Photochemical organonitrate formation in wet aerosols

Lim, Yong Bin; Kim, Hwajin; Kim, Jin Young; Turpin, Barbara J.

doi:10.5194/acp-16-12631-2016

Cited by 30 publications

(31 citation statements)

References 84 publications

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“…ON includes a wide variety of nitrogen-containing organic species that can be generally classified into three types, that is, reduced N (e.g., amines), oxidized N (e.g., organic nitrates), and ON from the biological or soil (e.g., humus) (Neff et al, 2002). Up to now, investigated components of particulate ON include amino acids (Zhang & Anastasio, 2003b), alkyl amines (Malloy et al, 2009;Murphy et al, 2007), organic nitrates (Ayres et al, 2015;Lim et al, 2016), nitrogen heterocycles (Ma & Hays, 2008), nitro-aromatics (Crimmins & Baker, 2006;Dimashki et al, 2000), and urea (Shi et al, 2010). ON compounds in the atmosphere have been shown to be important for the formation of particles and secondary organic aerosols (Lee et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

Water Soluble Organic Nitrogen (WSON) in Ambient Fine Particles Over a Megacity in South China: Spatiotemporal Variations and Source Apportionment

Zhu

et al. 2017

JGR Atmospheres

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Organic nitrogen aerosols are complex mixtures and important compositions in ambient fine particulate matters (PM2.5), yet their sources and spatiotemporal patterns are not well understood particularly in regions influenced by intensive human activities. In this study, filter‐based ambient PM2.5 samples at four stations (one urban, two rural, plus one urban roadside) and PM samples from combustion sources (vehicle exhaust, ship emission, and biomass burning) were collected in the coastal megacity Guangzhou, south China, for determining water soluble organic nitrogen (WSON) along with other organic and inorganic species. The annual average WSON concentrations, as well as the ratios of WSON to water soluble total nitrogen, were all significantly higher at rural sites than urban sites. Average WSON concentrations at the four sites during the wet season were quite near each other, ranging from 0.41 to 0.49 μg/m3; however, they became 2 times higher at the rural sites than at the urban sites during the dry season. Five major sources for WSON were identified through positive matrix factorization analysis. Vehicle emission (29.3%), biomass burning (22.8%), and secondary formation (20.2%) were three dominant sources of WSON at the urban station, while vehicle emission (45.4%) and dust (28.6%) were two dominant sources at the urban roadside station. At the two rural sites biomass burning (51.1% and 34.1%, respectively) and secondary formation (17.8% and 30.5%, respectively) were dominant sources of WSON. Ship emission contributed 8–12% of WSON at the four sites. Natural vegetation seemed to have very minor contribution to WSON.

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Section: Introductionmentioning

confidence: 99%

Water Soluble Organic Nitrogen (WSON) in Ambient Fine Particles Over a Megacity in South China: Spatiotemporal Variations and Source Apportionment

Zhu

et al. 2017

JGR Atmospheres

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“…The high correlation of RH with nitrate (r = 0.53; Table 5) implies a role of aqueous chemistry in nitrate aerosol formation in Seoul. A recent thermodynamic model simulation with smog chamber experiments and measurement data reveals that NO x photochemistry under high RH conditions facilitates the hygroscopic growth of aerosols through water and HNO 3 uptake cycles with organonitrate formation in aerosol liquid water (Lim et al, 2016) and thus contributes to the high nitrate proportion to PM 2.5 in Seoul (Fig. 4a).…”

Section: Temporal Evolution Of the Multiday Hazementioning

confidence: 99%

On the multiday haze in the Asian continental outflow: the important role of synoptic conditions combined with regional and local sources

et al. 2017

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Abstract. The air quality of the megacities in populated and industrialized regions like East Asia is affected by both local and regional emission sources. The combined effect of regional transport and local emissions on multiday haze was investigated through a synthetic analysis of PM 2.5 sampled at both an urban site in Seoul, South Korea and an upwind background site on Deokjeok Island over the Yellow Sea during a severe multiday haze episode in late February 2014. Inorganic components and carbonaceous species of daily PM 2.5 samples were measured, and gaseous pollutants, local meteorological factors, and synoptic meteorological conditions were also determined. A dominance of fine-mode particles (PM 2.5 / PM 10 ∼ 0.8), a large secondary inorganic fraction (76 %), high OC / EC (> 7), and highly oxidized aerosols (oxygen-to-carbon ratio of ∼ 0.6 and organic-mass-to-carbon ratio of ∼ 1.9) under relatively warm, humid, and stagnant conditions characterize the multiday haze episode in Seoul; however, the early and late stages of the episode show different chemical compositions of PM 2.5 . High concentrations of sulfate in both Seoul and the upwind background in the early stage suggest a significant regional influence on the onset of the multiday haze. At the same time, high concentrations of nitrate and organic compounds in Seoul, which are local and highly correlated with meteorological factors, suggest the contribution of local emissions and secondary formation under stagnant meteorological conditions to the haze. A slow eastward-moving high-pressure system from southern China to the East China Sea induces the regional transport of aerosols and potential gaseous precursors for secondary aerosols from the North China Plain in the early stage but provides stagnant conditions conducive to the accumulation and the local formation of aerosols in the late stage. A blocking ridge over Alaska that developed during the episode hinders the zonal propagation of synoptic-scale systems and extends the haze period to several days. This study provides chemical insights into haze development sequentially by regional transport and local sources, and shows that the synoptic condition plays an important role in the dynamical evolution of long-lasting haze in the Asian continental outflow region.

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“…Descriptions can be found elsewhere (Lim et al, 2016). In summary, 5 m 3 PTFE smog chamber at Korea Institute of Science and Technology (KIST), Seoul, Korea was used.…”

Section: Chamber Methodsmentioning

confidence: 99%

“…We have conducted smog chamber experiments of photochemistry of wet aerosols containing glyoxal, (NH 4 ) 2 SO 4 (or H 2 SO 4 ,), and H 2 O 2 in the presence of NO x and O 3 at high (> 70 % RH) and low (< 5 % RH) humid conditions (Lim et al, 2016). AS aerosols (the atomized aqueous solution of glyoxal, (NH 4 ) 2 SO 4 , and H 2 O 2 ) or SA aerosols (the atomized aqueous solution of glyoxal, H 2 SO 4 , and H 2 O 2 ) were introduced into a 5 m 3 PTFE smog chamber for photooxidation or dark reactions.…”

Section: Photochemical Aging Of Wet Aerosolsmentioning

confidence: 99%

“…to an aqueous chemistry full kinetic model (Lim et al, 2013;Lim and Turpin, 2015;Lim et al, 2016), and these concentrations of OH in the aqueous phase and the gas phase are atmospheric (Arakaki et al, 2013;Finlayson-Pitts and Pitts Jr, 1999). The aqueous-phase OH reactions of glyoxal also generate HO 2 (Lim et al, 2010) with ~ 10 -7 M in the aqueous phase according to the aqueous-phase kinetic model.…”

Section: Photochemical Aging Of Wet Aerosolsmentioning

confidence: 99%

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Multiday haze in the East Asia: Transport and chemical aging of hygroscopic particles

Lim

Seo

Kim

et al. 2018

Preprint

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Abstract. East Asian countries (Korea and China) have been experiencing exceedingly high concentrations of particulate matter (PM) that threatens health and potentially alters climate. However, the formation of East Asian PM is poorly understood. Furthermore, during the winter high PM concentrations at Seoul, Korea often occurs via the combination of the transport of Chinese haze through the prevailing Westerlies and the local formation at Seoul, and this complicates the PM formation. A severe multiday haze event occurred at Seoul during February 24&ndash;28, 2014, and the synoptic meteorological conditions suggest the combination the transport and the local formation (Seo et al., 2017). PM at Seoul and Deokjeok Island during this haze period was sampled and analyzed. Deokjeok Island provides background for Seoul PM since it is upwind and emission free. We hypothesize that transported PM from China (PM at Deokjeok Island) is hygroscopic (thus contains water due to high RH) and undergoes multiphase photochemical aging at Seoul. To validate our hypothesis, we conducted smog chamber experiments. In a humid smog chamber, photochemistry of NOx initiates hygroscopic growth of particles and aerosol liquid water in turn facilitates aqueous chemistry forming organonitrates and oligomers. This multiphase chemistry provides chemical insights of chemical aging during a haze event in East Asia. NOx effects on photochemical aging of particles are substantial. Even a few ppb of NOx form nitrates in aerosol liquid water, and acidify neutral particles. NOx reduction is not likely to be an effective strategy for nitrate- and acidity-related health.

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Photochemical organonitrate formation in wet aerosols

Cited by 30 publications

References 84 publications

Water Soluble Organic Nitrogen (WSON) in Ambient Fine Particles Over a Megacity in South China: Spatiotemporal Variations and Source Apportionment

Water Soluble Organic Nitrogen (WSON) in Ambient Fine Particles Over a Megacity in South China: Spatiotemporal Variations and Source Apportionment

On the multiday haze in the Asian continental outflow: the important role of synoptic conditions combined with regional and local sources

Multiday haze in the East Asia: Transport and chemical aging of hygroscopic particles

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