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Determination of highly carcinogenic dibenzopyrene isomers in particulate emissions from two diesel- and two gasoline-fuelled light-duty vehicles
Stockholm University, Faculty of Science, Department of Analytical Chemistry.
Stockholm University, Faculty of Science, Department of Analytical Chemistry.
2009 (English)In: Atmospheric Environment, ISSN 1352-2310, Vol. 43, no 25, 3883-3890 p.Article in journal (Refereed) Published
Abstract [en]

Emission factors of particulate-bound Polycyclic Aromatic Hydrocarbons (PAHs) including benzo(a)pyrene and, for the first time, the highly carcinogenic dibenzo(a,l)pyrene, dibenzo(a,e)pyrene, dibenzo(a,i)pyrene and dibenzo(a,h)pyrene have been determined in exhausts from two diesel- (DFVs) and two gasoline-fuelled light-duty vehicles (GFVs) operated in the Urban (AU), Rural Road (AR) and Motorway (AM) transient ARTEMIS driving cycles. The obtained results showed the DFVs to emit higher amounts of PAHs than the GFVs per km driving distance at low average speed in the AU driving cycle, while the GFVs emitted higher amounts of PAHs than the DFVs per km driving distance at higher average speeds in the AR and AM driving cycles. Furthermore, the study showed an increase in PAH emissions per km driving distance with increasing average speed for the GFVs with the opposite trend found for the DFVs. The GFVs generated particulate matter with higher PAH content than the DFVs in all three driving cycles tested with the highest concentrations obtained in the AR driving cycle. Dibenzo(a,l)pyrene was found to be a major contributor to the potential carcinogenicity accounting for 58–67% and 25–31% of the sum added potential carcinogenicity of the measured PAHs in the emitted particulate matter from the DFVs and GFVs, respectively. Corresponding values for benzo(a)pyrene were 16–25% and 11–40% for the DFVs and GFVs, respectively. The DFVs displayed higher sum added potential carcinogenicity of the measured PAHs than the GFVs in the AU driving cycle with the opposite trend found in the AR and AM driving cycles. The findings of this study show the importance of including the dibenzopyrenes in vehicle exhaust chemical characterizations to avoid potential underestimation of the carcinogenic activity of the emissions. The lower emissions and the lower sum added potential carcinogenicity of the measured PAHs found in this study for the GFVs compared to the DFVs in the AU driving cycle indicate the GFVs to be preferred in dense urban areas with traffic moving at low average speeds with multiple start and stops. However, the obtained results suggest the opposite to be true at higher average speeds with driving at rural roads and motorways. Further studies are, however, needed to establish if the observed differences between GFVs and DFVs are generally valid as well as to study the effects on variations in vehicle/engine type, ambient temperature, fuel and driving conditions on the emission factors.

Place, publisher, year, edition, pages
2009. Vol. 43, no 25, 3883-3890 p.
Keyword [en]
Regulated emissions, Particle emissions, Unregulated emissions, Gasoline, Diesel, Light-duty vehicles, PAH, Benzo(a)pyrene, Dibenzopyrenes, Dibenzo(a, l)pyrene, Toxic Equivalency Factor, TEF
National Category
Analytical Chemistry
Research subject
Analytical Chemistry
Identifiers
URN: urn:nbn:se:su:diva-29585DOI: 10.1016/j.atmosenv.2009.04.055ISI: 000268851600010OAI: oai:DiVA.org:su-29585DiVA: diva2:234333
Available from: 2009-09-09 Created: 2009-09-07 Last updated: 2009-09-16Bibliographically approved
In thesis
1. Methods for Determination of Benzo(a)pyrene and High Molecular Weight (>300 Da) Polycyclic Aromatic Hydrocarbons in Particulate Matter from Ambient Air and Vehicle Exhausts
Open this publication in new window or tab >>Methods for Determination of Benzo(a)pyrene and High Molecular Weight (>300 Da) Polycyclic Aromatic Hydrocarbons in Particulate Matter from Ambient Air and Vehicle Exhausts
2009 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Air pollution with particulate matter (PM) raises considerable concern because of its adverse effects on human health. For this reason, and because the mechanisms of PM toxicity are not fully known, there is an urgent need to determine the chemical constituents of atmospheric PM, especially PM emanating from traffic - a major source of urban PM.

This thesis describes analytical methods that have been developed for determining polycyclic aromatic hydrocarbons (PAHs) in ambient air and vehicle exhaust PM, focusing particularly on benzo(a)pyrene (B(a)P) and the dibenzopyrenes: dibenzo(a,l)pyrene, dibenzo(a,e)pyrene, dibenzo(a,i)pyrene and dibenzo(a,h)pyrene. Trace amounts in complex matrices have been met by coupling parts or the entire clean-up step using liquid chromatography on-line with the analysis step using gas chromatography-mass spectrometry into one automated system.

Application of the methodology, using either ultrasonic assisted extraction (USE) or accelerated solvent extraction (ASE), to a National Institute of Standards and Technology (NIST) urban air standard reference material (SRM) yielded comparable or higher concentrations than the assigned NIST values, validating the approach. However, ASE provided higher extraction yields from diesel particulate SRMs than USE, and ASE of diesel SRMs generally yielded higher concentrations than the corresponding NIST values.

Concentrations of dibenzopyrenes in Stockholm air PM, and gasoline- and diesel-fuelled vehicle emissions (ng/km), are reported for the first time. When adjusted in terms of their relative carcinogenic potencies, the dibenzopyrenes were found to pose greater carcinogenic hazards than B(a)P, indicating that the current use of B(a)P as a marker probably leads to underestimates of the carcinogenicity of PAHs in ambient air.

The developed methods also worked well for analyzing larger molecular weight PAHs: more than 60 and 170 potential PAHs were detected in ambient air PM and diesel PM, respectively.

Place, publisher, year, edition, pages
Stockholm: Department of Analytical Chemistry, Stockholm, 2009. 97 p.
Keyword
PAH, dibenzopyrene, benzo(a)pyrene, standard reference material, air particulate matter, diesel particulate matter, toxic equivalence factor, ultrasonic assisted extraction, accelerated solvent extraction, automation, online coupling, GC/MC, LC/GC/MS
National Category
Analytical Chemistry
Research subject
Analytical Chemistry
Identifiers
urn:nbn:se:su:diva-29749 (URN)978-91-7155-920-3 (ISBN)
Public defence
2009-10-16, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2009-09-24 Created: 2009-09-11 Last updated: 2009-09-22Bibliographically approved

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