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  • Copernicus GmbH  (12)
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  • Copernicus GmbH  (12)
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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 21 ( 2020-11-13), p. 13591-13610
    Abstract: Abstract. Atmospheric black carbon (BC) in the Tibetan Plateau (TP) can largely impact regional and global climate. Still, studies on the inter-annual variation in atmospheric BC over the TP and associated variation in BC sources and controlling factors are rather limited. In this study, we characterize the variations in atmospheric BC over the TP surface layer through analysis of 20-year (1995–2014) simulations from a global chemical transport model, GEOS-Chem. The results show that surface BC concentrations over the TP vary largely in space and by season, reflecting complicated interplays of BC sources from different origins. Of all areas in the TP, surface BC concentrations are highest over the eastern and southern TP, where surface BC is susceptible to BC transport from East Asia and South Asia, respectively. Applying a backward-trajectory method that combines BC concentrations from GEOS-Chem and trajectories from the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model, we assess the contributions of worldwide source regions to surface BC in the TP. We estimate that on the 20-year average, 77 % of surface BC in the TP comes from South Asia (43 %) and East Asia (35 %). Regarding seasonal variation in non-local influences, South Asia and East Asia are dominant source regions in winter and summer, respectively, in terms of the amount of BC imported. However, in terms of affected areas in the TP, South Asia is the dominant contributor throughout the year. Inter-annually, surface BC over the TP is largely modulated by atmospheric transport of BC from non-local regions year-round and by biomass burning in South Asia, mostly in spring. We find that the extremely strong biomass burning in South Asia in the spring of 1999 greatly enhanced surface BC concentrations in the TP (31 % relative to the climatology). We find that the strength of the Asian monsoon correlates significantly with the inter-annual variation in the amount of BC transported to the TP from non-local regions. In summer, a stronger East Asian summer monsoon and a stronger South Asian summer monsoon tend to, respectively, lead to more BC transport from central China and north-eastern South Asia to the TP. In winter, BC transport from central China is enhanced in years with a strong East Asian winter monsoon or a strong Siberian High. A stronger Siberian High can also bring more BC from northern South Asia to the TP. This study underscores the impacts of atmospheric transport and biomass burning on the inter-annual variation in surface BC over the TP. It reveals a close connection between the Asian monsoon and atmospheric transport of BC from non-local regions to the TP.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 2
    Online Resource
    Online Resource
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 12 ( 2018-06-18), p. 8491-8504
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 12 ( 2018-06-18), p. 8491-8504
    Abstract: Abstract. During the Asian summer monsoon season, prevailing southeasterly–southwesterly winds are subject to delivering air pollutants from the North China Plain (NCP) to northeast and northwest China. In the present study, the WRF-CHEM model is used to evaluate contributions of trans-boundary transport of NCP emissions to the air quality in northeast and northwest China during a persistent air pollution episode from 22 to 28 May 2015. The WRF-CHEM model generally performs well in capturing the observed temporal variation and spatial distribution of fine particulate matter (PM2.5), ozone (O3), and NO2. The simulated temporal variation of aerosol species is also in good agreement with measurements in Beijing during the episode. Model simulations show that NCP emissions contribute substantially to the PM2.5 level in Liaoning and Shanxi provinces, the adjacent downwind areas of the NCP, with an average of 24.2 and 13.9 µg m−3 during the episode, respectively. The PM2.5 contributions in Jilin and Shaanxi provinces are also appreciable, with an average of 9.6 and 6.5 µg m−3, respectively. The average percentage contributions of NCP emissions to the PM2.5 level in Liaoning, Jilin, Shanxi, and Shaanxi provinces are 40.6, 27.5, 32.2, and 20.9 %, respectively. The NCP emissions contribute remarkably to the O3 level in Liaoning province, with an average of 46.5 µg m−3, varying from 23.9 to 69.5 µg m−3. The O3 level in Shanxi province is also influenced considerably by NCP emissions, with an average contribution of 35.1 µg m−3. The O3 level in Shanxi province is also influenced considerably by NCP emissions, with an average contribution of 35.1 µg m−3. The average O3 contributions of NCP emissions to Jilin and Shaanxi provinces are 28.7 and 20.7 µg m−3, respectively. The average percentage contributions of NCP emissions to the afternoon O3 level in Liaoning, Jilin, Shanxi, and Shaanxi provinces are 27.4, 19.5, 21.2, and 15.8 %, respectively. However, the effect of NCP emissions on the air quality in Inner Mongolia is generally insignificant. Therefore, effective mitigation of NCP emissions not only improves the local air quality, but is also beneficial to the air quality in northeast and northwest China during the Asian summer monsoon season.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 13 ( 2019-07-10), p. 8703-8719
    Abstract: Abstract. Atmospheric aerosols scatter or absorb a fraction of the incoming solar radiation to cool or warm the atmosphere, decreasing surface temperature and altering atmospheric stability to further affect the dispersion of air pollutants in the planetary boundary layer (PBL). In the present study, simulations during a persistent and heavy haze pollution episode from 5 December 2015 to 4 January 2016 in the North China Plain (NCP) were performed using the Weather Research and Forecasting model with Chemistry (WRF-Chem) to comprehensively quantify contributions of aerosol shortwave radiative feedback (ARF) to near-surface (around 15 m above the ground surface) PM2.5 mass concentrations. The WRF-Chem model generally performs well in simulating the temporal variations and spatial distributions of air pollutants concentrations compared to observations at ambient monitoring sites in the NCP, and the simulated diurnal variations of aerosol species are also consistent with the measurements in Beijing. Additionally, the model simulates the aerosol radiative properties, the downward shortwave flux, and the PBL height against observations in the NCP well. During the episode, ARF deteriorates the haze pollution, increasing the near-surface PM2.5 concentrations in the NCP by 10.2 µg m−3 or with a contribution of 7.8 % on average. Sensitivity studies have revealed that high loadings of PM2.5 attenuate the incoming solar radiation reaching the surface to cool the low-level atmosphere, suppressing the development of the PBL, decreasing the surface wind speed, further hindering the PM2.5 dispersion, and consequently exacerbating the haze pollution in the NCP. Furthermore, when the near-surface PM2.5 mass concentration increases from around 50 to several hundred µg m−3, ARF contributes to the near-surface PM2.5 by more than 20 % during daytime in the NCP, substantially aggravating the heavy haze formation. However, when the near-surface PM2.5 concentration is less than around 50 µg m−3, ARF generally reduces the near-surface PM2.5 concentration due to the consequent perturbation of atmospheric dynamic fields.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 11 ( 2019-06-05), p. 7429-7443
    Abstract: Abstract. The implementation of the Air Pollution Prevention and Control Action Plan in China since 2013 has profoundly altered the ambient pollutants in the Beijing–Tianjin–Hebei (BTH) region. Here we show observations of substantially increased O3 concentrations (about 30 %) and a remarkable increase in the ratio of organic carbon (OC) to elemental carbon (EC) in BTH during the autumn from 2013 to 2015, revealing an enhancement in atmospheric oxidizing capacity (AOC) and secondary organic aerosol (SOA) formation. To explore the impacts of increasing AOC on the SOA formation, a severe air pollution episode from 3 to 8 October 2015 with high O3 and PM2.5 concentrations is simulated using the WRF-Chem model. The model performs reasonably well in simulating the spatial distributions of PM2.5 and O3 concentrations over BTH and the temporal variations in PM2.5, O3, NO2, OC, and EC concentrations in Beijing compared to measurements. Sensitivity studies show that the change in AOC substantially influences the SOA formation in BTH. A sensitivity case characterized by a 31 % O3 decrease (or 36 % OH decrease) reduces the SOA level by about 30 % and the SOA fraction in total organic aerosol by 17 % (from 0.52 to 0.43, dimensionless). Spatially, the SOA decrease caused by reduced AOC is ubiquitous in BTH, but the spatial relationship between SOA concentrations and the AOC is dependent on the SOA precursor distribution. Studies on SOA formation pathways further show that when the AOC is reduced, the SOA from oxidation and partitioning of semivolatile primary organic aerosol (POA) and co-emitted intermediate volatile organic compounds (IVOCs) decreases remarkably, followed by those from anthropogenic and biogenic volatile organic compounds (VOCs). Meanwhile, the SOA decrease in the irreversible uptake of glyoxal and methylglyoxal on the aerosol surfaces is negligible.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 13 ( 2019-07-10), p. 8721-8739
    Abstract: Abstract. Water vapor has been proposed to amplify the severe haze pollution in China by enhancing the aerosol–radiation feedback (ARF). Observations have revealed that the near-surface PM2.5 concentrations ([PM2.5]) generally exhibit an increasing trend with relative humidity (RH) in the North China Plain (NCP) during 2015 wintertime, indicating that the aerosol liquid water (ALW) caused by hygroscopic growth could play an important role in the PM2.5 formation and accumulation. Simulations during a persistent and heavy haze pollution episode from 5 December 2015 to 4 January 2016 in the NCP were conducted using the WRF-Chem Model to comprehensively quantify contributions of the ALW effect to near-surface [PM2.5]. The WRF-Chem Model generally performs reasonably well in simulating the temporal variations in RH against measurements in the NCP. The factor separation approach (FSA) was used to evaluate the contribution of the ALW effect on the ARF, photochemistry, and heterogeneous reactions to [PM2.5]. The ALW not only augments particle sizes to enhance aerosol backward scattering but also increases the effective radius to favor aerosol forward scattering. The contribution of the ALW effect on the ARF and photochemistry to near-surface [PM2.5] is not significant, being generally within 1.0 µg m−3 on average in the NCP during the episode. Serving as an excellent substrate for heterogeneous reactions, the ALW substantially enhances the secondary aerosol (SA) formation, with an average contribution of 71 %, 10 %, 26 %, and 48 % to near-surface sulfate, nitrate, ammonium, and secondary organic aerosol concentrations. Nevertheless, the SA enhancement due to the ALW decreases the aerosol optical depth and increases the effective radius to weaken the ARF, reducing near-surface primary aerosols. The contribution of the ALW total effect to near-surface [PM2.5] is 17.5 % on average, which is overwhelmingly dominated by enhanced SA. Model sensitivities also show that when the RH is less than 80 %, the ALW progressively increases near-surface [PM2.5] but commences to decrease when the RH exceeds 80 % due to the high occurrence frequencies of precipitation.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
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  • 6
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 4 ( 2022-02-24), p. 2507-2524
    Abstract: Abstract. Aerosol–planetary boundary layer (PBL) interaction has been proposed as a key mechanism for stabilizing the atmosphere and exacerbating surface air pollution. Although the understanding of this process has progressed enormously, its magnitude and impact remain uncertain and vary widely concerning aerosol types, vertical distributions, synoptic conditions, etc. In this study, our primary interest is to distinguish the aerosol–PBL interaction of absorbing and scattering aerosols under contrasting synoptic patterns and aerosol vertical distributions. Detailed in situ aircraft (King Air 350) measurements and online coupled model Weather Research and Forecasting with Chemistry (WRF-Chem) simulations are explored over the North China Plain (NCP). Furthermore, a long-term PBL stability trend from 1980 to 2020 over the NCP is also investigated. The aircraft measurements and surface observations show that the surface air pollution over the city of Baoding on 3 January is heavier than that on 4 January 2020. In addition, the aerosols are restricted to the low layer on 3 January, whereas the aerosols mix more homogeneously in an upwards direction on 4 January. Thus, we focus on the 2 d with distinct synoptic circumstances, PBL stability, and aerosol vertical distributions over the NCP. According to the WRF-Chem modeling, the synoptic pattern over Baoding differs between the 2 d. The prevailing wind direction is opposite with a southwesterly wind on 3 January and a northeasterly wind on 4 January. The results indicate that the synoptic condition may affect the PBL thermal structure, thus affecting the aerosol vertical distribution. Additionally, the sensitive numerical experiments reveal that the light-absorbing and light-scattering aerosols have different effects on altering the PBL thermal structure. The inhibition effect of scattering aerosols on the PBL appears to be independent of the aerosol height distribution and solely depends on its concentration. However, the aerosol–PBL feedback of absorbing aerosols is highly dependent on its vertical distribution. Besides the 2 d case investigation, the analysis of the modeling results for nearly 1 month from 3 to 30 January 2020 in Baoding yields a more robust and representative conclusion. Our analysis highlights that we should principally concentrate on controlling the emissions of scattering aerosols under the stable stratification, while cooperating to control the emissions of scattering and absorbing aerosols in an unstable stratification. Moreover, the long-term interannual variation in the PBL stability shows a strong correlation with the East Asian winter monsoon, which seems to be valuable in determining which pollutants to target in different monsoon years and attaining more precise air pollution control. Based on the numerical simulations and observational constraints, a concept scheme description has been concluded to deepen our recognition of the interactions between thermodynamic stability and aerosols within the PBL over the NCP region.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
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  • 7
    Online Resource
    Online Resource
    Copernicus GmbH ; 2017
    In:  Atmospheric Chemistry and Physics Vol. 17, No. 5 ( 2017-03-07), p. 3301-3316
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 5 ( 2017-03-07), p. 3301-3316
    Abstract: Abstract. Rapid industrialization and urbanization have caused frequent occurrence of haze in China during wintertime in recent years. The sulfate aerosol is one of the most important components of fine particles (PM2. 5) in the atmosphere, contributing significantly to the haze formation. However, the heterogeneous formation mechanism of sulfate remains poorly characterized. The relationships of the observed sulfate with PM2. 5, iron, and relative humidity in Xi'an, China have been employed to evaluate the mechanism and to develop a parameterization of the sulfate heterogeneous formation involving aerosol water for incorporation into atmospheric chemical transport models. Model simulations with the proposed parameterization can successfully reproduce the observed sulfate rapid growth and diurnal variations in Xi'an and Beijing, China. Reasonable representation of sulfate heterogeneous formation in chemical transport models considerably improves the PM2. 5 simulations, providing the underlying basis for better understanding the haze formation and supporting the design and implementation of emission control strategies.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 4 ( 2019-02-21), p. 2283-2298
    Abstract: Abstract. Particulate matter (PM) pollution is a severe environmental problem in the Beijing–Tianjin–Hebei (BTH) region in North China. PM studies have been conducted extensively in Beijing, but the chemical composition, sources, and atmospheric processes of PM are still relatively less known in nearby Tianjin and Hebei. In this study, fine PM in urban Shijiazhuang (the capital of Hebei Province) was characterized using an Aerodyne quadrupole aerosol chemical speciation monitor (Q-ACSM) from 11 January to 18 February in 2014. The average mass concentration of non-refractory submicron PM (diameter 〈1 µm, NR-PM1) was 178±101 µg m−3, and it was composed of 50 % organic aerosol (OA), 21 % sulfate, 12 % nitrate, 11 % ammonium, and 6 % chloride. Using the multilinear engine (ME-2) receptor model, five OA sources were identified and quantified, including hydrocarbon-like OA from vehicle emissions (HOA, 13 %), cooking OA (COA, 16 %), biomass burning OA (BBOA, 17 %), coal combustion OA (CCOA, 27 %), and oxygenated OA (OOA, 27 %). We found that secondary formation contributed substantially to PM in episodic events, whereas primary emissions were dominant (most significant) on average. The episodic events with the highest NR-PM1 mass range of 300–360 µg m−3 were comprised of 55 % of secondary species. On the contrary, a campaign-average low OOA fraction (27 %) in OA indicated the importance of primary emissions, and a low sulfur oxidation degree (FSO4) of 0.18 even at RH 〉90 % hinted at insufficient oxidation. These results suggested that in Shijiazhuang in wintertime fine PM was mostly from primary emissions without sufficient atmospheric aging, indicating opportunities for air quality improvement by mitigating direct emissions. In addition, secondary inorganic and organic (OOA) species dominated in pollution events with high-RH conditions, most likely due to enhanced aqueous-phase chemistry, whereas primary organic aerosol (POA) dominated in pollution events with low-RH and stagnant conditions. These results also highlighted the importance of meteorological conditions for PM pollution in this highly polluted city in North China.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 9
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 2 ( 2021-01-18), p. 681-694
    Abstract: Abstract. Aerosols at the top of the planetary boundary layer (PBL) could modify its atmospheric dynamics by redistributing the solar radiation and start to be activated to form low-level cloud at this layer. Black carbon (BC), as an aerosol component efficiently absorbing solar radiation, can introduce heating and positive radiative effects at this sensitive layer, especially in the polluted PBL over the continent. This study presents continuous measurements of detailed BC properties at a mountain site located at the top of the polluted PBL over the North China Plain, during seasons (3 and 4 weeks of data during winter and summer, respectively) with contrasting emission structure and meteorology. The pollution level was persistently influenced by local surface anthropogenic emission on a daily basis through daytime convective mixing, but the concentration was also enhanced or diluted depending on air mass direction, defined as a neutral, polluted and diluted PBL, respectively. Winter was observed to have a higher BC mass fraction (4 %–8 %) than summer (2 %–7 %). By resolving the detailed particle size-resolved mixing state of BC in optical and hygroscopic models, we found an enhanced BC mass absorption cross section (MACBC) for the polluted PBL (up to 13 m2 g−1 at λ = 550 nm), which was 5 % higher during summer than winter due to a smaller BC core size. The higher BC mass fraction in winter corresponded to a lower single-scattering albedo by 0.03–0.09 than summer, especially the lowest for the diluted winter PBL (0.86 ± 0.02). The water supersaturation (SS) required to activate half the number of BC decreased from 0.21 % ± 0.08 % to 0.1 % ± 0.03 % for the winter diluted and polluted PBL and from 0.22 % ± 0.06 % to 0.17 % ± 0.05 % for summer. Notably, at the top of the anthropogenically polluted PBL in both seasons, the enlarged BC with enhanced absorption capacity could also be efficiently droplet activated; e.g. winter (summer) BC with an MAC of 9.84 ± 1.2 (10.7 ± 1) m2 g−1 could be half activated at SS = 0.13 % ± 0.06 % (0.18 % ± 0.05 %). This BC at the top of the PBL can more directly interact with the free troposphere and be transported to a wider region, exerting important direct and indirect radiative impacts.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 15 ( 2016-08-09), p. 10045-10061
    Abstract: Abstract. The organic aerosol (OA) concentration is simulated in the Guanzhong Basin, China from 23 to 25 April 2013 utilizing the WRF-CHEM model. Two approaches are used to predict OA concentrations: (1) a traditional secondary organic aerosol (SOA) module; (2) a non-traditional SOA module including the volatility basis-set modeling method in which primary organic aerosol (POA) is assumed to be semivolatile and photochemically reactive. Generally, the spatial patterns and temporal variations of the calculated hourly near-surface ozone and fine particle matters agree well with the observations in Xi'an and surrounding areas. The model also yields reasonable distributions of daily PM2.5 and elemental carbon (EC) compared to the filter measurements at 29 sites in the basin. Filter-measured organic carbon (OC) and EC are used to evaluate OA, POA, and SOA using the OC ∕ EC ratio approach. Compared with the traditional SOA module, the non-traditional module significantly improves SOA simulations and explains about 88 % of the observed SOA concentration. Oxidation and partitioning of POA treated as semivolatile constitute the most important pathway for the SOA formation, contributing more than 75 % of the SOA concentrations in the basin. Residential emissions are the dominant anthropogenic OA source, constituting about 50 % of OA concentrations in urban and rural areas and 30 % in the background area. The OA contribution from transportation emissions decreases from 25 % in urban areas to 20 % in the background area, and the industry emission OA contribution is less than 6 %.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
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