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Oxidation of terpenes in indoor environments: A study of influencing factors
Umeå University, Faculty of Science and Technology, Ecology and Environmental Science.
2003 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In this thesis the oxidation of monoterpenes by O3 and NO2 and factors that influenced the oxidation were studied. In the environment both ozone (O3) and nitrogen dioxide (NO2) are present as oxidising gases, which causes sampling artefacts when using Tenax TA as an adsorbent to sample organic compounds in the air. A scrubber was developed to remove O3 and NO2 prior to the sampling tube, and artefacts during sampling were minimised when using the scrubber. The main organic compounds sampled in this thesis were two monoterpenes, alfa-pinene and delta-3-carene, due to their presence in both indoor and outdoor air. The recovery of the monoterpenes through the scrubber varied between 75-97% at relative humidities of 15-75%.

The reactions of alfa-pinene and delta-3-carene with O 3, NO2 and nitric oxide (NO) at different relative humidities (RHs) and reaction times were studied in a dark reaction chamber. The experiments were planned and performed according to an experimental design were the factors influencing the reaction (O3, NO2, NO, RH and reaction times) were varied between high and low levels. In the experiments up to 13% of the monoterpenes reacted when O3, NO2, and reaction time were at high levels, and NO, and RH were at low levels. In the evaluation eight and seven factors (including both single and interaction factors) were found to influence the amount of alfa-pinene and delta-3-carene reacted, respectively. The three most influencing factors for both of the monoterpenes were the O 3 level, the reaction time, and the RH. Increased O3 level and reaction time increased the amount of monoterpene reacted, and increased RH decreased the amount reacted.

A theoretical model of the reactions occurring in the reaction chamber was created. The amount of monoterpene reacted at different initial settings of O3, NO2, and NO were calculated, as well as the influence of different reaction pathways, and the concentrations of O3 and NO2, and NO at specific reaction times. The results of the theoretical model were that the reactivity of the gas mixture towards alfa-pinene and delta-3-carene was underestimated. But, the calculated concentrations of O3, NO2, and NO in the theoretical model were found to correspond to a high degree with experimental results performed under similar conditions. The possible associations between organic compounds in indoor air, building variables and the presence of sick building syndrome were studied using principal component analysis. The most complex model was able to separate 71% of the “sick” buildings from the “healthy” buildings. The most important variables that separated the “sick” buildings from the “healthy” buildings were a more frequent occurrence or a higher concentration of compounds with shorter retention times in the “sick” buildings.

The outcome of this thesis could be summarised as follows;

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Place, publisher, year, edition, pages
Umeå: Ekologi och geovetenskap , 2003. , 84 p.
Keyword [en]
Environmental chemistry, Monoterpene, Ozone (O3), Nitrogen dioxide (NO2), Nitrogen oxide (NO), Relative humidity (RH), Modelling, Scrubber, Experimental design, Interaction, Volatile organic compounds (VOC), Sick buildings syndrome (SBS), Principal component analysis (PCA), Indoor air, Ventilation, Tenax TA, Sodium sulphite
Keyword [sv]
Miljökemi
National Category
Environmental Sciences
Research subject
Analytical Chemistry
Identifiers
URN: urn:nbn:se:umu:diva-29ISBN: 91-7305-313-9 (print)OAI: oai:DiVA.org:umu-29DiVA: diva2:142965
Public defence
2003-04-29, Umeå, 10:00
Available from: 2003-04-29 Created: 2003-04-29 Last updated: 2017-01-24Bibliographically approved
List of papers
1. Development of a NO2 scrubber for accurate sampling of ambient levels of terpenes
Open this publication in new window or tab >>Development of a NO2 scrubber for accurate sampling of ambient levels of terpenes
2002 (English)In: Atmospheric Environment, ISSN 1352-2310, E-ISSN 1873-2844, Vol. 36, no 9, 1443-1452 p.Article in journal (Refereed) Published
Abstract [en]

The result of pumping air containing 56 ppb NO2 through a terpene-spiked adsorbent (90–130 ng, 90–100 ml min−1), Tenax TA, for 20 min (1.8–2.0 l) was that 8% of α-pinene, 7% of β-pinene, 21% of Δ3-carene and 5% of limonene were oxidised. In similar experiments with air containing 56 ppb O3, 3% of α-pinene, 4% of β-pinene, 10% of Δ3-carene and 38% of limonene were oxidised. Sampling a mixture of a terpene and NO2 using Tenax TA can give unwanted overestimation of the amount of reaction products from the terpene–NO2 reaction or underestimation of the original terpene levels. A scrubber was needed to reduce the problems caused by interfering reactions on the adsorbent of NO2 and to reduce discrimination of reactive compounds due to their relatively fast decay on the adsorbent. Several chemicals have been tested for their ability of removing NO2 and our objective was to develop a well functioning, reusable, easy to handle, easy manufactured NO2 scrubber. The result of the experiments was a scrubber consisting of two glass fibre filters coated with Na2SO3 assembled in a dust collector. The recovery of the terpenes through the scrubber varied between 75% and 97% at 15–75% relative humidity, and the scrubber is a one-use scrubber due to memory effects. The Na2SO3 scrubber could be stored in room air for at least one month without loosing the capacity of removing NO2.

Keyword
Nitrogen dioxide; Scrubber; Tenax TA; Terpene; Sodium sulphite
National Category
Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-8842 (URN)doi:10.1016/S1352-2310(01)00581-7 (DOI)
Available from: 2008-02-18 Created: 2008-02-18 Last updated: 2017-12-14Bibliographically approved
2. The influence of O3, relative humidity, NO and NO2 on the oxidation of α-pinene and Δ3-carene
Open this publication in new window or tab >>The influence of O3, relative humidity, NO and NO2 on the oxidation of α-pinene and Δ3-carene
2004 (English)In: Journal of Atmospheric Chemistry, ISSN 0167-7764, E-ISSN 1573-0662, Vol. 48, no 2, 173-189 p.Article in journal (Refereed) Published
Abstract [en]

Upto 13% of α-pinene and δ3-carene had reacted after 213 s in this dark experimental set-up, where O3, NO and NO2 were mixed with terpenes at different relative humidities (RHs). The different experiments were planned according to an experimental design, where O3, NO2, NO, RH and reaction time were varied between high and low settings (25 and 75 ppb, 15 and 42%, 44 and 213 s). An increased amount of α-pinene and δ3-carene reacted in the chamber was observed, when the level of O3, NO and reaction time was increased and RH was decreased. In the study, it was found that different interactions affected the amount of terpene reacted as well. These interactions were between O3 and NO, O3 and reaction time, NO and RH, and between NO and reaction time.

Place, publisher, year, edition, pages
Dordrecht: Kluwer Academic Publishers, 2004
Keyword
terpene, oxidation, NO, NO2, humidity
National Category
Environmental Sciences Ecology Meteorology and Atmospheric Sciences
Identifiers
urn:nbn:se:umu:diva-14009 (URN)10.1023/B:JOCH.0000036847.09169.4a (DOI)000223094700004 ()
Available from: 2007-05-21 Created: 2007-05-21 Last updated: 2017-12-14Bibliographically approved
3. An experimental comparison of a kinetic model for the reaction of α-pinene and Δ3-carene with ozone and nitrogen oxides
Open this publication in new window or tab >>An experimental comparison of a kinetic model for the reaction of α-pinene and Δ3-carene with ozone and nitrogen oxides
2004 (English)In: Indoor Air, ISSN 0905-6947, E-ISSN 1600-0668, Vol. 14, no S8, 75-83 p.Article in journal (Refereed) Published
Abstract [en]

A kinetic model was compiled to simulate reactions of the monoterpenes, α-pinene and Δ3-carene, with O3, NO2 and NO. The influence of different initial settings of O3, NO2 and NO on the monoterpene reaction was evaluated. At initial levels of 75 p.p.b. of O3, NO2 and NO each, 1.5% of α-pinene and 1.1% of Δ3-carene were calculated to react after 215 s. The corresponding experimental results showed that 9.3–12.2% of α-pinene and 9.9–11.7% of Δ3-carene reacted. The calculated levels of O3, NO2 and NO were compared to experimental measurements and were shown to correspond well. However, comparison of the amount of monoterpene reacted between calculated and experimental results, demonstrated that the calculations underestimated the amount of monoterpene reacted in the experimental chamber. The difference between experimental and calculated results could, e.g., be the effect of surfaces and the presence of water, which are parameters not included in the kinetic model known to have influence on these reactions.

Place, publisher, year, edition, pages
Köpenhamn: Blackwell Munksgaard, 2004
Keyword
modeling, monoterpene, oxidation, surface, water
National Category
Public Health, Global Health, Social Medicine and Epidemiology Engineering and Technology
Identifiers
urn:nbn:se:umu:diva-14012 (URN)10.1111/j.1600-0668.2004.00302.x (DOI)000227331500008 ()
Available from: 2007-08-17 Created: 2007-08-17 Last updated: 2017-12-14Bibliographically approved
4. Class separation of buildings with high and low prevalence of SBS by principal component analysis
Open this publication in new window or tab >>Class separation of buildings with high and low prevalence of SBS by principal component analysis
Show others...
2004 (English)In: Indoor Air, ISSN 0905-6947, E-ISSN 1600-0668, Vol. 14, no 1, 16-23 p.Article in journal (Refereed) Published
Abstract [en]

In this study, we were able to separate buildings with high and low prevalence of sick building syndrome (SBS) using principal component analysis. The prevalence of SBS was defined by the presence of at least one typical skin, mucosal and general (headache and fatigue) symptom. Data from the Swedish Office Illness Study describing the presence and level of chemical compounds in outdoor, supply, and room air, respectively, were evaluated together with information about the buildings in six models. When all data were included the most complex model was able to separate 71% of the high prevalence buildings from the low prevalence buildings. The most important variable that separates the high prevalence buildings from the low prevalence buildings was a more frequent occurrence or a higher concentration of compounds with shorter retention time in the high prevalence buildings. Elevated relative humidity in supply and room air and higher levels of total volatile organic compounds in outdoor and supply air were more common in high prevalence buildings. Ten building variables also contributed to the separation of the two classes of low and high prevalence buildings.

Place, publisher, year, edition, pages
John Wiley & Sons, 2004
Keyword
Principal component analysis, VOC, Sick building syndrome, Indoor air, Ventilation duct, Office building
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-14022 (URN)10.1111/j.1600-0668.2004.00203.x (DOI)
Note
Errata Indoor Air 14 (2), 144–144. doi:10.1111/j.1600-0668.2004.00246.xAvailable from: 2007-06-18 Created: 2007-06-18 Last updated: 2017-12-14Bibliographically approved

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