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Effect of OH radicals, relative humidity, and time on the composition of the products formed in the ozonolysis of α-pinene
Umeå University, Faculty of Science and Technology, Chemistry.
Umeå University, Faculty of Science and Technology, Chemistry.
Umeå University, Faculty of Science and Technology, Chemistry.
2003 (English)In: Atmospheric Environment, Vol. 37, no 29, 4087-96 p.Article in journal (Refereed) Published
Abstract [en]

The gas-phase ozonolysis of α-pinene at ppb levels were studied and the effects of OH radicals formed in the reaction, the relative humidity (RH), and time on the products formed were investigated. Identified products were pinic acid, glyoxal, methyl glyoxal, norpinonic acid and a norpinonic acid isomer, pinonic acid, a C4 dicarbonyl, a C5 dicarbonyl, norpinon aldehyde, and pinon aldehyde. The different parameters effect on the formation of these products were evaluated using experimental design and multivariate modeling. Pinonic acid, norpinonic acid and its isomer, were not detected in the absence of OH radicals. The amounts of pinic acid, norpinon aldehyde, and pinon aldehyde all decreased in the absence of OH radicals. Glyoxal and methyl glyoxal were not affected.

The formation of pinonic acid decreased when the RH was increased. The formation of pinic acid, glyoxal, methyl glyoxal, and pinon aldehyde increased with increasing RH, while norpinon aldehyde was not affected. The implications of these observations and additional interaction effects are discussed, and a novel route of the formation of pinic acid is presented.

Place, publisher, year, edition, pages
2003. Vol. 37, no 29, 4087-96 p.
Keyword [en]
Criegee intermediate, Experimental design, Monoterpenes, Pinic acid, Pinon aldehyde
Identifiers
URN: urn:nbn:se:umu:diva-9215DOI: doi:10.1016/S1352-2310(03)00522-3OAI: oai:DiVA.org:umu-9215DiVA: diva2:148886
Available from: 2008-03-11 Created: 2008-03-11 Last updated: 2012-05-22Bibliographically approved
In thesis
1. Chemical reactions in ventilation systems: Ozonolysis of monoterpenes
Open this publication in new window or tab >>Chemical reactions in ventilation systems: Ozonolysis of monoterpenes
2003 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Chemicals in indoor air, either emitted from a source or from a reaction, have been suggested to cause ill health in buildings. However, no clear correlations between exposure and health effects have been made.

In this thesis we studied the reaction between monoterpenes, a group of biogenic unsaturated C10 hydrocarbons, and ozone. Ozonolysis of monoterpenes was used as model reactions for unsaturated compounds in ambient air. Also the products formed from these reactions have been suggested as important participants in the occurrence of discomfort and ill health in buildings.

To enable a reliable and sensitive measurement of ppb-ppt levels of monoterpenes and the formed products in the presence of ozone an evaluation of available scrubber materials was made. Potassium iodide was shown to remove ambient levels of ozone and have a recovery of >95% for all monoterpenes and formed products included in the investigation.

Experimental conditions showed to have a large impact on the initial steps of the ozonolysis, and also on the composition of the formed products. We showed that water plays an important and complex role both in the initial stage of ozonolysis of ∆3-carene and in the formation and composition of products from the ozonolysis of ∆-pinene. The use of experimental design facilitated the evaluation of the investigated reactions. We showed that the formation of OH radicals could be studied using multiple linear regression models and that the presence or absence of OH radicals had a profound impact on the formation of many of the formed products. We also made an observation of the lack of formed OH radicals in the ozonolysis of limonene and discussed probable causes of this observation.

Despite the short reaction times and the ambient levels of ozone and monoterpenes used in our experiments we showed that a number of oxidation products were formed, and that the reaction rate is significantly increased in a ventilation system. This formation is underestimated by theoretical calculations and leads to high amounts of known irritants in the indoor air. We showed that theoretical calculations underestimate the formation of these oxidation products 3-13 times, depending on ventilation system and monoterpene.

Place, publisher, year, edition, pages
Umeå: Umeå universitet, 2003. 61 p.
Keyword
Environmental chemistry, Monoterpene, Ozone, OH Radical, Ozonolysis, Ventilation, Potassium Iodide, Experimental Design, Heat Exchanger, Miljökemi
National Category
Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-97 (URN)91-7305-511-5 (ISBN)
Public defence
2003-10-03, KB3B1, KBC, Umeå, 13:00
Opponent
Supervisors
Available from: 2003-09-10 Created: 2003-09-10 Last updated: 2012-05-22Bibliographically approved

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Fick, JerkerPommer, LindaAndersson, Barbro

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