Tropospheric aerosol as a reactive intermediate

Colussi, A. J.; Enami, Shinichi; Yabushita, Akihiro; Hoffmann, Michael R.; Liu, Wei Guang; Mishra, Himanshu; Goddard, William A.

doi:10.1039/c3fd00040k

Cited by 35 publications

(57 citation statements)

References 96 publications

(180 reference statements)

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“…In this experiment the initial NO 2 concentration (NO 2 (i) = 47 ppb) was higher than the measured outdoor levels. However, as discussed in previously published papers, NO 2 may react with O 3 and OH − (formed at ambient relative humidity) in the reaction chamber, leading to the formation of HNO 3 − , HONO, and other possible derivatives, and hence to a reduction in the NO 2 levels and the spore reaction rates (Colussi et al, 2013;Crutzen, 1988;Finlayson-Pitts and Pitts, 2000;Song et al, 2011;Spicer et al, 1993).…”

Section: Resultsmentioning

confidence: 95%

Impact of urban air pollution on the allergenicity of Aspergillus fumigatus conidia: Outdoor exposure study supported by laboratory experiments

Lang‐Yona

Shuster-Meiseles

Mazar

et al. 2016

Science of The Total Environment

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Section: Resultsmentioning

confidence: 95%

Impact of urban air pollution on the allergenicity of Aspergillus fumigatus conidia: Outdoor exposure study supported by laboratory experiments

Lang‐Yona

Shuster-Meiseles

Mazar

et al. 2016

Science of The Total Environment

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“…14−17 Aerosol uptake of NO 2 with γ on the order of 10 −4 ∼ 10 −3 has been observed and linked to the catalysis effect of photochemically formed dicarboxylic acid anions. 17 These findings suggest that tropospheric aerosols might play a much more important role in daytime HONO production than previously thought over regions with high loads of aerosols that have favorable chemical compositions.…”

Section: ■ Introductionmentioning

confidence: 91%

Evidence of Aerosols as a Media for Rapid Daytime HONO Production over China

Liu

Wang

Costabile

et al. 2014

Environ. Sci. Technol.

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Current knowledge of daytime HONO sources remains incomplete. A large missing daytime HONO source has been found in many places around the world, including polluted regions in China. Conventional understanding and recent studies attributed this missing source mainly to ground surface processes or gas-phase chemistry, while assuming aerosols to be an insignificant media for HONO production. We analyze in situ observations of HONO and its precursors at an urban site in Beijing, China, and report an apparent dependence of the missing HONO source strength on aerosol surface area and solar ultraviolet radiation. Based on extensive correlation analysis and process-modeling, we propose that the rapid daytime HONO production in Beijing can be explained by enhanced hydrolytic disproportionation of NO2 on aqueous aerosol surfaces due to catalysis by dicarboxylic acid anions. The combination of high abundance of NO2, aromatic hydrocarbons, and aerosols over broad regions in China likely leads to elevated HONO levels, rapid OH production, and enhanced oxidizing capacity on a regional basis. Our findings call for attention to aerosols as a media for daytime heterogeneous HONO production in polluted regions like Beijing. This study also highlights the complex and uncertain heterogeneous chemistry in China, which merits future efforts of reconciling regional modeling and laboratory experiments, in order to understand and mitigate the regional particulate and O3 pollutions over China.

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“…Liu et al (2012b) investigated satellite products and reported a relatively high concentration of glyoxal (discarboxylic acid precursor) in central China. Colussi et al (2013) reported that the carboxylate anions can work as a catalyst to promote the disproportionation of NO 2 on water and HONO formation. This may have driven the heterogeneous HONO generation in the northern central plain of China.…”

Section: Effect On O 3 Spatial Distributionmentioning

confidence: 99%

“…However, the importance of aerosol surface area with respect to heterogeneous HONO formation remains controversial. Some studies reported relatively low (10 −7 to 10 −6 ) NO 2 uptake coefficients on the aerosol surface area (Stemmler et al 2007), whereas others observed uptake coefficients of 10 −4 to 10 −3 (Colussi et al 2013).…”

Section: Introductionmentioning

confidence: 99%

Evidence of heterogeneous HONO formation from aerosols and the regional photochemical impact of this HONO source

Wang

et al. 2018

Environ. Res. Lett.

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Large missing daytime HONO sources have been reported by many previous studies around the world. Possible HONO sources include ground heterogeneous conversion, aerosol heterogeneous formation, soil emission, and photochemical production. In this study, a consistent 1D framework based on regional and 3D chemical transport models (CTMs) was used to analyze the unknown daytime HONO sources in 14 cases worldwide. We assume that the source of HONO from aerosols is through NO 2 hydrolysis (not including its oxidation products) and that non-local mixing effect is negligible. Assuming all the missing unknown HONO source is from the ground, it would imply a NO 2 -to-HONO ground heterogeneous conversion exceeding 100% in daytime, which is unphysical. In contrast, a strong R 2 reaching up to 0.92 is found between the unknown HONO sources and the products of aerosol wet surface area and short-wave radiation. Because the largest unknown daytime HONO sources are found in China due to high concentrations of aerosols and NO 2 , we derive an optimized NO 2 uptake coefficient on the basis of these measurements. The 3D CTM simulations suggest that in some regions of central, eastern, and southwestern (e.g. SiChuan province) China, the aerosol HONO source has the greatest effects on ozone (>10 ppbv) and OH (>200%) in winter. In January, the simulated particulate sulfate level over these three regions increases by 6-10 μg m −3 after including the aerosol-HONO source, which helps reduce the previous model underestimation of sulfate production in winter. Additional measurement studies that target the daytime HONO sources will be essential to a better understanding of the mechanisms and resulting effects on atmospheric oxidants.

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Tropospheric aerosol as a reactive intermediate

Abstract: In tropospheric chemistry, secondary organic aerosol (SOA) is deemed an end product.Here, on the basis of new evidence, we make the case that SOA is a key reactive

Cited by 35 publications

References 96 publications

Impact of urban air pollution on the allergenicity of Aspergillus fumigatus conidia: Outdoor exposure study supported by laboratory experiments

Impact of urban air pollution on the allergenicity of Aspergillus fumigatus conidia: Outdoor exposure study supported by laboratory experiments

Evidence of Aerosols as a Media for Rapid Daytime HONO Production over China

Evidence of heterogeneous HONO formation from aerosols and the regional photochemical impact of this HONO source

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