Synthesis and reactivity of triangular phosphido-bridged transition metal clusters

dc.contributor.authorDehghan, Khashayar
dc.contributor.supervisorDixon, Keith R.
dc.date.accessioned2018-06-19T21:51:32Z
dc.date.available2018-06-19T21:51:32Z
dc.date.copyright1990en_US
dc.date.issued2018-06-19
dc.degree.departmentDepartment of Chemistry
dc.degree.levelDoctor of Philosophy Ph.D.en_US
dc.description.abstractThe synthesis, reactivity, and spectroscopic properties of a series of triangular phosphido-bridged rhodium, iridium, palladium and platinum clusters are described. Throughout the project, X-ray diffraction and 31P{1H} NMR spectroscopy are the main techniques for characterizing compounds. In the first part of this report, the lability of μ-X and terminal phosphines in [M3(μ-X)(μ-PPh2)2(PPh3)3)[BF4](M= Pd, X= Cl; M=Pt, X= H) is utilized to prepare a number of compounds where the integrity of the triangular framework is maintained. The molecular structures of three representative examples: [Pd3(μ-SCH2Ph)(μ-PPh2)2(PEt3)3][BF4] [Pt3(μ-Cl)(μ-PPh2)2(PR3)3][BF4) (R= Ph, Et) were determined and are described. Reaction of these palladium and platinum trinuclear clusters with chelating ligands, R’2PYPR”2 (Y= O, CH2), results in unusual cluster fragmentation to give novel dinuclear monocations, [M2(μ-PP2)(μ-R’2PYPR”2) (PR3)2)+ (M= Pd, Pt) in which a metal-metal bond is supported by both dppm and phosphido bridges. These dimers are very inert failing to react with a number of reagents including C4H6, HCCCO2Me, CH2N2, CO, CH3I (when M= Pd), H2, HBF4 and CH2I2. The cluster, [Pt3(μ-H)(μ-PPh2)2(PPh3)3] [BF4], also reacts with ButNC to afford the dinuclear species (Pt2(μ-PPh2)2(ButNC)(PPh3)3]+. The crystal structures of fragmentation products [Pd2(μ-PPh2)( μ-Pri2PCH2PPh2)(PPh3)2] [BF4], (Pt2(μ-PPh2)( μ-Me2PCH2PMe2)(PPh3)2]2 [C2O4] and (Pt2(μ-PPh2)(ButNC)(PPh3)3]2(C2O4) are reported and discussed. In the last part, the synthesis of a novel trinuclear iridium cluster, [Ir3(μ-PPh2)3(CO)5], is described, and the reactions of this cluster and its previously reported rhodium analogue, [Rh3(μ-PPh2)3(PPh3)2(CO)3], with dppm afford not fragmentation, but substitution products. The complex (Ir3(μ-PPh2)3(CO)5] also reacts with ButNC to yield [Ir3(μ-PPh2)3(CO)5(ButNC)2]. The crystal structures of the compounds, [M3(μ-PPh2)3(μ-dppm)(CO)3] (M= Rh, Ir) and (Ir3(μ-PPh2)3(CO)5(ButNC)2], are also reported.en_US
dc.description.scholarlevelGraduateen_US
dc.identifier.urihttp://hdl.handle.net/1828/9475
dc.languageEnglisheng
dc.language.isoenen_US
dc.rightsAvailable to the World Wide Weben_US
dc.subjectTransition metal compoundsen_US
dc.subjectSynthesisen_US
dc.subjectReactivityen_US
dc.subjectSpectraen_US
dc.titleSynthesis and reactivity of triangular phosphido-bridged transition metal clustersen_US
dc.typeThesisen_US

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