CH )(-CO)(CO)] with 5 2 6 5 3 16 [Os (-H) (CO) ] resulted in moderate yields of two hydrogen-rich compounds: 3 2 10 [Os Rh (-H) (CO) ] 6 and [Os Rh Cl(-H) (CO) ] 7. The reaction of 7 3 11 23 5 3 8 18 [Os Rh (η -C H CH )(-CO)(CO) ] with hydrogen yielded a new cluster 5 2 6 5 3 16 compound, [Os Rh(-H) (CO) ] 8. A deuterium exchange experiment was 5 5 18 performed on 6, and 7. Both the compounds proved to be able to exchange the H atom with D in the presence of D SO, and the absence of the hydride signal in the 2 4 H NMR spectrum is consistent with this. Therefore, clusters 6 and 7 may serve as appropriate new hydrogen storage models. A detailed discussion of the chemistry of anionic osmium-rhodium mixed-metal clusters with Au cationic fragments using [Au(PPh )Cl] and [(AuCl) L-L], where L 3 2 = dppe (bis(diphenylphosphino)ethane) or dppp (bis(diphenylphosphino)propane), is presented. Two mono-anionic osmium-rhodium mixed-metal clusters [PPN][Os Rh(μ-CO)(CO) ] 9 and [PPN][Os Rh (μ-CO) (CO) ] 10 were prepared 6 19 9 3 2 26 by the thermolysis of [Os Rh(μ-H) (CO) ]. Electrochemistry studies on 10 showed 3 3 12 four successive redox couples, and revealed a novel electron reservoir property. Treatment of 9 with two equivalent of [Au(PPh)Cl] gave compounds [Os Rh Au(CO) (PPh )] 11, and [Os Au (CO) (PPh ) ][Os Rh(μ-CO)(CO) ] 12. 4 3 18 3 5 3 15 3 3 6 19 Both compounds successfully demonstrated the introduction of the Au(PR ) units 3into transition-metal clusters. Two linked clusters [{Os RhAu(μ-CO)(CO) } (dppp)] 6 19 2 13 and [{Os RhAu(μ-CO)(CO) } (dppe)] 14 were prepared by the reaction of 9 6 19 2 with two equivalent [(AuCl) dppp] and [(AuCl) dppe], respectively. 2 2 The synthesis and characterization of linked cluster [{Os (CO) (μ -H)} 3 10 2 2 {μ,μ -NC H C H N}] 15 from the reaction of [Os Rh(μ-H) (CO) ] with aniline in 2 2 6 4 6 4 3 3 12 the presence of an excess amount of 4-vinyl phenol
Author: University of Illinois at Urbana-Champaign. Department of Chemistry
Publisher:
ISBN:
Category : Chemistry, Inorganic
Languages : en
Pages : 154
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Author: Thomas Alan Wolfe
Publisher:
ISBN:
Category : Metal crystals
Languages : en
Pages : 468
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Author: Gregory L. Geoffroy
Publisher:
ISBN:
Category :
Languages : en
Pages : 39
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Transition metal cluster complexes have become a very important class of compounds, principally because of their potential in catalysis. Clusters have been shown to behave as catalysts in their own right and they hold considerable promise for serving as models for catalytic surfaces. Clusters comprised of two or more different transition metals in the cluster framework are particularly interesting in this regard because of possible bimetallic effects. Further, mixed-metal clusters have non-equivalent bonding sites. As such they are ideally suited for modeling studies which employ variable temperature NMR to follow the movements of substrates over their surfaces. One of the problems which has hampered studies of mixed-metal clusters is their relative lack of availability. Only a very few isostructural series have been achieved, and general synthetic methods for mixed-metal clusters are lacking. Carbonylmetalates have been widely used as synthetic reagents in cluster chemistry and several of the reported reactions appear to be adaptable to design. This is particularly true of the reactions of Knight and Mays who prepared a series of Group 7 - Group 8 tetrameric mixed-metal clusters through the addition of a carbonylmetalate to a closed M3(CO)12 trimer.
Author: Reuben D. Rieke
Publisher: John Wiley & Sons
ISBN: 1118929144
Category : Science
Languages : en
Pages : 484
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Written by the creator of Rieke metals, valuable for chemical reaction methods and efficiency, this groundbreaking book addresses a significant aspect of organic and inorganic chemistry. The author discusses synthetic methods, preparation procedures, chemical reactions, and applications for highly reactive metals and organometallic reagents. • Addresses a new generation of chemistry that goes beyond the standard use of metals and activation • Provides step-by-step guidelines, chemical equations, and experimental descriptions for handling metals including zinc, magnesium, copper, indium, nickel, manganese, calcium, barium, iron, palladium, platinum, uranium, thorium, aluminum, cobalt, and chromium • Uses a unique approach to highlight methods and techniques that make chemical synthesis and activation of Rieke metals more safe and efficient • Discusses novel applications and special topics, such as highly reactive metals for novel organometallic reagents, semiconducting polymers, plastics electronics, photovoltaics, and the Reformatsky reagent
Author: R. M. Sorrell
Publisher:
ISBN:
Category :
Languages : en
Pages : 0
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Author: University Microfilms International
Publisher: Ann Arbor, Mich. : University Microfilms International
ISBN:
Category : Reference
Languages : en
Pages : 712
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Author:
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Category : Dissertations, Academic
Languages : en
Pages : 548
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Author:
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ISBN:
Category : Dissertation abstracts
Languages : en
Pages : 724
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