Direct polymerization of isoprene and <i>α</i>‐pinene on acidic aerosols

Liggio, John; Li, Shao-Meng; Brook, Jeffrey R.; Mihele, C.

doi:10.1029/2006gl028468

Cited by 105 publications

(85 citation statements)

References 19 publications

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“…It has been shown recently that on highly acidic particles even the direct uptake of isoprene and α-pinene is possible, i.e. without any prior photooxidation step (Liggio et al, 2007), confirming the hypothesis based on previous bulk experiments (Limbeck et al, 2003).…”

Section: Introductionsupporting

confidence: 85%

Quantitative assessment of organosulfates in size-segregated rural fine aerosol

Lukács

Gelencsér²,

Hoffer

et al. 2009

Atmos. Chem. Phys.

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Abstract.Organosulfates have recently come into the focus of organic aerosol research as potentially important components of water-soluble secondary organic aerosol (SOA) which now dominate tropospheric fine aerosol. Their presence has been confirmed by the identification of sulfate esters of abundant biogenic carbonyl compounds in both smog chamber and continental aerosol. However, none of the studies have been able to determine the mass contribution of organosulfates to SOA.In this paper, as possibly the very first attempt to quantify organosulfates in ambient aerosol, we inferred the mass concentrations of organosulfates by concurrently determining mass concentrations of total sulfur, sulfate and methanesulfonate in rural fine aerosol using two highly sensitive analytical techniques. Although uncertainties were relatively large, we found that mass concentrations of organosulfates in water-soluble fine aerosol ranged from 0.02 µgS m −3 to 0.09 µgS m −3 yielding a mass contribution of 6-12% to bulk sulfur concentrations (or 6-14% to sulfate concentrations). The inferred size distribution of organosulfates suggested that they possibly form in heterogeneous reactions from semi-volatile carbonyl compounds with subsequent or concurrent condensation of gaseous sulfuric acid producing a refractory organic film on particle surfaces.

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Section: Introductionsupporting

confidence: 85%

Quantitative assessment of organosulfates in size-segregated rural fine aerosol

Lukács

Gelencsér²,

Hoffer

et al. 2009

Atmos. Chem. Phys.

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“…Edney, Kleindienst, and coworkers found similar results for isoprene photooxidation, with SOA yields greatly increased in the presence of SO 2 (which forms sulfuric acid aerosol upon oxidation) or H 2 SO 4 seed (Edney et al, 2005;Kleindienst et al, 2007b;Surratt et al, 2007b). Aerosol is also observed when high concentrations of isoprene are exposed to H 2 SO 4 seed in the absence of any oxidants (Limbeck et al, 2003;Liggio et al, 2007). These results likely arise from particle-phase reactions promoting SOA growth, in agreement with the conclusions of Jang et al (2002).…”

Section: Laboratory Measurements Of Aerosol Growth From Isoprene Oxidsupporting

confidence: 66%

A review of Secondary Organic Aerosol (SOA) formation from isoprene

2009

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Abstract. Recent field and laboratory evidence indicates that the oxidation of isoprene, (2-methyl-1,3-butadiene, C 5 H 8 ) forms secondary organic aerosol (SOA). Global biogenic emissions of isoprene (600 Tg yr −1 ) are sufficiently large that the formation of SOA in even small yields results in substantial production of atmospheric particulate matter, likely having implications for air quality and climate. Here we present a review of field measurements, experimental work, and modeling studies aimed at understanding the mechanisms, yield, and atmospheric importance of isoprene-derived SOA. SOA yields depend on a number of factors, including organic aerosol loading (M o ), NO x level (RO 2 chemistry), and, because of the importance of multigenerational chemistry, the degree of oxidation. These dependences are not always included in SOA modules used in atmospheric transport models, and instead most yield parameterizations rely on a single set of chamber experiments (carried out over a limited range of conditions); this may lead to very different estimates of the atmospheric importance of isoprene SOA. New yield parameterizations, based on all available laboratory data (M o =0-50 µg m −3 ), are presented here, so that SOA formation may be computed as a function of M o , NO x level, and temperature. Current research needs and future research directions are identified.

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“…The contribution of NO 3 to the total isoprene SOA is approximately 50% greater than OH in this regionally polluted area. However, this does not consider other possible routes for SOA formation from isoprene, such as heterogeneous reactions (Altieri et al, 2006;Ervens et al, 2008;Liggio et al, Analysis of several other flights showed correlations between nocturnally oxidized isoprene and observed WSOC, non-negligible contributions of NO 3 -isoprene SOA to total organic aerosol, and large nighttime isoprene-SOA compared to photochemical isoprene-SOA, as shown in Table 3. Figure 12 gives one additional example, from the night flight on 7 August which sampled mainly along the coastline from New Jersey to Massachusetts under conditions of offshore flow.…”

Section: Secondary Organic Aerosolmentioning

confidence: 99%

Nocturnal isoprene oxidation over the Northeast United States in summer and its impact on reactive nitrogen partitioning and secondary organic aerosol

et al. 2009

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Abstract. Isoprene is the largest single VOC emission to the atmosphere. Although it is primarily oxidized photochemically during daylight hours, late-day emissions that remain in the atmosphere at sunset undergo oxidation by NO 3 in regionally polluted areas with large NO x levels. A recent aircraft study examined isoprene and its nocturnal oxidants in a series of night flights across the Northeast US, a region with large emissions of both isoprene and NO x . Substantial amounts of isoprene that were observed after dark were strongly anticorrelated with measured NO 3 and were the most important factor determining the lifetime of this radical. The products of photochemical oxidation of isoprene, methyl vinyl ketone and methacrolein, were more uniformly distributed, and served as tracers for the presence of isoprene at sunset, prior to its oxidation by NO 3 . A determination of the mass of isoprene oxidized in darkness showed it to be a large fraction (>20%) of emitted isoprene. Organic nitrates produced from the NO 3 +isoprene reaction, though not directly measured, were estimated to account for 2-9% of total reactive nitrogen. The mass of isoprene oxidized by NO 3 was comparable to and correlated with the organic aerosol Correspondence to: S. S. Brown (steven.s.brown@noaa.gov) loading for flights with relatively low organic aerosol background. The contribution of nocturnal isoprene oxidation to secondary organic aerosol was determined in the range 1-17%, and isoprene SOA mass derived from NO 3 was calculated to exceed that due to OH by approximately 50%.

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Direct polymerization of isoprene and α‐pinene on acidic aerosols

Cited by 105 publications

References 19 publications

Quantitative assessment of organosulfates in size-segregated rural fine aerosol

Quantitative assessment of organosulfates in size-segregated rural fine aerosol

A review of Secondary Organic Aerosol (SOA) formation from isoprene

Nocturnal isoprene oxidation over the Northeast United States in summer and its impact on reactive nitrogen partitioning and secondary organic aerosol

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