Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing

Mehra, Archit; Canagaratna, Manjula R.; Bannan, Thomas J.; Worrall, Stephen D.; Bacak, Asan; Priestley, Michael; Liu, Dantong; Zhao, Jian; Xu, Weiqi; Sun, Yele; Hamilton, Jacqueline F.; Squires, Freya A.; Lee, James; Bryant, Daniel; Hopkins, James R.; Elzein, Atallah; Budisulistiorini, Sri Hapsari; Cheng, Xi; Chen, Qi; Wang, Yuwei; Wang, Lin; Stark, Harald; Krechmer, Jordan E.; Brean, James; Slater, Eloise; Whalley, Lisa K.; Heard, D. E.; Ouyang, Bin; Acton, W. Joe F.; Hewitt, C. Nicholas; Wang, Xinming; Fu, Pingqing; Jayne, John T.; Worsnop, Douglas R.; Allan, J. D.; Percival, Carl J.; Coe, Hugh

doi:10.1039/d0fd00080a

Cited by 17 publications

(13 citation statements)

References 123 publications

(125 reference statements)

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“…One possible explanation was the different formation mechanisms of LO-OOA in summer and winter. Although LO-OOA was dominantly from oxidation of anthropogenic VOCs, for example, organic nitrates from NO 3 oxidation at nighttime in winter due to low emissions of biogenic VOCs, it could have a large contribution from oxidation of biogenic VOCs in summer . Indeed, previous studies found that the monoterpene- and sesquiterpene-derived SOA decreased and the anthropogenic SOA from toluene oxidation increased with the increase in the height in the city …”

Section: Resultsmentioning

confidence: 99%

“…Although LO-OOA was dominantly from oxidation of anthropogenic VOCs, for example, organic nitrates from NO 3 oxidation at nighttime 58 in winter due to low emissions of biogenic VOCs, it could have a large contribution from oxidation of biogenic VOCs in summer. 59 Indeed, previous studies found that the monoterpene-and sesquiterpene-derived SOA decreased and the anthropogenic SOA from toluene oxidation increased with the increase in the height in the city. 43 We further compared the vertical differences between daytime and nighttime that were defined according to the diurnal variations of MLH (Figure S9).…”

Section: Aerosol Composition In the Urban Boundarymentioning

confidence: 98%

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Vertically Resolved Aerosol Chemistry in the Low Boundary Layer of Beijing in Summer

et al. 2022

Environ. Sci. Technol.

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Air quality in Beijing has been improved significantly in recent years; however, our knowledge of the vertically resolved aerosol chemistry in summer remains poor. Here, we carried out comprehensive measurements of aerosol composition, gaseous species, and aerosol optical properties on a meteorological tower in Beijing in summer and compared with those measured in winter. Our results showed that aerosol liquid water (ALW) contributing approximately 50% of the total mass with higher values aloft played a crucial role in aerosol formation. Particularly, the higher nitrate concentration in city aloft than at the ground level during daytime was mainly due to the enhanced gas–particle partitioning driven by ALW and particle acidity. The vertical profiles of organic aerosol (OA) factors varied more differently in the urban boundary layer. Although the ubiquitous decreases in primary OA with the increase in height were mainly due to the influences of local emissions and vertical convection, the vertical differences in oxygenated OA between summer and winter may be related to the photochemical processing of different biogenic and anthropogenic volatile organic compounds. The single-scattering albedo, brown carbon, and absorption Ångstrom exponent of aerosol particles also presented different vertical profiles between day and night due to the vertical changes in aerosol chemistry.

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Section: Resultsmentioning

confidence: 99%

Section: Aerosol Composition In the Urban Boundarymentioning

confidence: 98%

Vertically Resolved Aerosol Chemistry in the Low Boundary Layer of Beijing in Summer

et al. 2022

Environ. Sci. Technol.

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“…These I – -adduct ions (C x H y O z X n , where X = S or N, x , y , z ≥ 1 and n ≤ 2) contributed to 90–97% of the total signals of the detected organic ions, which consist of 989 C x H y O z , 856 C x H y O z N n , and 36 C x H y O z S n I – -adduct ions. In the C x H y O z N n category, 583 compounds with the formula of C x H y O z N 1 ( y is an odd number ≤ 2 x + 3 and z ≥ 4 except C 6 H 5 NO 4 , C 7 H 7 NO 4 , and C 8 H 9 NO 4 that were more likely nitrated phenols in urban environments) were tentatively designated as ONs. − Signal contributions of ions with two nitrogen or sulfur atoms are relatively minor. We also fitted three deprotonated organosulfate ions (i.e., C 3 H 5 SO 5 – , C 2 H 3 SO 6 – , C 3 H 5 SO 6 – ) in the analysis.…”

Section: Experimental Methodsmentioning

confidence: 99%

Precursors and Pathways Leading to Enhanced Secondary Organic Aerosol Formation during Severe Haze Episodes

Zheng

Chen

Cheng

et al. 2021

Environ. Sci. Technol.

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Molecular analyses help to investigate the key precursors and chemical processes of secondary organic aerosol (SOA) formation. We obtained the sources and molecular compositions of organic aerosol in PM 2.5 in winter in Beijing by online and offline mass spectrometer measurements. Photochemical and aqueous processing were both involved in producing SOA during the haze events. Aromatics, isoprene, long-chain alkanes or alkenes, and carbonyls such as glyoxal and methylglyoxal were all important precursors. The enhanced SOA formation during the severe haze event was predominantly contributed by aqueous processing that was promoted by elevated amounts of aerosol water for which multifunctional organic nitrates contributed the most followed by organic compounds having four oxygen atoms in their formulae. The latter included dicarboxylic acids and various oxidation products from isoprene and aromatics as well as products or oligomers from methylglyoxal aqueous uptake. Nitrated phenols, organosulfates, and methanesulfonic acid were also important SOA products but their contributions to the elevated SOA mass during the severe haze event were minor. Our results highlight the importance of reducing nitrogen oxides and nitrate for future SOA control. Additionally, the formation of highly oxygenated long-chain molecules with a low degree of unsaturation in polluted urban environments requires further research.

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“…POs are also frequently detected in ambient particles. ,,,, Particulate POs have been measured as HOMs using offline filter analysis by LC-ESI-MS. ,,, In recent years, online analytical techniques such as FIGAERO-ToF-CIMS ,− and EESI-ToF-MS ,, have been applied to characterize POs in ambient particles. Oxygenated organic compounds in the particle phase measured by FIGAERO-ToF-CIMS explained 24% of the total organic aerosol mass measured by AMS at an urban site during the autumn season in Guangzhou, among which substantial species could be POs .…”

Section: Observations Of Pos In Laboratory and Field Studiesmentioning

confidence: 99%

“…Oxygenated organic compounds in the particle phase measured by FIGAERO-ToF-CIMS explained 24% of the total organic aerosol mass measured by AMS at an urban site during the autumn season in Guangzhou, among which substantial species could be POs . Source apportionment analyses, like positive matrix factorization (PMF) and clustering analysis of MS data derived from online measurements, have helped reveal the major sources of particulate HOMs and their temporal evolution in different atmospheric environments. ,, The enrichment of HOMs in ambient particles may be relevant to the activation of cloud condensation nuclei (CCN). ,, Organic aerosol with higher oxygenation level was observed to have higher CCN activity. , In boreal regions, monoterpene-derived HOMs could result in an overall 10% enhancement in CCN concentration . There may also be implications on potential health impacts of PM that is rich in HOMs.…”

Section: Observations Of Pos In Laboratory and Field Studiesmentioning

confidence: 99%

Organic Peroxides in Aerosol: Key Reactive Intermediates for Multiphase Processes in the Atmosphere

et al. 2023

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Organic peroxides (POs) are organic molecules with one or more peroxide (−O−O−) functional groups. POs are commonly regarded as chemically labile termination products from gas-phase radical chemistry and therefore serve as temporary reservoirs for oxidative radicals (HO x and RO x ) in the atmosphere. Owing to their ubiquity, active gasparticle partitioning behavior, and reactivity, POs are key reactive intermediates in atmospheric multiphase processes determining the life cycle (formation, growth, and aging), climate, and health impacts of aerosol. However, there remain substantial gaps in the origin, molecular diversity, and fate of POs due to their complex nature and dynamic behavior. Here, we summarize the current understanding on atmospheric POs, with a focus on their identification and quantification, state-of-the-art analytical developments, molecular-level formation mechanisms, multiphase chemical transformation pathways, as well as environmental and health impacts. We find that interactions with SO 2 and transition metal ions are generally the fast PO transformation pathways in atmospheric liquid water, with lifetimes estimated to be minutes to hours, while hydrolysis is particularly important for α-substituted hydroperoxides. Meanwhile, photolysis and thermolysis are likely minor sinks for POs. These multiphase PO transformation pathways are distinctly different from their gas-phase fates, such as photolysis and reaction with OH radicals, which highlights the need to understand the multiphase partitioning of POs. By summarizing the current advances and remaining challenges for the investigation of POs, we propose future research priorities regarding their origin, fate, and impacts in the atmosphere.

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Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing

Abstract: We study the anthropogenic and biogenic contributions to organic aerosol.

Cited by 17 publications

References 123 publications

Vertically Resolved Aerosol Chemistry in the Low Boundary Layer of Beijing in Summer

Vertically Resolved Aerosol Chemistry in the Low Boundary Layer of Beijing in Summer

Precursors and Pathways Leading to Enhanced Secondary Organic Aerosol Formation during Severe Haze Episodes

Organic Peroxides in Aerosol: Key Reactive Intermediates for Multiphase Processes in the Atmosphere

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