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Hydration and secondary ozonide of the Criegee intermediate of Sabinene
Journal article   Open access   Peer reviewed

Hydration and secondary ozonide of the Criegee intermediate of Sabinene

M.H. Almatarneh, I.A. Elayan, M. Altarawneh and J.W. Hollett
ACS Omega, Vol.3(2), pp.2417-2427
2018
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Abstract

A computational study of the formation of secondary ozonide (SOZ) from the Criegee intermediates (CIs) of sabinene, including hydration reactions with H2O and 2H2O, was performed. All of the geometries were optimized at the B3LYP and M06-2X with several basis sets. Further single-point energy calculation at the CCSD(T) was performed. Two major pathways of SOZ formation suggest that it is mainly formed from the sabinene CI and formaldehyde rather than sabina ketone and formaldehyde-oxide. However, in both pathways, the activation energies are within a range of ±5 kJ mol–1. Furthermore, the hydration reactions of the anti-CI with H2O and 2H2O showed that the role of the second water molecule is a mediator (catalyst) in this reaction. The dimer hydration reaction has lower activation energies than the monomer by 60 and 69 kJ mol–1, at the M06-2X/6-31G(d) and CCSD(T)+CF levels of the theory, respectively. A novel water-mediated vinyl hydroperoxide (VHP) channel from both the monomer and dimer has been investigated. The results indicate that the direct nonmediated VHP formation and dissociation is interestingly more possible than the water-mediated VHP. The density functional theory calculations show that the monomer is faster than the dimer by roughly 22 kJ mol–1. Further, the infrared spectrum of sabina ketone was calculated at B3LYP/6-311+G(2d,p); the calculated carbonyl stretching of 1727 cm–1 is in agreement with the experimental range of 1700–1800 cm–1.

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8 Earth Sciences
8.124 Environmental Sciences
8.124.10 Atmospheric Aerosols
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Chemistry, Multidisciplinary
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Chemistry
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