Uptake of Water‐soluble Gas‐phase Oxidation Products Drives Organic Particulate Pollution in Beijing

Gkatzelis, Georgios I.; Papanastasiou, Dimitrios K.; Karydis, Vlassis A.; Hohaus, Thorsten; Liu, Ying; Schmitt, Sebastian; Schlag, Patrick; Fuchs, Hendrik; Novelli, Anna; Chen, Qi; Cheng, Xi; Broch, Sebastian; Dong, Huabin; Holland, F.; Li, Xin; Liu, Yuhan; Ma, Xuefei; Reimer, David; Rohrer, Franz; Shao, Min; Tan, Zhaofeng; Taraborrelli, Domenico; Tillmann, Ralf; Wang, Haichao; Wang, Yu; Wu, Yusheng; Wu, Zhijun; Zeng, Limin; Zheng, Jun; Hu, Min; Lu, Keding; Hofzumahaus, A.; Zhang, Yuanhang; Wahner, Andreas; Kiendler‐Scharr, Astrid

doi:10.1029/2020gl091351

Cited by 29 publications

(49 citation statements)

References 105 publications

(75 reference statements)

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“…Given the high relative humidity (RH%) (74 ± 9%; Supplementary Table 2) and the abundant hygroscopic particles (particularly for particulate nitrate as shown in Supplementary Fig. 4) in our continental out ow samples, we expect that the changes in the gas-particle partitioning driven by the increased ALW could have enhanced the formation of aqSOA species, such as oxalic acid 23,26,32 . This can be supported by the sixfold higher aqSOA precursors (Gly + MeGly) mass fractions in OC observed in the continental out ow samples than the coastal background (Supplementary Table 4).…”

Section: Meteorological Setting and Aerosol Molecular Compositionsmentioning

confidence: 99%

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China

Zhang

Gustafsson

et al. 2021

Preprint

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Incomplete understanding of the sources of secondary organic aerosol (SOA) leads to large uncertainty in both air quality management and in climate change assessment. Chemical reactions occurring in the atmospheric aqueous phase represent an important source of SOA mass, yet, the effects of anthropogenic emissions on the aqueous SOA (aqSOA) are not well constrained. Here we use compound-specific dual-carbon isotopic fingerprints (δ13C and Δ14C) of dominant aqSOA molecules, such as oxalic acid, to track the precursor sources and formation mechanisms of aqSOA. Substantial stable carbon isotope fractionation of aqSOA molecules provides robust evidence for extensive aqueous-phase processing. Contrary to the paradigm that these aqSOA compounds are largely biogenic, radiocarbon-based source apportionments show that fossil precursors produced over one-half of the aqSOA molecules. Large fractions of fossil-derived aqSOA contribute substantially to the total water-soluble organic aerosol load and hence impact projections of both air quality and anthropogenic radiative forcing. Our findings reveal the importance of fossil emissions for aqSOA with effects on climate and air quality.

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Section: Meteorological Setting and Aerosol Molecular Compositionsmentioning

confidence: 99%

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China

Zhang

Gustafsson

et al. 2021

Preprint

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“…Therefore, fundamental processes of SOA formation in the aqueous phase (e.g., from isoprene epoxydiols (Nguyen et al, 2009) and glyoxal (Fu et al, 2008)) are typically missing from the conventionally used parameterizations. In addition, the uptake of small carbonyls (e.g., aldehydes and acids) to the aqueous phase and their subsequent oxidation and oligomerization has been recently linked to significant increases of SOA mass during pollution events (Gkatzelis et al, 2021).…”

Section: Discussionmentioning

confidence: 99%

“…This is mostly evident during winter (e.g., over Europe), when the relative importance of these processes on SOA formation is increasing due to the lower photochemical activity and the limited conversion of gas phase organic precursors to SOA. In addition, recent studies have provided strong evidence that the uptake of water-soluble gas-phase oxidation products (even small carbonyls like formaldehyde and acetic acid) can be the main driver of SOA pollution during haze events over Eastern Asia (Gkatzelis et al, 2020).…”

Section: Organic Aerosols (Oa)mentioning

confidence: 99%

“…The mechanism has been employed to study the impact of isoprene OH−recycling above pristine tropical forests (Taraborrelli et al, 2012), oxidation of monoterpenes as a source of HO 2 (Hens et al, 2014;Mallik et al, 2018) and the influence of aromatics on tropospheric ozone (Taraborrelli et al, 2021). Furthermore, MOM has been used with extensions in order to simulate product yields of β-caryophyllene oxidation (van Eijck et al, 2013), the oxidation of alkyl amines and formamide as source of HNCO (Rosanka et al, 2020), the atmospheric losses of stabilised Criegee intermediates (Vereecken et al, 2017), and the most recent OH-recycling mechanisms in isoprene oxidation (Novelli et al, 2020). Yet, a full evaluation of the VOC distribution predicted by MOM in a global numerical model has not been published.…”

Section: Introductionmentioning

confidence: 99%

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Simulation of organics in the atmosphere: evaluation of EMACv2.54 with the Mainz Organic Mechanism (MOM) coupled to the ORACLE (v1.0) submodel

Pozzer

Reifenberg

Kumar

et al. 2021

Preprint

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Abstract. An updated and expanded representation of organics in the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) has been evaluated. First, the comprehensive Mainz Organic Mechanism (MOM) in the submodel MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) was activated with explicit degradation of organic species up to five carbon atoms and a simplified mechanism for larger molecules. Second, the ORACLE submodel (version 1.0) considers now condensation on aerosols for all organics in the mechanism. Parameterizations for aerosol yields are used only for the lumped species that are not included in the explicit mechanism. The simultaneous usage of MOM and ORACLE allows an efficient estimation, not only of the chemical degradation of the simulated volatile organic compounds, but also of the contribution of organics to the growth and fate of (organic) aerosol, with a complexity of the mechanism largely increased compared to EMAC simulations with more simplified chemistry. The model evaluation presented here reveals that the OH concentration is well reproduced globally, while significant biases for observed oxygenated organics are present. We also investigate the general properties of the aerosols and their composition, showing that the more sophisticated and process-oriented secondary aerosol formation does not degrade the good agreement of previous model configurations with observations at the surface, allowing further research in the field of gas-aerosol interactions.

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“…This is mostly evident during winter (e.g., over Europe), when the relative importance of these processes on SOA formation is increasing due to the lower photochemical activity and the limited conversion of gas phase organic precursors to SOA. In addition, recent studies have 550 provided strong evidence that the uptake of water-soluble gas-phase oxidation products (even small carbonyls like formaldehyde and acetic acid) can be the main driver of SOA pollution during haze events over Eastern Asia (Gkatzelis et al, 2020).…”

Uptake of Water‐soluble Gas‐phase Oxidation Products Drives Organic Particulate Pollution in Beijing

Cited by 29 publications

References 105 publications

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China

Simulation of organics in the atmosphere: evaluation of EMACv2.54 with the Mainz Organic Mechanism (MOM) coupled to the ORACLE (v1.0) submodel

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