Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements

Lambe, Andrew T.; Ahern, Adam; Williams, Leah R.; Slowik, Jay G.; Wong, J. P. S.; Abbatt, Jonathan P. D.; Brune, William H.; Ng, N. L.; Wright, Justin P.; Croasdale, D. R.; Worsnop, Douglas R.; Davidovits, P.; Onasch, T. B.

doi:10.5194/amt-4-445-2011

Cited by 307 publications

(455 citation statements)

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“…These extreme PM concentrations mean that diffusional losses to the particulate surface area (condensation sink; CS) are normally much higher than similar losses to the chamber-wall surface area during aerosol oxidation. Condensing gases are much more likely to condense onto aerosol particles than onto the walls, in contrast to smog chambers (Zhang et al 2014), and larger WOOD-STOVE OM COMPOSITION flow reactors operated with lower PM concentrations (Lambe et al 2011). Figure 2 illustrates this relationship between CS and wall (diffusional) losses for the MSC in terms of the lifetimes against 50% loss, t CS , and t wall .…”

Section: Msc Wall Lossesmentioning

confidence: 99%

Organic Emissions from a Wood Stove and a Pellet Stove Before and After Simulated Atmospheric Aging

Corbin

Keller

Lohmann

et al. 2015

Aerosol Science and Technology

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Logwood and pellet stoves are popular heating sources around the world. The particulate matter emitted from such stoves contains organic particulate matter (OM), soot, and ash, each of which may have significant effects on climate and health. In this study, the primary OM (POM) emitted from a wood stove and a pellet stove operated according to standard Swiss testing protocols were characterized using aerosol mass spectrometry. The POM mass spectra were found to be highly reproducible, and contained CO C as the dominant ion. Because the POM emitted by such stoves is typically enhanced by the condensation of gaseous organics following atmospheric aging, the secondary OM (SOM) formation potential of these stoves was simulated using the Micro Smog Chamber (MSC) designed by Keller and Burtscher in 2012. In general, OM emission factors from MSCaged aerosols were comparable to lower-time-resolution results from the literature, although the MSC exposed aerosols to much higher concentrations of oxidants and therefore produced OM that was more oxidized than expected for atmospheric samples. In addition, the logwood-stove particles remained highly aspherical even after oxidation, indicating that mixing with an external aerosol is required for these particles to become spherical. The one exception to this observation occurred when the wood failed to ignite and appeared to generate tar-ball OM particles.

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Section: Msc Wall Lossesmentioning

confidence: 99%

Organic Emissions from a Wood Stove and a Pellet Stove Before and After Simulated Atmospheric Aging

Corbin

Keller

Lohmann

et al. 2015

Aerosol Science and Technology

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“…3-MBTCA, a second generation oxidation product of α-pinene, was synthesized as described by Dette et al (2014). The α-pinene SOA samples investigated in this study were generated with a Potential Aerosol Mass (PAM) flow tube reactor as described in detail by Lambe et al (2011) from the gas phase oxidation of α-pinene with OH radicals and collected onto 47 mm teflon filters. To collect sufficient sample mass (4-5 mg) for the offline analysis, steady-state SOA mass concentrations of approximately 300-400 µg m −3 were produced in the reactor and collected at 8.5 L min −1 for 24 h. In order to prepare injection into the EDB, the material was extracted from the filter with methanol which was subsequently evaporated in N 2 gas.…”

Section: Methodsmentioning

confidence: 99%

Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?

Lienhard

Huisman

Krieger³

et al. 2015

Atmos. Chem. Phys.

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117

189

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Abstract. New measurements of water diffusion in secondary organic aerosol (SOA) material produced by oxidation of α-pinene and in a number of organic/inorganic model mixtures (3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA), levoglucosan, levoglucosan/NH 4 HSO 4 , raffinose) are presented. These indicate that water diffusion coefficients are determined by several properties of the aerosol substance and cannot be inferred from the glass transition temperature or bouncing properties. Our results suggest that water diffusion in SOA particles is faster than often assumed and imposes no significant kinetic limitation on water uptake and release at temperatures above 220 K. The fast diffusion of water suggests that heterogeneous ice nucleation on a glassy core is very unlikely in these systems. At temperatures below 220 K, model simulations of SOA particles suggest that heterogeneous ice nucleation may occur in the immersion mode on glassy cores which remain embedded in a liquid shell when experiencing fast updraft velocities. The particles absorb significant quantities of water during these updrafts which plasticize their outer layers such that these layers equilibrate readily with the gas phase humidity before the homogeneous ice nucleation threshold is reached. Glass formation is thus unlikely to restrict homogeneous ice nucleation. Only under most extreme conditions near the very high tropical tropopause may the homogeneous ice nucleation rate coefficient be reduced as a consequence of slow condensed-phase water diffusion. Since the differences between the behavior limited or non limited by diffusion are small even at the very high tropical tropopause, condensed-phase water diffusivity is unlikely to have significant consequences on the direct climatic effects of SOA particles under tropospheric conditions.

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“…The oxidation of precursor gas, nucleation, and gas-particle partitioning, which took hours in the atmosphere, was shortened to a few minutes in the PAM reactor. The PAM reactor was used to simulate the formation and aging of aerosols (Chen et al, 2013;Kang et al, 2011;Lambe et al, 2011Lambe et al, , 2012, to evaluate of the secondary organic aerosol (SOA) formation potential of source emissions (Keller and Burtscher, 2012;Ortega et al, 2013), and to quantify secondary aerosol production in situ (Farmer and Jimenez, 2010). The PAM results, including particle chemical composition and size distributions, were comparable to those observed in environmental chambers, which have been widely used to simulate secondary aerosol formation (Kang et al, 2007).…”

Section: Introductionmentioning

confidence: 56%

Distinct potential aerosol masses under different scenarios of transport at a suburban site of Beijing

Chu

et al. 2016

Journal of Environmental Sciences

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In order to evaluate the secondary aerosol formation potential at a suburban site of Beijing, in situ perturbation experiments in a potential aerosol mass (PAM) reactor were carried out in the winter of 2014. The variations of secondary aerosol formation as a function of time, OH exposure, and the concentrations of gas phase pollutants and particles were reported in this study. Two periods with distinct secondary aerosol formation potentials, marked as Period I and Period II, were identified during the observation. In Period I, the secondary aerosol formation potential was high, and correlated well to the air pollutants, i.e., SO 2 , NO 2 , and CO. The maximal secondary aerosol formation was observed with an aging time equivalent to about 3 days of atmospheric oxidation. In period II, the secondary aerosol formation potential was low, with no obvious correlation with the air pollutants. Meanwhile, the aerosol mass decreased, instead of showing a peak, with increasing aging time.Backward trajectory analysis during the two periods confirmed that the air mass in Period I was mainly from local sources, while it was attributed mostly to long distance transport in Period II. The air lost its reactivity during the long transport and the particles became highly aged, resulting in a low secondary aerosol formation potential. Our experimental results indicated that the in situ measurement of the secondary aerosol formation potential could provide important information for evaluating the contributions of local emission and long distance transport to the aerosol pollution.

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Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements

Cited by 307 publications

References 50 publications

Organic Emissions from a Wood Stove and a Pellet Stove Before and After Simulated Atmospheric Aging

Organic Emissions from a Wood Stove and a Pellet Stove Before and After Simulated Atmospheric Aging

Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?

Distinct potential aerosol masses under different scenarios of transport at a suburban site of Beijing

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