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• W2894639339 abstract "The sequential activation of up to 4 CH4 molecules by Ir+ is investigated through a gas-phase infrared multiple photon dissociation (IRMPD) experiment and theoretical calculations. A molecular beam apparatus was used to generate Ir+ by laser ablation and expose it to controlled amounts of CH4. Product ions were irradiated with IR light from a free electron laser over the 500–1800 cm−1 spectral range and photodissociation was monitored using a time-of-flight mass spectrometer. Experimental spectra were obtained for five distinct species: [Ir,3C,8 H]+, [Ir,3C,10 H]+, [Ir,4C,10 H]+, [Ir,4C,12 H]+, and [Ir,O,3C,12 H]+. To identify these species, B3LYP/def2-TZVPPD geometry optimizations were performed on a variety of possible structures, with computed IR spectra compared to the experimental IRMPD spectra. This has led to the following assignments: [Ir,3C,8 H]+ = IrCH2(CH3)2+, [Ir,3C,10 H]+ = HIr(CH3)3+, [Ir,4C,10 H]+ = Ir(CH3)2(C2H4)+, [Ir,4C,12 H]+ = a mixture of HIr(CH3)(C2H4)+(CH4), HIr(CH3)2(C2H5)+, Ir(CH3)4+, and (H2)Ir(CH3)2(C2H4)+, and [Ir,O,3C,12 H]+ = (H2O)HIr(CH3)3+. Notably, evidence for CC coupling is observed upon reaction with a fourth methane. Mechanisms for the formation of the observed products were also explored computationally by examining the reaction coordinate pathways for the reactions of methane with HIrCH+, IrCH2+, Ir(CH3)2+, HIrCH2(CH3)+, HIr(CH3)3+, and IrCH2(CH3)2+." @default.
• W2894639339 created "2018-10-12" @default.
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• W2894639339 date "2019-01-01" @default.
• W2894639339 modified "2023-10-14" @default.
• W2894639339 title "Sequential activation of methane by Ir+: An IRMPD and theoretical investigation" @default.
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• W2894639339 doi "https://doi.org/10.1016/j.ijms.2018.10.007" @default.
• W2894639339 hasPublicationYear "2019" @default.
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