Kinetic and Thermodynamic Studies of Gaseous Metallo-Organic Cationic Complexes

Computer Science

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The construction of a custom fabricated photodissociation spectrometer permits the determination of thermodynamic properties (activation energies), reaction rates, and mechanistic details of bare metal cation mediated σ -bond activation in the gas phase. Specifically, the products and rates resulting from the unimolecular decomposition of the Ni^+Acetaldehyde adduct are monitored after absorption of a known amount of energy. The two dissociative products which are observed in high yield are Ni^+ and Ni^+CO. The Ni^+CO fragment ion could result from the activation of a C-C σ-bond or from the activation of a C-H σ-bond. The rate constant for the decarbonylation of Ni^+Acetaldehyde was approximately 30 percent greater than that of the rate constant for the decarbonylation of Ni^+Acetone. For the decarbonylation of Ni^+Acetone, there needs to be a methide shift, whereas in the decarbonylation of Ni^+Acetaldehyde one could have C-C insertion followed by an aldhyde H-shift. The rate-limiting step of the decarbonylation process will be discussed.

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