Measurement of the ambient organic aerosol volatility distribution: application during the Finokalia Aerosol Measurement Experiment (FAME-2008)

Lee, B. H.; Kostenidou, Evangelia; Hildebrandt, L.; Riipinen, Ilona; Engelhart, G. J.; Mohr, Claudia; DeCarlo, P. F.; Mihalopoulos, N.; Prévôt, Andrê S. H.; Baltensperger, Urs; Pandis, Spyros Ν.

doi:10.5194/acp-10-12149-2010

Cited by 84 publications

(92 citation statements)

References 41 publications

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“…To measure the number particle size distribution in this size range, scanning mobility particle sizers (SMPS) have been used after the TD (Wehner et al, 2004;Kim et al, 2010;Saleh et al, 2012). For the determination of the chemical composition of these particles, aerosol mass spectrometers (AMSs) have been increasingly applied (Lee et al, 2010;Poulain et al, 2010;Cappa and Jimenez, 2010).…”

Section: G I Gkatzelis Et Al: Measurement Of Nonvolatile Particle mentioning

confidence: 99%

Measurement of nonvolatile particle number size distribution

et al. 2016

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Abstract. An experimental methodology was developed to measure the nonvolatile particle number concentration using a thermodenuder (TD). The TD was coupled with a highresolution time-of-flight aerosol mass spectrometer, measuring the chemical composition and mass size distribution of the submicrometer aerosol and a scanning mobility particle sizer (SMPS) that provided the number size distribution of the aerosol in the range from 10 to 500 nm. The method was evaluated with a set of smog chamber experiments and achieved almost complete evaporation (> 98 %) of secondary organic as well as freshly nucleated particles, using a TD temperature of 400 • C and a centerline residence time of 15 s.This experimental approach was applied in a winter field campaign in Athens and provided a direct measurement of number concentration and size distribution for particles emitted from major pollution sources. During periods in which the contribution of biomass burning sources was dominant, more than 80 % of particle number concentration remained after passing through the thermodenuder, suggesting that nearly all biomass burning particles had a nonvolatile core. These remaining particles consisted mostly of black carbon (60 % mass contribution) and organic aerosol (OA; 40 %). Organics that had not evaporated through the TD were mostly biomass burning OA (BBOA) and oxygenated OA (OOA) as determined from AMS source apportionment analysis. For periods during which traffic contribution was dominant 50-60 % of the particles had a nonvolatile core while the rest evaporated at 400 • C. The remaining particle mass consisted mostly of black carbon with an 80 % contribution, while OA was responsible for another 15-20 %. Organics were mostly hydrocarbon-like OA (HOA) and OOA. These results suggest that even at 400 • C some fraction of the OA does not evaporate from particles emitted from common combustion processes, such as biomass burning and car engines, indicating that a fraction of this type of OA is of extremely low volatility.

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Section: G I Gkatzelis Et Al: Measurement Of Nonvolatile Particle mentioning

confidence: 99%

Measurement of nonvolatile particle number size distribution

et al. 2016

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“…The methods applied here fall into two general categories: (i) heating of the polydisperse particle distribution (Huffman et al, 2008;Lee et al, 2010;Saha et al, 2017) and (ii) heating of monodisperse particles selected by the differential mobility analyzer (DMA-selected; volatility tandem DMA approach, V-TDMA; Biswas et al, 2007;Kuhn et al, 2005;Tiitta et al, 2010). A custom-built, multi-tube thermodenuder (MT-TD) system was used for high-time-resolution volatility measurements.…”

Section: Thermodenuder (Td) Experimentsmentioning

confidence: 99%

Downwind evolution of the volatility and mixing state of near-road aerosols near a US interstate highway

2018

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Abstract. We present spatial measurements of particle volatility and mixing state at a site near a North Carolina interstate highway (I-40) applying several heating (thermodenuder; TD) experimental approaches. Measurements were conducted in summer 2015 and winter 2016 in a roadside trailer (10 m from road edge) and during downwind transects at different distances from the highway under favorable wind conditions using a mobile platform. Results show that the relative abundance of semi-volatile species (SVOCs) in ultrafine particles decreases with downwind distance, which is consistent with the dilution and mixing of traffic-sourced particles with background air and evaporation of semi-volatile species during downwind transport. An evaporation kinetics model was used to derive particle volatility distributions by fitting TD data. While the TD-derived distribution apportions about 20–30 % of particle mass as semi-volatile (SVOCs; effective saturation concentration, C∗ ≥ 1µm−3) at 10 m from the road edge, approximately 10 % of particle mass is attributed to SVOCs at 220 m, showing that the particle-phase semi-volatile fraction decreases with downwind distance. The relative abundance of semi-volatile material in the particle phase increased during winter. Downwind spatial gradients of the less volatile particle fraction (that remaining after heating at 180 °C) were strongly correlated with black carbon (BC). BC size distribution and mixing state measured using a single-particle soot photometer (SP2) at the roadside trailer showed that a large fraction (70–80 %) of BC particles were externally mixed. Heating experiments with a volatility tandem differential mobility analyzer (V-TDMA) also showed that the nonvolatile fraction in roadside aerosols is mostly externally mixed. V-TDMA measurements at different distances downwind from the highway indicate that the mixing state of roadside aerosols does not change significantly (e.g., BC mostly remains externally mixed) within a few hundred meters from the highway. Our analysis indicates that a superposition of volatility distributions measured in laboratory vehicle tests and of background aerosol can be used to represent the observed partitioning of near-road particles. The results from this study show that exposures and impacts of BC and semi-volatile organics-containing particles in a roadside microenvironment may differ across seasons and under changing ambient conditions.

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“…Figure 9 compares model-predicted OA volatility to measurements from three different field campaigns: (a) FAME campaign in May-June 2008(FAME-2008 The OA volatility was measured using thermodenuders and is represented as a thermogram, which is a plot of the OA mass fraction remaining as a function of temperature. The measured thermograms have been corrected for non-equilibrium effects in the thermodenuder using the work of Lee et al (2010) for FAME-2008 and the work of Cappa and Jimenez (2010) for MILAGRO-2006. For SOAR-2005, the thermogram has not been corrected for non-equlibrium conditions in the thermodenuder.…”

Section: Oxygenated Organic Aerosolmentioning

confidence: 99%

The influence of semi-volatile and reactive primary emissions on the abundance and properties of global organic aerosol

et al. 2011

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Abstract.Semi-volatile and reactive primary organic aerosols are modeled on a global scale using the GISS GCM II' "unified" climate model. We employ the volatility basis set framework to simulate emissions, chemical reactions and phase partitioning of primary and secondary organic aerosol (POA and SOA). The model also incorporates the emissions and reactions of intermediate volatility organic compounds (IVOCs) as a source of organic aerosol (OA), one that has been missing in most prior work. Model predictions are evaluated against a broad set of observational constraints including mass concentrations, degree of oxygenation, volatility and isotopic composition. A traditional model that treats POA as non-volatile and non-reactive is also compared to the same set of observations to highlight the progress made in this effort. The revised model predicts a global dominance of SOA and brings the POA/SOA split into better agreement with ambient measurements. This change is due to traditionally defined POA evaporating and the evaporated vapors oxidizing to form non-traditional SOA. IVOCs (traditionally not included in chemical transport models) oxidize to form condensable products that account for a third of total OA, suggesting that global models have been missing a large source of OA. Predictions of the revised model for the SOA fraction at 17 different locations compared much better to observations than predictions from the traditional model. Modelpredicted volatility is compared with thermodenuder data collected at three different different field campaigns: FAME-2008, MILAGRO-2006 and SOAR-2005. The revised model predicts the OA volatility much more closely than the traditional model. When compared against monthly averaged OA Correspondence to: P. J. Adams (peter.adams@cmu.edu) mass concentrations measured by the IMPROVE network, predictions of the revised model lie within a factor of two in summer and mostly within a factor of five during winter. A sensitivity analysis indicates that the winter comparison can be improved either by increasing POA emissions or lowering the volatility of those emissions. Model predictions of the isotopic composition of OA are compared against those computed via a radiocarbon isotope analysis of field samples. The contemporary fraction, on average, is slightly under-predicted (20 %) during the summer months but is a factor of two lower during the winter months. We hypothesize that the large wintertime under-prediction of surface OA mass concentrations and the contemporary fraction is due to an under-representation of biofuel (particularly, residential wood burning) emissions in the emissions inventory. Overall, the model evaluation highlights the importance of treating POA as semi-volatile and reactive in order to predict accurately the sources, composition and properties of ambient OA.

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Measurement of the ambient organic aerosol volatility distribution: application during the Finokalia Aerosol Measurement Experiment (FAME-2008)

Cited by 84 publications

References 41 publications

Measurement of nonvolatile particle number size distribution

Measurement of nonvolatile particle number size distribution

Downwind evolution of the volatility and mixing state of near-road aerosols near a US interstate highway

The influence of semi-volatile and reactive primary emissions on the abundance and properties of global organic aerosol

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