Aqueous production of secondary organic aerosol from fossil-fuel emissions in winter Beijing haze

Wang, Jun Feng; Ye, Jianhuai; Zhang, Qi; Zhao, Jian; Wu, Yangzhou; Li, Jingyi; Liu, Dantong; Li, Weijun; Zhang, Yange; Wu, Cheng; Xie, Conghui; Qin, Yi-Ping; Lei, Yali; Huang, Xiaoyong; Guo, Jianping; Liu, Pengfei; Fu, Pingqing; Li, Yongjie; Lee, Hyun Chul; Choi, Hyoungwoo; Zhang, Jie; Liao, Hong; Chen, Mindong; Sun, Yele; Ge, Xinlei; Martin, Scot T.; Jacob, Daniel J.

doi:10.1073/pnas.2022179118

Cited by 115 publications

(126 citation statements)

References 69 publications

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“…The contribution of SOA formed by aqueous-phase ways (aqSOA) is also much greater in summer (9-13%) because high emissions of isoprene enhance the formation of IEPOX, glyoxal, and methylglyoxal (Hu et al, 2017). Field observations suggest an important role of aqSOA in SOA formation during the winter haze periods (Kuang et al, 2020;Wang et al, 2021). The simulated mass fraction of aqSOA is only 3-5% in SOA in winter herein, indicating that more precursors are perhaps involved in the SOA formation related to aerosol liquid water than the model has considered (Gkatzelis et al, 2021).…”

Section: Resultsmentioning

confidence: 99%

Process-based and Observation-constrained SOA Simulations in China: The Role of Semivolatile and Intermediate-Volatility Organic Compounds and OH Levels

Miao¹,

Chen²,

Shrivastava³

et al. 2021

Preprint

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Abstract. Organic aerosol (OA) is a major component of tropospheric submicron aerosol that contributes to air pollution and causes adverse effects on human health. Chemical transport models have difficulties to reproduce the variability of OA concentrations in polluted areas, hindering understanding of the OA budget. Herein, we applied both process-based and observation-constrained schemes to simulate OA in GEOS-Chem. Comprehensive data sets of surface OA, OA components, secondary organic aerosol (SOA) precursors, and oxidants were used for model-observation comparisons. In the revised schemes, updates of the emissions, volatility distributions, and SOA yields of semivolatile and intermediate volatility organic compounds (S/IVOCs) were made. These updates are however insufficient to reproduce the SOA concentrations in observations. The addition of nitrous acid sources is an important model modification, which improves the simulation of surface concentrations of hydroxyl radical (OH) in winter in northern China. The increased surface OH concentrations enhance the SOA formation and lead to greater SOA mass concentrations by over 30 %, highlighting the importance of having good OH simulations in air quality models. There is a greater sensitivity of the SOA formation to the oxidant levels in winter than in summer in China. With all the model improvements, both the process-based and observation-constrained SOA schemes can reproduce the observed mass concentrations of SOA and show spatial and seasonal consistency with each other. Our best model simulations suggest that anthropogenic S/IVOCs are the dominant source of SOA in China with a contribution of over 50 %. The residential sector may be the predominant source of S/IVOCs in winter, despite large uncertainty remains in the emissions of IVOCs from the residential sector in northern China. The industry sector is also an important source of IVOCs, especially in summer. More S/IVOC measurements are needed to constrain their emissions.

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Section: Resultsmentioning

confidence: 99%

Process-based and Observation-constrained SOA Simulations in China: The Role of Semivolatile and Intermediate-Volatility Organic Compounds and OH Levels

Miao¹,

Chen²,

Shrivastava³

et al. 2021

Preprint

View full text Add to dashboard Cite

show abstract

“…The contribution of SOA formed by aqueous-phase ways (aqSOA) is also much greater in summer (9 %-13 %) because high emis-sions of isoprene enhance the formation of isoprene epoxydiols (IEPOX), glyoxal, and methylglyoxal (Hu et al, 2017). Field observations suggest an important role of aqSOA in SOA formation during the winter haze periods (Kuang et al, 2020;Wang et al, 2021). The simulated mass fraction of aq-SOA is only 3 %-5 % in SOA in winter herein, indicating that more precursors are perhaps involved in the SOA formation related to aerosol liquid water than the model has considered (Gkatzelis et al, 2021).…”

Section: Budget and Sources Of Oa In Eastern Chinamentioning

confidence: 99%

Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels

et al. 2021

View full text Add to dashboard Cite

Abstract. Organic aerosol (OA) is a major component of tropospheric submicron aerosol that contributes to air pollution and causes adverse effects on human health. Chemical transport models have difficulties in reproducing the variability in OA concentrations in polluted areas, hindering understanding of the OA budget and sources. Herein, we apply both process-based and observation-constrained schemes to simulate OA in GEOS-Chem. Comprehensive data sets of surface OA, OA components, secondary organic aerosol (SOA) precursors, and oxidants were used for model–observation comparisons. The base models generally underestimate the SOA concentrations in China. In the revised schemes, updates were made on the emissions, volatility distributions, and SOA yields of semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) and additional nitrous acid sources. With all the model improvements, both the process-based and observation-constrained SOA schemes can reproduce the observed mass concentrations of SOA and show spatial and seasonal consistency with each other. Our best model simulations suggest that anthropogenic SVOCs and IVOCs are the dominant source of SOA, with a contribution of over 50 % in most of China, which should be considered for pollution mitigation in the future. The residential sector may be the predominant source of SVOCs and IVOCs in winter, despite large uncertainty remaining in the emissions of IVOCs from the residential sector in northern China. The industry sector is also an important source of IVOCs, especially in summer. More SVOC and IVOC measurements are needed to constrain their emissions. Besides, the results highlight the sensitivity of SOA to hydroxyl radical (OH) levels in winter in polluted environments. The addition of nitrous acid sources can lead to over 30 % greater SOA mass concentrations in winter in northern China. It is important to have good OH simulations in air quality models.

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“…whereas Wang et al (2021) propose that rapid aqueous-phase oxidation of primary OA dominates SOA formation and would resolve the observed decline in SOA in Beijing in winter at the same time that NMVOCs emissions have remained relatively constant.…”

Section: Influence Of Emissions and Meteorology On Air Quality In Aw2017mentioning

confidence: 95%

Assessment of strict autumn-winter emission controls on air quality in the Beijing-Tianjin-Hebei region

Marais

et al. 2021

Preprint

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Abstract. Strict seasonal emission controls are a popular measure in China for addressing severe air pollution, in particular fine particulate matter (PM2.5). Here we evaluate the efficacy of these measures, with a particular focus on the strict emission controls imposed on pollution sources in 28 cities in and around the Beijing-Tianjin-Hebei region (BTH) in autumn-winter 2017/2018. For this we use the GEOS-Chem chemical transport model and air pollutant measurements from the national and Beijing local monitoring networks, after evaluating the network data with independent measurements and correcting large biases in the bottom-up emissions inventory. The network measurements are temporally consistent (r > 0.9 for PM2.5 and r > 0.7 for gases) with the independent measurements, though with systematic differences of 5–17 % for nitrogen dioxide (NO2) and 16–28 % for carbon monoxide (CO). The average decrease in monitoring network PM2.5 in BTH in autumn-winter 2017/2018 relative to the previous year is 27 %, declining from 103 to 75 µg m−3. The regional decline in PM2.5 in the model is 20 %, exceeding the regional target of 15 %. According to the model, pollution control measures led to decline in PM2.5 precursor emissions of 0.27 Tg NOx (as NO), 0.66 Tg sulfur dioxide (SO2), 70 Gg organic carbon (OC), and 50 Gg black carbon (BC). We find though that these alone only lead to an 8 % decline in PM2.5 and that interannual variability in meteorology accounts for more than half (57 %) the decline. This demonstrates that year-on-year comparisons are misleading for assessing the efficacy of air pollution measures and should be taken into consideration when extending such measures beyond BTH.

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Aqueous production of secondary organic aerosol from fossil-fuel emissions in winter Beijing haze

Cited by 115 publications

References 69 publications

Process-based and Observation-constrained SOA Simulations in China: The Role of Semivolatile and Intermediate-Volatility Organic Compounds and OH Levels

Process-based and Observation-constrained SOA Simulations in China: The Role of Semivolatile and Intermediate-Volatility Organic Compounds and OH Levels

Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels

Assessment of strict autumn-winter emission controls on air quality in the Beijing-Tianjin-Hebei region

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