Competition Kinetics of the Nonbranched-Chain Addition of Free Radicals to Olefins, Formaldehyde, and Oxygen

Five reaction schemes are suggested for the initiated nonbranched-chain addition of free radicals to the multiple bonds of alkenes, formaldehyde, and oxygen. The schemes include reactions competing with chain propagation through a reactive free radical. The chain evolution stage in these schemes inv...

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Main Author: M. M. Silaev
Format: Article
Language:English
Published: Wiley 2011-01-01
Series:International Journal of Chemical Engineering
Online Access:http://dx.doi.org/10.1155/2011/830610
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author M. M. Silaev
author_facet M. M. Silaev
author_sort M. M. Silaev
collection DOAJ
description Five reaction schemes are suggested for the initiated nonbranched-chain addition of free radicals to the multiple bonds of alkenes, formaldehyde, and oxygen. The schemes include reactions competing with chain propagation through a reactive free radical. The chain evolution stage in these schemes involves three or four types of free radicals. One of them— CH2=C(CH3)•CH2, CH2=CH•CHOH, H•C=O, 𝑜−CH3C6H4CH2O•4, or HO•4—is relatively low-reactive and inhibits the chain process by shortening of the kinetic chain length. Based on the suggested schemes, nine rate equations containing one to three parameters to be determined directly are set up using quasi-steady-state treatment. These equations provide good fits for the nonmonotonic (peaking) dependences of the formation rates of the molecular addition products (1 : 1 adducts) on the concentration of the unsaturated component in liquid homogeneous binary systems consisting of a saturated component (hydrocarbon, alcohol, etc.) and an unsaturated component (olefin, formaldehyde, or dioxygen). The unsaturated compound in these systems is both a reactant and an autoinhibitor generating low-reactive free radicals. A similar kinetic description is applicable to nonbranched-chain free-radical hydrogen oxidation. The energetics of the key radical-molecule reactions is considered.
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spelling doaj-art-59bc33de295b41a3a62153f56d2b51fc2025-08-20T02:05:32ZengWileyInternational Journal of Chemical Engineering1687-806X1687-80782011-01-01201110.1155/2011/830610830610Competition Kinetics of the Nonbranched-Chain Addition of Free Radicals to Olefins, Formaldehyde, and OxygenM. M. Silaev0Department of Chemistry, Moscow State University, Vorob'evy Gory, Moscow 119991, RussiaFive reaction schemes are suggested for the initiated nonbranched-chain addition of free radicals to the multiple bonds of alkenes, formaldehyde, and oxygen. The schemes include reactions competing with chain propagation through a reactive free radical. The chain evolution stage in these schemes involves three or four types of free radicals. One of them— CH2=C(CH3)•CH2, CH2=CH•CHOH, H•C=O, 𝑜−CH3C6H4CH2O•4, or HO•4—is relatively low-reactive and inhibits the chain process by shortening of the kinetic chain length. Based on the suggested schemes, nine rate equations containing one to three parameters to be determined directly are set up using quasi-steady-state treatment. These equations provide good fits for the nonmonotonic (peaking) dependences of the formation rates of the molecular addition products (1 : 1 adducts) on the concentration of the unsaturated component in liquid homogeneous binary systems consisting of a saturated component (hydrocarbon, alcohol, etc.) and an unsaturated component (olefin, formaldehyde, or dioxygen). The unsaturated compound in these systems is both a reactant and an autoinhibitor generating low-reactive free radicals. A similar kinetic description is applicable to nonbranched-chain free-radical hydrogen oxidation. The energetics of the key radical-molecule reactions is considered.http://dx.doi.org/10.1155/2011/830610
spellingShingle M. M. Silaev
Competition Kinetics of the Nonbranched-Chain Addition of Free Radicals to Olefins, Formaldehyde, and Oxygen
International Journal of Chemical Engineering
title Competition Kinetics of the Nonbranched-Chain Addition of Free Radicals to Olefins, Formaldehyde, and Oxygen
title_full Competition Kinetics of the Nonbranched-Chain Addition of Free Radicals to Olefins, Formaldehyde, and Oxygen
title_fullStr Competition Kinetics of the Nonbranched-Chain Addition of Free Radicals to Olefins, Formaldehyde, and Oxygen
title_full_unstemmed Competition Kinetics of the Nonbranched-Chain Addition of Free Radicals to Olefins, Formaldehyde, and Oxygen
title_short Competition Kinetics of the Nonbranched-Chain Addition of Free Radicals to Olefins, Formaldehyde, and Oxygen
title_sort competition kinetics of the nonbranched chain addition of free radicals to olefins formaldehyde and oxygen
url http://dx.doi.org/10.1155/2011/830610
work_keys_str_mv AT mmsilaev competitionkineticsofthenonbranchedchainadditionoffreeradicalstoolefinsformaldehydeandoxygen