| 1. |
- Yttri, K. E., et al.
(författare)
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An intercomparison study of analytical methods used for quantification of levoglucosan in ambient aerosol filter samples
- 2015
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Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 8:1, s. 125-147
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Tidskriftsartikel (refereegranskat)abstract
- The monosaccharide anhydrides (MAs) levoglucosan, galactosan and mannosan are products of incomplete combustion and pyrolysis of cellulose and hemicelluloses, and are found to be major constituents of biomass burning (BB) aerosol particles. Hence, ambient aerosol particle concentrations of levoglucosan are commonly used to study the influence of residential wood burning, agricultural waste burning and wildfire emissions on ambient air quality. A European-wide intercomparison on the analysis of the three monosaccharide anhydrides was conducted based on ambient aerosol quartz fiber filter samples collected at a Norwegian urban background site during winter. Thus, the samples' content of MAs is representative for BB particles originating from residential wood burning. The purpose of the intercomparison was to examine the comparability of the great diversity of analytical methods used for analysis of levoglucosan, mannosan and galactosan in ambient aerosol filter samples. Thirteen laboratories participated, of which three applied high-performance anion-exchange chromatography (HPAEC), four used high-performance liquid chromatography (HPLC) or ultra-performance liquid chromatography (UPLC) and six resorted to gas chromatography (GC). The analytical methods used were of such diversity that they should be considered as thirteen different analytical methods. All of the thirteen laboratories reported levels of levoglucosan, whereas nine reported data for mannosan and/or galactosan. Eight of the thirteen laboratories reported levels for all three isomers. The accuracy for levoglucosan, presented as the mean percentage error (PE) for each participating laboratory, varied from -63 to 20 %; however, for 62% of the laboratories the mean PE was within +/- 10 %, and for 85% the mean PE was within +/- 20 %. For mannosan, the corresponding range was 60 to 69 %, but as for levoglucosan, the range was substantially smaller for a subselection of the laboratories; i.e. for 33% of the laboratories the mean PE was within +/- 10 %. For galactosan, the mean PE for the participating laboratories ranged from 84 to 593 %, and as for mannosan 33% of the laboratories reported a mean PE within +/- 10 %. The variability of the various analytical methods, as defined by their minimum and maximum PE value, was typically better for levoglucosan than for mannosan and galactosan, ranging from 3.2 to 41% for levoglucosan, from 10 to 67% for mannosan and from 6 to 364% for galactosan. For the levoglucosan to mannosan ratio, which may be used to assess the relative importance of softwood versus hardwood burning, the variability only ranged from 3.5 to 24 %. To our knowledge, this is the first major intercomparison on analytical methods used to quantify monosaccharide anhydrides in ambient aerosol filter samples conducted and reported in the scientific literature. The results show that for levoglucosan the accuracy is only slightly lower than that reported for analysis of SO42- (sulfate) on filter samples, a constituent that has been analysed by numerous laboratories for several decades, typically by ion chromatography and which is considered a fairly easy constituent to measure. Hence, the results obtained for levoglucosan with respect to accuracy are encouraging and suggest that levels of levoglucosan, and to a lesser extent mannosan and galactosan, obtained by most of the analytical methods currently used to quantify monosaccharide anhydrides in ambient aerosol filter samples, are comparable. Finally, the various analytical methods used in the current study should be tested for other aerosol matrices and concentrations as well, the most obvious being summertime aerosol samples affected by wildfires and/or agricultural fires.
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| 2. |
- Tomasi, C., et al.
(författare)
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Aerosols in polar regions : A historical overview based on optical depth and in situ observations
- 2007
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Ingår i: Journal of Geophysical Research. - 0148-0227 .- 2156-2202. ; 112:D16, s. D16205-
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Forskningsöversikt (refereegranskat)abstract
- Large sets of filtered actinometer, filtered pyrheliometer and Sun photometer measurements have been carried out over the past 30 years by various groups at different Arctic and Antarctic sites and for different time periods. They were examined to estimate ensemble average, long-term trends of the summer background aerosol optical depth AOD(500 nm) in the polar regions ( omitting the data influenced by Arctic haze and volcanic eruptions). The trend for the Arctic was estimated to be between -1.6% and -2.0% per year over 30 years, depending on location. No significant trend was observed for Antarctica. The time patterns of AOD( 500 nm) and angstrom ngstrom's parameters a and beta measured with Sun photometers during the last 20 years at various Arctic and Antarctic sites are also presented. They give a measure of the large variations of these parameters due to El Chichon, Pinatubo, and Cerro Hudson volcanic particles, Arctic haze episodes most frequent in winter and spring, and the transport of Asian dust and boreal smokes to the Arctic region. Evidence is also shown of marked differences between the aerosol optical parameters measured at coastal and high-altitude sites in Antarctica. In situ optical and chemical composition parameters of aerosol particles measured at Arctic and Antarctic sites are also examined to achieve more complete information on the multimodal size distribution shape parameters and their radiative properties. A characterization of aerosol radiative parameters is also defined by plotting the daily mean values of a as a function of AOD( 500 nm), separately for the two polar regions, allowing the identification of different clusters related to fifteen aerosol classes, for which the spectral values of complex refractive index and single scattering albedo were evaluated.
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| 3. |
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| 4. |
- Crippa, M., et al.
(författare)
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Organic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach
- 2014
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 14:12, s. 6159-6176
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Tidskriftsartikel (refereegranskat)abstract
- Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May-June and September-October) and 2009 (February-March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.
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| 5. |
- Kiendler-Scharr, A., et al.
(författare)
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Ubiquity of organic nitrates from nighttime chemistry in the European submicron aerosol
- 2016
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Ingår i: Geophysical Research Letters. - 0094-8276. ; 43:14, s. 7735-7744
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Tidskriftsartikel (refereegranskat)abstract
- In the atmosphere nighttime removal of volatile organic compounds is initiated to a large extent by reaction with the nitrate radical (NO3) forming organic nitrates which partition between gas and particulate phase. Here we show based on particle phase measurements performed at a suburban site in the Netherlands that organic nitrates contribute substantially to particulate nitrate and organic mass. Comparisons with a chemistry transport model indicate that most of the measured particulate organic nitrates are formed by NO3 oxidation. Using aerosol composition data from three intensive observation periods at numerous measurement sites across Europe, we conclude that organic nitrates are a considerable fraction of fine particulate matter (PM1) at the continental scale. Organic nitrates represent 34% to 44% of measured submicron aerosol nitrate and are found at all urban and rural sites, implying a substantial potential of PM reduction by NOx emission control.
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| 6. |
- Mueller, T., et al.
(författare)
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Characterization and intercomparison of aerosol absorption photometers : result of two intercomparison workshops
- 2011
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Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 4:2, s. 245-268
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Tidskriftsartikel (refereegranskat)abstract
- Absorption photometers for real time application have been available since the 1980s, but the use of filter-based instruments to derive information on aerosol properties (absorption coefficient and black carbon, BC) is still a matter of debate. Several workshops have been conducted to investigate the performance of individual instruments over the intervening years. Two workshops with large sets of aerosol absorption photometers were conducted in 2005 and 2007. The data from these instruments were corrected using existing methods before further analysis. The inter-comparison shows a large variation between the responses to absorbing aerosol particles for different types of instruments. The unit to unit variability between instruments can be up to 30% for Particle Soot Absorption Photometers (PSAPs) and Aethalometers. Multi Angle Absorption Photometers (MAAPs) showed a variability of less than 5%. Reasons for the high variability were identified to be variations in sample flow and spot size. It was observed that different flow rates influence system performance with respect to response to absorption and instrumental noise. Measurements with non absorbing particles showed that the current corrections of a cross sensitivity to particle scattering are not sufficient. Remaining cross sensitivities were found to be a function of the total particle load on the filter. The large variation between the response to absorbing aerosol particles for different types of instruments indicates that current correction functions for absorption photometers are not adequate.
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| 7. |
- Hussein, T., et al.
(författare)
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Evaluation and modeling of the size fractionated aerosol particle number concentration measurements nearby a major road in Helsinki - Part II : Aerosol measurements within the SAPPHIRE project
- 2007
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 7:15, s. 4081-4094
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Tidskriftsartikel (refereegranskat)abstract
- This study presents an evaluation and modeling exercise of the size fractionated aerosol particle number concentrations measured nearby a major road in Helsinki during 23 August-19 September 2003 and 14 January-11 February 2004. The available information also included electronic traffic counts, on-site meteorological measurements, and urban background particle number size distribution measurement. The ultrafine particle (UFP, diameter < 100 nm) number concentrations at the roadside site were approximately an order of magnitude higher than those at the urban background site during daytime and downwind conditions. Both the modal structure analysis of the particle number size distributions and the statistical correlation between the traffic density and the UFP number concentrations indicate that the UFP were evidently from traffic related emissions. The modeling exercise included the evolution of the particle number size distribution nearby the road during downwind conditions. The model simulation results revealed that the evaluation of the emission factors of aerosol particles might not be valid for the same site during different time.
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| 8. |
- Paglione, M., et al.
(författare)
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Primary and secondary biomass burning aerosols determined by proton nuclear magnetic resonance (H-1-NMR) spectroscopy during the 2008 EUCAARI campaign in the Po Valley (Italy)
- 2014
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 14:10, s. 5089-5110
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric organic aerosols are generally classified as primary and secondary (POA and SOA) according to their formation processes. An actual separation, however, is challenging when the timescales of emission and gas-to-particle formation overlap. The presence of SOA formation in biomass burning plumes leads to scientific questions about whether the oxidized fraction of biomass burning aerosol is rather of secondary or primary origin, as some studies would suggest, and about the chemical compositions of oxidized biomass burning POA and SOA. In this study, we apply nuclear magnetic resonance (NMR) spectroscopy to investigate the functional group composition of fresh and aged biomass burning aerosols during an intensive field campaign in the Po Valley, Italy. The campaign was part of the EUCAARI project and was held at the rural station of San Pietro Capofiume in spring 2008. Factor analysis applied to the set of NMR spectra was used to apportion the wood burning contribution and other organic carbon (OC) source contributions, including aliphatic amines. Our NMR results, referred to the polar, water-soluble fraction of OC, show that fresh wood burning particles are composed of polyols and aromatic compounds, with a sharp resemblance to wood burning POA produced in wood stoves, while aged samples are clearly depleted of alcohols and are enriched in aliphatic acids with a smaller contribution of aromatic compounds. The comparison with biomass burning organic aerosols (BBOA) determined by high-resolution aerosol mass spectrometry (HR-TOF-AMS) at the site shows only a partial overlap between NMR BB-POA and AMS BBOA, which can be explained by either the inability of BBOA to capture all BB-POA composition, especially the alcohol fraction, or the fact that BBOA account for insoluble organic compounds unmeasured by the NMR. Therefore, an unambiguous composition for biomass burning POA could not be derived from this study, with NMR analysis indicating a higher O / C ratio compared to that measured for AMS BBOA. The comparison between the two techniques substantially improves when adding factors tracing possible contributions from biomass burning SOA, showing that the operational definitions of biomass burning organic aerosols are more consistent between techniques when including more factors tracing chemical classes over a range of oxidation levels. Overall, the non-fossil total carbon fraction was 50-57%, depending on the assumptions about the C-14 content of non-fossil carbon, and the fraction of organic carbon estimated to be oxidized organic aerosol (OOA) from HR-TOF-AMS measurements was 73-100% modern.
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| 9. |
- Timonen, Hilkka, et al.
(författare)
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Influence of fuel ethanol content on primary emissions and secondary aerosol formation potential for a modern flex-fuel gasoline vehicle
- 2017
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:8, s. 5311-5329
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Tidskriftsartikel (refereegranskat)abstract
- The effect of fuel ethanol content (10, 85 and 100 %) on primary emissions and on subsequent secondary aerosol formation was investigated for a Euro 5 flex-fuel gasoline vehicle. Emissions were characterized during a New European Driving Cycle (NEDC) using a comprehensive setup of high time-resolution instruments. A detailed chemical composition of the exhaust particulate matter (PM) was studied using a soot particle aerosol mass spectrometer (SPAMS), and secondary aerosol formation was studied using a potential aerosol mass (PAM) chamber. For the primary gaseous compounds, an increase in total hydrocarbon emissions and a decrease in aromatic BTEX (benzene, toluene, ethylbenzene and xylenes) compounds was observed when the amount of ethanol in the fuel increased. In regard to particles, the largest primary particulate matter concentrations and potential for secondary particle formation was measured for the E10 fuel (10% ethanol). As the ethanol content of the fuel increased, a significant decrease in the average primary particulate matter concentrations over the NEDC was found. The PM emissions were 0.45, 0.25 and 0.15 mgm-3 for E10, E85 and E100, respectively. Similarly, a clear decrease in secondary aerosol formation potential was observed with a larger contribution of ethanol in the fuel. The secondary-toprimary PM ratios were 13.4 and 1.5 for E10 and E85, respectively. For E100, a slight decrease in PM mass was observed after the PAM chamber, indicating that the PM produced by secondary aerosol formation was less than the PM lost through wall losses or the degradation of the primary organic aerosol (POA) in the chamber. For all fuel blends, the formed secondary aerosol consisted mostly of organic compounds. For E10, the contribution of organic compounds containing oxygen increased from 35 %, measured for primary organics, to 62% after the PAM chamber. For E85, the contribution of organic compounds containing oxygen increased from 42% (primary) to 57% (after the PAM chamber), whereas for E100 the amount of oxidized organics remained the same (approximately 62 %) with the PAM chamber when compared to the primary emissions.
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| 10. |
- Yttri, K. E., et al.
(författare)
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Source apportionment of the summer time carbonaceous aerosol at Nordic rural background sites
- 2011
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:24, s. 13339-13357
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Tidskriftsartikel (refereegranskat)abstract
- In the present study, natural and anthropogenic sources of particulate organic carbon (OCp) and elemental carbon (EC) have been quantified based on weekly filter samples of PM10 (particles with aerodynamic diameter
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