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Comparative Study of Cl-Atom Reactions in Solution Using Time-Resolved Vibrational Spectroscopy.

Jae Yoon Shin1, Amanda S Case1, F Fleming Crim1

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Summary
This summary is machine-generated.

Chlorine atoms react with alkanes and alkenes, forming vibrationally excited HCl. Solvent viscosity and reaction exoergicity influence HCl excitation, while C=C bonds accelerate reaction rates, especially for DMHD.

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Area of Science:

  • Chemical Kinetics
  • Reaction Dynamics
  • Physical Chemistry

Background:

  • Understanding the reaction mechanisms of chlorine atoms with hydrocarbons is crucial for atmospheric chemistry and combustion processes.
  • Hydrogen abstraction reactions are fundamental in radical chemistry.
  • The influence of molecular structure and solvent properties on reaction outcomes requires detailed investigation.

Purpose of the Study:

  • To investigate the hydrogen-abstraction reactions of chlorine atoms with 2,3-dimethylbutane (DMB), 2,3-dimethyl-2-butene (DMBE), and 2,5-dimethyl-2,4-hexadiene (DMHD).
  • To determine the extent of vibrational excitation in the HCl product and its dependence on reaction exoergicity and solvent viscosity.
  • To measure the bimolecular reaction rates and elucidate the role of intermolecular forces and molecular structure.

Main Methods:

  • Solution-phase reactions studied using hydrogen-abstraction pathways.
  • Detection and quantification of vibrationally excited HCl (v=1) using branching fractions (Γ(v=1)).
  • Measurement of bimolecular reaction rate constants in CCl4 and CDCl3 solvents.

Main Results:

  • Vibrationally excited HCl (v=1) was observed for reactions with alkenes (DMBE and DMHD) due to high exoergicity.
  • Branching fractions for HCl (v=1) were higher in less viscous CDCl3, indicating reduced damping of vibrational excitation.
  • Reaction rates were diffusion-limited, with Cl + DMHD exceeding typical limits due to attractive forces with the C=C bond.

Conclusions:

  • Reaction exoergicity and solvent viscosity significantly impact the vibrational excitation of HCl products.
  • The presence of a C=C bond enhances reaction rates, with multiple C=C bonds and molecular geometry further increasing reactivity.
  • Attractive intermolecular forces between Cl atoms and C=C bonds play a key role in accelerating reaction rates beyond diffusion control.