Journal of Aerosol Science

2007

DOI: 10.1016/j.jaerosci.2006.12.002

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Aerosol volatility measurement using an improved thermodenuder: Application to secondary organic aerosol

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,

Ravi Kant Pathak

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,

Byong-Hyoek Lee

³

et al.

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Thermodenuder Description2

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Cited by 209 publications

(194 citation statements)

References 23 publications

(33 reference statements)

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“…Nonvolatile particle number concentration and size distribution were measured using a TD operating at 400 • C. The TD is based on the design of An et al (2007), providing high residence times for the aerosol. The TD maximum temperature was set at 400 • C. The TD setup was coupled with a HRToF-AMS, measuring the chemical composition and mass size distribution of the PM 1 aerosol and a SMPS that provided the number size distribution of the aerosol in the range from 10 to 500 nm.…”

Section: Discussionmentioning

confidence: 99%

“…The TD setup used in this study was based on the design of An et al (2007). A detailed schematic of the TD apparatus is shown in Fig.…”

Section: Thermodenuder Descriptionmentioning

confidence: 99%

See 1 more Smart Citation

Measurement of nonvolatile particle number size distribution

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et al. 2016

Atmos. Meas. Tech.

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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.

“…Nonvolatile particle number concentration and size distribution were measured using a TD operating at 400 • C. The TD is based on the design of An et al (2007), providing high residence times for the aerosol. The TD maximum temperature was set at 400 • C. The TD setup was coupled with a HRToF-AMS, measuring the chemical composition and mass size distribution of the PM 1 aerosol and a SMPS that provided the number size distribution of the aerosol in the range from 10 to 500 nm.…”

Section: Discussionmentioning

confidence: 99%

“…The TD setup used in this study was based on the design of An et al (2007). A detailed schematic of the TD apparatus is shown in Fig.…”

Section: Thermodenuder Descriptionmentioning

confidence: 99%

Measurement of nonvolatile particle number size distribution

¹

,

²

,

³

et al. 2016

Atmos. Meas. Tech.

View full text Add to dashboard Cite

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.

“…This "chamber" SOA is modestly oxidized, with an oxygen to carbon ratio ðO∶CÞ < 0.4 (7). It is unambiguously semivolatile: Yields rise with increasing SOA mass loading (8,9) and decreasing temperature (10), and the SOA evaporates upon heating (11)(12)(13) and after isothermal dilution (14).…”

mentioning

confidence: 99%

Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions

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et al. 2012

Proc. Natl. Acad. Sci. U.S.A.

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The Multiple Chamber Aerosol Chemical Aging Study (MUCHA-CHAS) tested the hypothesis that hydroxyl radical (OH) aging significantly increases the concentration of first-generation biogenic secondary organic aerosol (SOA). OH is the dominant atmospheric oxidant, and MUCHACHAS employed environmental chambers of very different designs, using multiple OH sources to explore a range of chemical conditions and potential sources of systematic error. We isolated the effect of OH aging, confirming our hypothesis while observing corresponding changes in SOA properties. The mass increases are consistent with an existing gap between global SOA sources and those predicted in models, and can be described by a mechanism suitable for implementation in those models.atmospheric chemistry | biosphere-atmosphere interactions O rganic aerosol (OA) comprises a large fraction of fine-particle mass (PM 2.5 ) (1). In the developed world, 1-2% of deaths are blamed on inhalation of PM 2.5 (2), and the leading uncertainty in climate forcing is the interplay between the number of fine particles large enough to nucleate cloud droplets and the amount of sunlight reflected by those clouds (3). Oxidation and condensation of organics play a major but uncertain role in both phenomena.Traditional models treat most OA as nonvolatile primary OA (POA), augmented by secondary OA (SOA) (4), and they underpredict OA concentrations by a factor of 3-10 (5). α-Pinene is a major biogenic SOA source, sometimes used to represent all SOA in global models (4, 6). However, less than 20% of the carbon from fresh α-pinene oxidation condenses in chambers at room temperature; (7) the remainder is gaseous (Fig. 1A). This "chamber" SOA is modestly oxidized, with an oxygen to carbon ratio ðO∶CÞ < 0.4 (7). It is unambiguously semivolatile: Yields rise with increasing SOA mass loading (8, 9) and decreasing temperature (10), and the SOA evaporates upon heating (11-13) and after isothermal dilution (14).In contrast, ambient OA is highly oxidized (0.5 ≤ O∶C ≤ 1.0) (1, 15) and not very volatile (16). Ambient SOA is much less volatile than ambient POA (16). Consequently, "chamber" SOA does not represent the atmosphere. Our hypothesis is that homogeneous gas-phase aging by OH is a major missing process connecting chamber studies to the atmosphere. Considerable attention has been paid to heterogeneous uptake of oxidants to particles (17, 18), and recently gas-phase oxidation of semivolatile primary emissions (19), but the degree to which gas-phase oxidation can age chamber SOA is uncertain (1,4,18,20).OA resides in the atmosphere for about one week (21), while the gas-phase lifetimes of major semivolatile SOA constituents are far shorter. Typical α-pinene products pinonaldehyde, cispinonic acid, and pinic acid all have lifetimes of only a few hours for summertime conditions (22). Without question, oxidation of semivolatile SOA vapors will perturb the equilibrium phase partitioning of these constituents. Because almost all of the first-generation products are less volatile than α...

“…• C (Clarke 1991;Burtscher et al 2001;An et al 2007). As diffusional and thermophoretic effects are dependent on particle size, aerosol were size-selected using a differential mobility analyzer (DMA; Model 3081, TSI) then split to a concentration particle counter (CPC; Model 3010, TSI) and the thermodenuder.…”

Section: Thermodenuder Characterizationmentioning

confidence: 99%

Toward the Determination of Joint Volatility-Hygroscopicity Distributions: Development and Response Characterization for Single-Component Aerosol

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et al. 2014

Aerosol Science and Technology

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This work presents the development and characterization of a thermodenuder for the study and interpretation of aerosol volatility. Thermodenuder measurements are further combined with a continuous-flow streamwise thermal gradient CCN counter to obtain the corresponding aerosol hygroscopicity. The thermodenuder response function is characterized with monodisperse aerosol of variable volatility and hygroscopicity. The measurements are then interpreted with a comprehensive instrument model embedded within an optimization framework to retrieve aerosol properties with constrained uncertainty. Special attention is given to the interpretation of the size distribution of the thermodenuded aerosol, deconvoluting the effects of impurities and multiple charging, and to simplifications on the treatment of thermodenuder geometry, temperature, the cooling section, and the effects of curvature and accommodation coefficient on inferred particle volatility. Retrieved vapor pressures are consistent with published literature and shown to be most sensitive to uncertainty in the accommodation coefficient.

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