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• W2014533252 abstract "This work investigates the unimolecular dissociation of the 2-buten-2-yl radical. This radical has three potentially competing reaction pathways: C−C fission to form CH3 + propyne, C−H fission to form H + 1,2-butadiene, and C−H fission to produce H + 2-butyne. The experiments were designed to probe the branching to the three unimolecular dissociation pathways of the radical and to test theoretical predictions of the relevant dissociation barriers. Our crossed laser-molecular beam studies show that 193 nm photolysis of 2-chloro-2-butene produces 2-buten-2-yl in the initial photolytic step. A minor C−Cl bond fission channel forms electronically excited 2-buten-2-yl radicals and the dominant C−Cl bond fission channel produces ground-state 2-buten-2-yl radicals with a range of internal energies that spans the barriers to dissociation of the radical. Detection of the stable 2-buten-2-yl radicals allows a determination of the translational, and therefore internal, energy that marks the onset of dissociation of the radical. The experimental determination of the lowest-energy dissociation barrier gave 31 ± 2 kcal/mol, in agreement with the 32.8 ± 2 kcal/mol barrier to C−C fission at the G3//B3LYP level of theory. Our experiments detected products of all three dissociation channels of unstable 2-buten-2-yl as well as a competing HCl elimination channel in the photolysis of 2-chloro-2-butene. The results allow us to benchmark electronic structure calculations on the unimolecular dissociation reactions of the 2-buten-2-yl radical as well as the CH3 + propyne and H + 1,2-butadiene bimolecular reactions. They also allow us to critique prior experimental work on the H + 1,2-butadiene reaction." @default.
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• W2014533252 date "2005-06-30" @default.
• W2014533252 modified "2023-10-18" @default.
• W2014533252 title "A Study of the Unimolecular Dissociation of the 2-Buten-2-yl Radical via the 193 nm Photodissociation of 2-Chloro-2-butene" @default.
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• W2014533252 doi "https://doi.org/10.1021/jp050970e" @default.
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