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From source to the environment: Strategies for identification and determination of hydroxylated polycyclic aromatic hydrocarbons in complex particulate matrices
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
2017 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

Adverse health effects have been linked to exposure to particulate matter, and wood combustion is considered as an important source of harmful particulate matter in the urban air and environment. Hydroxylated polycyclic aromatic hydrocarbons are a group of compounds with toxic, endocrine disrupting and carcinogenic properties. Sources of hydroxylated polycyclic aromatic hydrocarbons are different incomplete combustion processes, such as coal and wood combustion. They can also be formed by microbiological and/or photochemical degradation of polycyclic aromatic hydrocarbons in the environment.

This thesis describes analytical strategies and methods that have been developed and used for screening, tentative identification and determination of hydroxylated polycyclic aromatic hydrocarbons in wood combustion and urban air particles. Conventional targeted analytical methods have been developed for compounds with available reference standards, while suspect and non-target screening strategies have been used for the identification of suspects and unknown compounds lacking reference standards. Each step of the developed analytical methods is described and discussed: the choice of the analytical strategy, sampling of the matrices, extraction, clean-up, instrumental analysis, data processing and validation of the methods.

The influence of wood type (birch, spruce, pine and aspen) and burning conditions (nominal and high burn rate) on the hydroxylated polycyclic aromatic hydrocarbon emissions has been examined, showing that emissions from nominal burn rate combustion correspond on average to 14 % of the emissions from high burn rate combustion. It has been shown that spruce and pine have the highest emissions for nominal burn rate and high burn rate combustion, respectively.

The composition of wood combustion particles has been examined and 32 suspect hydroxylated polycyclic aromatic hydrocarbons have been tentatively identified together with 20 other oxygen-containing small molecular weight compounds. Furthermore, the presence of hydroxylated polycyclic aromatic hydrocarbons in airborne particles from an urban background and a car tunnel has been investigated, and nine target and 11 suspect hydroxylated polycyclic aromatic hydrocarbons have been determined and tentatively identified, respectively.

In summary, this thesis has shown that wood combustion is an important emission source of hydroxylated aromatic hydrocarbons and that the chemical composition of the emitted particles strongly depends on both burning conditions and wood type. Furthermore, the findings suggest that there might be other sources of these compounds in the urban environment than wood burning, such as the traffic. Thus, further investigations are required to fully understand the formation, sources and presence of hydroxylated polycyclic aromatic hydrocarbons in the atmosphere. The suitability of different analytical strategies and methods for identification and determination of hydroxylated polycyclic aromatic hydrocarbons is also discussed.

Ort, förlag, år, upplaga, sidor
Stockholm: Department of Environmental Science and Analytical Chemistry, Stockholm University , 2017. , s. 80
Nyckelord [en]
OH-PAHs, hydroxy-PAHs, particulate matter, PM, airborne particles, combustion particles, wood combustion, suspect screening, non-target screening, high resolution mass spectrometry, HRMS, atmospheric pressure photoionization, APPI
Nationell ämneskategori
Analytisk kemi
Forskningsämne
analytisk kemi
Identifikatorer
URN: urn:nbn:se:su:diva-137214ISBN: 978-91-7649-646-6 (tryckt)ISBN: 978-91-7649-647-3 (tryckt)OAI: oai:DiVA.org:su-137214DiVA, id: diva2:1061042
Disputation
2017-02-24, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 10:00 (Engelska)
Opponent
Handledare
Anmärkning

At the time of the doctoral defense, the following paper was unpublished and had a status as follows: Paper 4: Manuscript.

Tillgänglig från: 2017-02-01 Skapad: 2016-12-30 Senast uppdaterad: 2019-08-27Bibliografiskt granskad
Delarbeten
1. Determination of hydroxylated polycyclic aromatic hydrocarbons by HPLC-photoionization tandem mass spectrometry in wood smoke particles and soil samples
Öppna denna publikation i ny flik eller fönster >>Determination of hydroxylated polycyclic aromatic hydrocarbons by HPLC-photoionization tandem mass spectrometry in wood smoke particles and soil samples
2015 (Engelska)Ingår i: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650, Vol. 407, nr 16, s. 4523-4534Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

A simple and fast method for analysis of hydroxylated polycyclic aromatic hydrocarbons using pressurized liquid extraction and high performance liquid chromatography utilizing photoionization tandem mass spectrometry was developed. Simultaneous separation and determination of nine hydroxylated polycyclic aromatic hydrocarbons and two hydroxy biphenyls could be performed in negative mode with a run time of 12 min, including equilibration in 5 min. The calibration curves were in two concentration ranges; 1-50 ng/mL and 0.01-50 mu g/mL, with coefficients of correlation R (2) > 0.997. The limits of detection and method quantification limits were in the range of 9-56 pg and 5-38 ng/g, respectively. A two-level full factorial experimental design was used for screening of conditions with the highest impact on the extraction. The extraction procedure was automated and suitable for a large number of samples. The extraction recoveries ranged from 70 to 102 % and the matrix effects were between 92 and 104 %. The overall method was demonstrated on wood smoke particles and soil samples with good analytical performance, and five OH-PAHs were determined in the concentration range of 0.19-210 mu g/g. As far as we know, hydroxylated polycyclic aromatic hydrocarbons were determined in wood smoke and soil samples using photoionization mass spectrometry for the first time in this present study. Accordingly, this study shows that high performance liquid chromatography photoionization tandem mass spectrometry can be a good option for the determination of hydroxylated polycyclic aromatic hydrocarbons in complex environmental samples.

Nyckelord
HPLC-APPI-MS/MS, Photoionization, Hydroxylated PAHs, OH-PAHs, Wood smoke, Soil
Nationell ämneskategori
Biologiska vetenskaper Kemi
Forskningsämne
analytisk kemi
Identifikatorer
urn:nbn:se:su:diva-118521 (URN)10.1007/s00216-015-8638-x (DOI)000355152500003 ()
Tillgänglig från: 2015-06-23 Skapad: 2015-06-22 Senast uppdaterad: 2017-12-04Bibliografiskt granskad
2. Particulate hydroxy-PAH emissions from a residential wood log stove using different fuels and burning conditions
Öppna denna publikation i ny flik eller fönster >>Particulate hydroxy-PAH emissions from a residential wood log stove using different fuels and burning conditions
Visa övriga...
2016 (Engelska)Ingår i: Atmospheric Environment, ISSN 1352-2310, E-ISSN 1873-2844, Vol. 140, s. 1-9Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Hydroxylated polycyclic aromatic hydrocarbons are oxidation products of polycyclic aromatic hydrocarbons, but have not been studied as extensively as polycyclic aromatic hydrocarbons. Several studies have however shown that hydroxylated polycyclic aromatic hydrocarbons have toxic and carcinogenic properties. They have been detected in air samples in semi urban areas and combustion is assumed to be the primary source of those compounds. To better understand the formation and occurrence of particulate hydroxylated polycyclic aromatic hydrocarbons from residential wood log stove combustion, 9 hydroxylated polycyclic aromatic hydrocarbons and 2 hydroxy biphenyls were quantified in particles generated from four different types of wood logs (birch, spruce, pine, aspen) and two different combustion conditions (nominal and high burn rate). A previously developed method utilizing liquid chromatography photo ionization tandem mass spectrometry and pressurized liquid extraction was used. Polycyclic aromatic hydrocarbons were analyzed along with hydroxylated polycyclic aromatic hydrocarbons. The hydroxylated polycyclic aromatic hydrocarbon emissions varied significantly across different wood types and burning conditions; the highest emissions for nominal burn rate were from spruce and for high burn rate from pine burning. Emissions from nominal burn rate corresponded on average to 15% of the emissions from high burn rate, with average emissions of 218 mu g/MJ(fuel) and 32.5 mu g/MJ(fuel) for high burn rate and nominal burn rate, respectively. Emissions of the measured hydroxylated polycyclic aromatic hydrocarbons corresponded on average to 28% of polycyclic aromatic hydrocarbons emissions. This study shows that wood combustion is a large emission source of hydroxylated polycyclic aromatic hydrocarbons and that not only combustion conditions, but also wood type influences the emissions of hydroxylated polycyclic aromatic hydrocarbons and polycyclic aromatic hydrocarbons. There are few studies that have determined hydroxylated polycyclic aromatic hydrocarbons in emissions from wood combustion, and it is therefore necessary to further investigate the formation, occurrence and distribution of these compounds as they are present in significant amounts in wood smoke particles.

Nyckelord
OH-PAHs, Hydroxy-PAHs, PAHs, Wood combustion, Wood burning, Wood log stove
Nationell ämneskategori
Geovetenskap och miljövetenskap Kemi
Forskningsämne
analytisk kemi
Identifikatorer
urn:nbn:se:su:diva-133368 (URN)10.1016/j.atmosenv.2016.05.041 (DOI)000380083200001 ()
Tillgänglig från: 2016-09-12 Skapad: 2016-09-06 Senast uppdaterad: 2017-11-21Bibliografiskt granskad
3. Suspect screening of OH-PAHs and non-target screening of other organic compounds in wood smoke particles using HR-Orbitrap-MS
Öppna denna publikation i ny flik eller fönster >>Suspect screening of OH-PAHs and non-target screening of other organic compounds in wood smoke particles using HR-Orbitrap-MS
2016 (Engelska)Ingår i: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 163, s. 313-321Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Wood combustion has been shown to contribute significantly to emissions of polycyclic aromatic hydrocarbons and hydroxylated polycyclic aromatic hydrocarbons, compounds with toxic and carcinogenic properties. However, only a small number of hydroxylated polycyclic aromatic hydrocarbons have been determined in particles from wood combustion, usually compounds with available reference standards. In this present study, suspect and non-target screening strategies were applied to characterize the wood smoke particles from four different wood types and two combustion conditions with respect to hydroxylated polycyclic aromatic hydrocarbons and other organic compounds. In the suspect screening, 32 peaks corresponding to 12 monohydroxylated masses were tentatively identified by elemental composition assignments and matching of isotopic pattern and fragments. More than one structure was suggested for most of the measured masses. Statistical analysis was performed on the non-target screening data in order to single out significant peaks having intensities that depend on the wood type and/or combustion condition. Significant peaks were found in both negative and positive ionization modes, with unique peaks for each wood type and combustion condition, as well as a combination of both factors. Furthermore, structural elucidation of some peaks was done by comparing the spectra in the samples with spectra found in the spectral databases. Six compounds were tentatively identified in positive ionization mode, and 19 in negative ionization mode. The results in this present study demonstrate that there are significant overall differences in the chemistry of wood smoke particles that depends on both the wood type and the combustion condition used.

Nyckelord
OH-PAHs, Wood smoke particles, Suspect screening, Non-target screening, Orbitrap, TracMass 2
Nationell ämneskategori
Geovetenskap och miljövetenskap Kemi
Forskningsämne
analytisk kemi
Identifikatorer
urn:nbn:se:su:diva-135213 (URN)10.1016/j.chemosphere.2016.08.039 (DOI)000384776800036 ()27544654 (PubMedID)
Tillgänglig från: 2016-11-15 Skapad: 2016-11-01 Senast uppdaterad: 2017-11-29Bibliografiskt granskad
4. Target and suspect screening of OH-PAHs in air particulate using liquid chromatography- orbitrap high resolution mass spectrometry
Öppna denna publikation i ny flik eller fönster >>Target and suspect screening of OH-PAHs in air particulate using liquid chromatography- orbitrap high resolution mass spectrometry
(Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
Nyckelord
OH-PAHs, air particulate, suspect screening, high resolution mass spectrometry, orbitrap, particles
Nationell ämneskategori
Kemi
Forskningsämne
analytisk kemi
Identifikatorer
urn:nbn:se:su:diva-137209 (URN)
Tillgänglig från: 2016-12-30 Skapad: 2016-12-30 Senast uppdaterad: 2017-01-16Bibliografiskt granskad

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