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Anharmonic kinetics of the cyclopentane reaction with hydroxyl radical

Junjun Wu, Lu Gem Gao, Wei Ren, Donald G. Truhlar

2020Chemical Science31 citationsDOIOpen Access PDF

Abstract

for reaction energies and barrier heights. A quadratic-quartic function is adopted to describe the ring bending potential of cyclopentane, and the quartic anharmonicity in the bending mode is treated by a one-dimensional Schrödinger equation using both Wentzel-Kramers-Brillouin (WKB) and Fourier Grid Hamiltonian (FGH) methods. The torsional anharmonicity in the transition state is treated in turn by the free rotor approximation, the one-dimensional hindered rotor approximation, and the multi-structural torsional anharmonicity method. Rate constants of the title reaction are computed by canonical variational transition state theory including tunneling by the multi-dimensional small-curvature tunneling approximation (CVT/SCT). The final rate constants include the quasiharmonic, quadratic-quartic, and torsional anharmonicity. Our calculations are in excellent agreement with all the experimental data available at both combustion and atmospheric temperatures with a deviation of less than 30%.

Topics & Concepts

CyclopentaneAnharmonicityKineticsQuartic functionChemistryHydrocarbonPhotochemistryQuadratic equationComputational chemistryOrganic chemistryPhysicsClassical mechanicsMathematicsQuantum mechanicsGeometryPure mathematicsFree Radicals and AntioxidantsThermal and Kinetic AnalysisChemical Thermodynamics and Molecular Structure