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  • Copernicus GmbH  (47)
  • 2015-2019  (47)
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  • Copernicus GmbH  (47)
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  • 2015-2019  (47)
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  • 1
    Online Resource
    Online Resource
    Molecular distribution and stable carbon isotopic compositions of dicarboxylic acids and related SOA from biogenic sources in the summertime atmosphere of Mt. Tai in the North China Plain
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 20 ( 2018-10-19), p. 15069-15086
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 20 ( 2018-10-19), p. 15069-15086
    Abstract: Abstract. Molecular distributions and stable carbon isotopic (δ13C values) compositions of dicarboxylic acids and related secondary organic aerosols (SOA) in PM2.5 aerosols collected on a day/night basis at the summit of Mt. Tai (1534 m a.s.l.) in the summer of 2016 were analyzed to investigate the sources and photochemical aging process of organic aerosols in the forested highland region of the North China Plain. The molecular distributions of dicarboxylic acids and related SOA are characterized by the dominance of oxalic acid (C2), followed by malonic (C3), succinic (C4) and azelaic (C9) acids. The concentration ratios of C2 ∕ C4, diacid-C ∕ OC and C2 ∕ total diacids are larger in the daytime than in the nighttime, suggesting that the daytime aerosols are more photochemically aged than those in the nighttime due to the higher temperature and stronger solar radiation. Both ratios of C2 ∕ C4 (R2〉0.5) and C3 ∕ C4 (R2〉0.5) correlated strongly with the ambient temperatures, indicating that SOA in the mountaintop atmosphere are mainly derived from the photochemical oxidation of local emissions rather than long-range transport. The mass ratios of azelaic acid to adipic acid (C9 ∕ C6), azelaic acid to phthalic aid (C9 ∕ Ph) and glyoxal to methylglyoxal (Gly ∕ mGly) and the strong linear correlations of major dicarboxylic acids and related SOA (i.e., C2, C3, C4, ωC2, Pyr, Gly and mGly) with biogenic precursors (SOA tracers derived from isoprene, α/β-pinene and β-caryophyllene) further suggest that aerosols in this region are mainly originated from biogenic sources (i.e., tree emissions). C2 concentrations correlated well with aerosol pH, indicating that particle acidity favors the organic acid formation. The stable carbon isotopic compositions (δ13C) of the dicarboxylic acids are higher in the daytime than in the nighttime, with the highest value (-16.5±1.9 ‰) found for C2 and the lowest value (-25.2±2.7 ‰) found for C9. An increase in δ13C values of C2 along with increases in C2 ∕ Gly and C2 ∕ mGly ratios was observed, largely due to the isotopic fractionation effect during the precursor oxidation process.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-18-15069-2018
    DOI: 10.5194/acp-18-15069-2018-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 2
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    Changes in PM〈sub〉2.5〈/sub〉 peat combustion source profiles with atmospheric aging in an oxidation flow reactor
    Copernicus GmbH ; 2019
    In:  Atmospheric Measurement Techniques Vol. 12, No. 10 ( 2019-10-17), p. 5475-5501
    Details
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 12, No. 10 ( 2019-10-17), p. 5475-5501
    Abstract: Abstract. Smoke from laboratory chamber burning of peat fuels from Russia, Siberia, the USA (Alaska and Florida), and Malaysia representing boreal, temperate, subtropical, and tropical regions was sampled before and after passing through a potential-aerosol-mass oxidation flow reactor (PAM-OFR) to simulate intermediately aged (∼2 d) and well-aged (∼7 d) source profiles. Species abundances in PM2.5 between aged and fresh profiles varied by several orders of magnitude with two distinguishable clusters, centered around 0.1 % for reactive and ionic species and centered around 10 % for carbon. Organic carbon (OC) accounted for 58 %–85 % of PM2.5 mass in fresh profiles with low elemental carbon (EC) abundances (0.67 %–4.4 %). OC abundances decreased by 20 %–33 % for well-aged profiles, with reductions of 3 %–14 % for the volatile OC fractions (e.g., OC1 and OC2, thermally evolved at 140 and 280 ∘C). Ratios of organic matter (OM) to OC abundances increased by 12 %–19 % from intermediately aged to well-aged smoke. Ratios of ammonia (NH3) to PM2.5 decreased after intermediate aging. Well-aged NH4+ and NO3- abundances increased to 7 %–8 % of PM2.5 mass, associated with decreases in NH3, low-temperature OC, and levoglucosan abundances for Siberia, Alaska, and Everglades (Florida) peats. Elevated levoglucosan was found for Russian peats, accounting for 35 %–39 % and 20 %–25 % of PM2.5 mass for fresh and aged profiles, respectively. The water-soluble organic carbon (WSOC) fractions of PM2.5 were over 2-fold higher in fresh Russian peat (37.0±2.7 %) than in Malaysian (14.6±0.9 %) peat. While Russian peat OC emissions were largely water-soluble, Malaysian peat emissions were mostly water-insoluble, with WSOC ∕ OC ratios of 0.59–0.71 and 0.18–0.40, respectively. This study shows significant differences between fresh and aged peat combustion profiles among the four biomes that can be used to establish speciated emission inventories for atmospheric modeling and receptor model source apportionment. A sufficient aging time (∼7 d) is needed to allow gas-to-particle partitioning of semi-volatilized species, gas-phase oxidation, and particle volatilization to achieve representative source profiles for regional-scale source apportionment.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    URL: Article
    URL: Article
    DOI: 10.5194/amt-12-5475-2019
    DOI: 10.5194/amt-12-5475-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2505596-3
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  • 3
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    Typical synoptic situations and their impacts on the wintertime air pollution in the Guanzhong basin, China
    Copernicus GmbH ; 2016
    In:  Atmospheric Chemistry and Physics Vol. 16, No. 11 ( 2016-06-14), p. 7373-7387
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 11 ( 2016-06-14), p. 7373-7387
    Abstract: Abstract. Rapid industrialization and urbanization have caused severe air pollution in the Guanzhong basin, northwestern China, with heavy haze events occurring frequently in recent winters. Using the NCEP reanalysis data, the large-scale synoptic situations influencing the Guanzhong basin during wintertime of 2013 are categorized into six types to evaluate the contribution of synoptic situations to the air pollution, including “north-low”, “southwest-trough”, “southeast-high”, “transition”, “southeast-trough”, and “inland-high”. The FLEXPART model has been utilized to demonstrate the corresponding pollutant transport patterns for the typical synoptic situations in the basin. Except for “southwest-trough” and “southeast-high” (defined as favorable synoptic situations), the other four synoptic conditions (defined as unfavorable synoptic situations) generally facilitate the accumulation of air pollutants, causing heavy air pollution in the basin. In association with the measurement of PM2.5 (particulate matter with aerodynamic diameter less than 2.5 µm) in the basin, the unfavorable synoptic situations correspond to high PM2.5 mass concentrations or poor air quality and vice versa. The same analysis has also been applied to winters of 2008–2012, which shows that the basin was mainly influenced by the unfavorable synoptic situations during wintertime leading to poor air quality. The WRF-CHEM model has further been applied to simulate the selected 6 days representing the typical synoptic situations during the wintertime of 2013, and the results generally show a good agreement between the modeled distributions and variations of PM2.5 and the corresponding synoptic situations, demonstrating reasonable classification for the synoptic situations in the basin. Detailed meteorological conditions, such as temperature inversion, low-level horizontal wind speed, and planetary boundary layer, all contribute to heavy air pollution events in the basin under unfavorable synoptic conditions. Considering the proportion of occurrence of unfavorable synoptic situations during wintertime, reduction of emissions is the optimum approach to mitigate the air pollution in the Guanzhong basin.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-16-7373-2016
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2092549-9
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  • 4
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    A possible pathway for rapid growth of sulfate during haze days in China
    Copernicus GmbH ; 2017
    In:  Atmospheric Chemistry and Physics Vol. 17, No. 5 ( 2017-03-07), p. 3301-3316
    Details
    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
    URL: Article
    DOI: 10.5194/acp-17-3301-2017
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 5
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    Black carbon (BC) in a northern Tibetan mountain: effect of Kuwait fires on glaciers
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 18 ( 2018-09-27), p. 13673-13685
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 18 ( 2018-09-27), p. 13673-13685
    Abstract: Abstract. The black carbon (BC) deposition on the ice core at Muztagh Ata Mountain, northern Tibetan Plateau, was analyzed. Two sets of measurements were used in this study, which included the air samplings of BC particles during 2004–2006 and the ice core drillings of BC deposition during 1986–1994. Two numerical models were used to analyze the measured data. A global chemical transportation model (MOZART-4) was used to analyze the BC transport from the source regions, and a radiative transfer model (SNICAR) was used to study the effect of BC on snow albedo. The results show that during 1991–1992, there was a strong spike in the BC deposition at Muztagh Ata, suggesting that there was an unusual emission in the upward region during this period. This high peak of BC deposition was investigated by using the global chemical transportation model (MOZART-4). The analysis indicated that the emissions from large Kuwait fires at the end of the first Gulf War in 1991 caused this high peak of the BC concentrations and deposition (about 3–4 times higher than other years) at Muztagh Ata Mountain, suggesting that the upward BC emissions had important impacts on this remote site located on the northern Tibetan Plateau. Thus, there is a need to quantitatively estimate the effect of surrounding emissions on the BC concentrations on the northern Tibetan Plateau. In this study, a sensitivity study with four individual BC emission regions (Central Asia, Europe, the Persian Gulf, and South Asia) was conducted by using the MOZART-4 model. The result suggests that during the “normal period” (non-Kuwait fires), the largest effect was due to the Central Asia source (44 %) during the Indian monsoon period, while during the non-monsoon period, the largest effect was due to the South Asia source (34 %). The increase in radiative forcing increase (RFI) due to the deposition of BC on snow was estimated by using the radiative transfer model (SNICAR). The results show that under the fresh snow assumption, the estimated increase in RFI ranged from 0.2 to 2.5 W m−2, while under the aged snow assumption, the estimated increase in RFI ranged from 0.9 to 5.7 W m−2. During the Kuwait fires period, the RFI values increased about 2–5 times higher than in the “normal period”, suggesting a significant increase for the snow melting on the northern Tibetan Plateau due to this fire event. This result suggests that the variability of BC deposition at Muztagh Ata Mountain provides useful information to study the effect of the upward BC emissions on environmental and climate issues in the northern Tibetan Plateau. The radiative effect of BC deposition on the snow melting provides important information regarding the water resources in the region.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-18-13673-2018
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 6
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    Primary emissions versus secondary formation of fine particulate matter in the most polluted city (Shijiazhuang) in North China
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 4 ( 2019-02-21), p. 2283-2298
    Details
    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
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-2283-2019
    DOI: 10.5194/acp-19-2283-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 7
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    Impact of particle number and mass size distributions of major chemical components on particle mass scattering efficiency in urban Guangzhou in southern China
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 13 ( 2019-07-04), p. 8471-8490
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 13 ( 2019-07-04), p. 8471-8490
    Abstract: Abstract. To grasp the key factors affecting particle mass scattering efficiency (MSE), particle mass and number size distribution, PM2.5 and PM10 and their major chemical compositions, and the particle scattering coefficient (bsp) under dry conditions were measured at an urban site in Guangzhou, southern China, during 2015–2016. On an annual average, 10±2 %, 48±7 % and 42±8 % of PM10 mass were in the condensation, droplet and coarse modes, respectively, with mass mean aerodynamic diameters (MMADs) of 0.78±0.07 in the droplet mode and 4.57±0.42 µm in the coarse mode. The identified chemical species mass concentrations can explain 79±3 %, 82±6 % and 57±6 % of the total particle mass in the condensation, droplet and coarse mode, respectively. Organic matter (OM) and elemental carbon (EC) in the condensation mode, OM, (NH4)2SO4, NH4NO3, and crustal element oxides in the droplet mode, and crustal element oxides, OM, and CaSO4 in the coarse mode, were the dominant chemical species in their respective modes. The measured bsp can be reconstructed to the level of 91±10 % using Mie theory with input of the estimated chemically resolved number concentrations of NaCl, NaNO3, Na2SO4, NH4NO3, (NH4)2SO4, K2SO4, CaSO4, Ca(NO3)2, OM, EC, crustal element oxides and unidentified fraction. MSEs of particle and individual chemical species were underestimated by less than 13 % in any season based on the estimated bsp and chemical species mass concentrations. Seasonal average MSEs varied in the range of 3.5±0.1 to 3.9±0.2 m2 g−1 for fine particles (aerodynamic diameter smaller than 2.1 µm), which was mainly caused by seasonal variations in the mass fractions and MSEs of the dominant chemical species (OM, NH4NO3, (NH4)2SO4) in the droplet mode. MSEs of the dominant chemical species were determined by their lognormal size-distribution parameters, including MMADs and standard deviation (σ) in the droplet mode.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-8471-2019
    DOI: 10.5194/acp-19-8471-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 8
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    Impacts of short-term mitigation measures on PM〈sub〉2.5〈/sub〉 and radiative effects: a case study at a regional background site near Beijing, China
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 3 ( 2019-02-12), p. 1881-1899
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 3 ( 2019-02-12), p. 1881-1899
    Abstract: Abstract. Measurements at a background site near Beijing showed that pollution controls implemented during the 19th National Congress of the Communist Party of China (NCCPC) were effective in reducing PM2.5. Mass concentrations of PM2.5 and its major chemical components were 20.6 %–43.1 % lower during the NCCPC-control period compared with a non-control period, and differences were greater on days with stable meteorological conditions. A receptor model showed that PM2.5 from traffic-related emissions, biomass burning, industrial processes, and mineral dust was 38.5 %–77.8 % lower during the NCCPC-control versus non-control period, but differences in PM2.5 from coal burning were small, and secondary sources were higher during the NCCPC-control period. During one pollution episode in the non-control period, secondary sources dominated, and the WRF-Chem model showed that the Beijing–Tianjin–Hebei (BTH) region contributed 73.6 % of PM2.5 mass. A second pollution episode was linked to biomass burning, and BTH contributed 46.9 % of PM2.5 mass. Calculations based on Interagency Monitoring of Protected Visual Environments (IMPROVE) algorithms showed that organic matter was the largest contributor to light extinction during the non-control period whereas NH4NO3 was the main contributor during the NCCPC. The Tropospheric Ultraviolet and Visible radiation model showed that the average direct radiative forcing (DRF) values at the Earth's surface were −14.0 and −19.3 W m−2 during the NCCPC-control and non-control periods, respectively, and the DRF for the individual PM2.5 components were 22.7 %–46.7 % lower during the NCCPC. The information and dataset from this study will be useful for developing air pollution control strategies in the BTH region and for understanding associated aerosol radiative effects.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-1881-2019
    DOI: 10.5194/acp-19-1881-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 9
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    Mechanistic and kinetics investigations of oligomer formation from Criegee intermediate reactions with hydroxyalkyl hydroperoxides
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 6 ( 2019-04-02), p. 4075-4091
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 6 ( 2019-04-02), p. 4075-4091
    Abstract: Abstract. Although secondary organic aerosol (SOA) is a major component of PM2.5 and organic aerosol (OA) particles and therefore profoundly influences air quality, climate forcing, and human health, the mechanism of SOA formation via Criegee chemistry is poorly understood. Herein, we perform high-level theoretical calculations to study the gas-phase reaction mechanism and kinetics of four Criegee intermediate (CI) reactions with four hydroxyalkyl hydroperoxides (HHPs) for the first time. The calculated results show that the consecutive reactions of CIs with HHPs are both thermochemically and kinetically favored, and the oligomers contain CIs as chain units. The addition of an −OOH group in HHPs to the central carbon atom of CIs is identified as the most energetically favorable channel, with a barrier height strongly dependent on both CI substituent number (one or two) and position (syn- or anti-). In particular, the introduction of a methyl group into the anti-position significantly increases the rate coefficient, and a dramatic decrease is observed when the methyl group is introduced into the syn-position. These findings are expected to broaden the reactivity profile and deepen our understanding of atmospheric SOA formation processes.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-4075-2019
    DOI: 10.5194/acp-19-4075-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
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  • 10
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    Impact of the Green Light Program on haze in the North China Plain, China
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 17 ( 2019-09-04), p. 11185-11197
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 17 ( 2019-09-04), p. 11185-11197
    Abstract: Abstract. As the world's largest developing country, China has undergone ever-increasing demand for electricity during the past few decades. In 1996, China launched the Green Light Program (GLP), which became a national energy conservation activity for saving lighting electricity as well as an effective reduction of the coal consumption for power generation. Despite the great success of the GLP, its effects on haze have not been investigated and well understood. This study focused on assessing the potential coal saving induced by the improvement of luminous efficacy, the core of the GLP, and on estimating the consequent effects on the haze in the North China Plain (NCP), where a large number of power plants are located and are often engulfed by severe haze. The estimated potential coal saving induced by the GLP can reach a massive value of 120–323 million tons, accounting for 6.7 %–18.0 % of the total coal consumption for thermal power generation in China. There was a massive potential emission reduction of air pollutants from thermal power generation in the NCP, which was estimated to be 20.0–53.8 Gg for NOx and 6.9–18.7 Gg for SO2 in December 2015. The potential emission reduction induced by the GLP plays important roles in the haze formation, because the NOx and SO2 are important precursors for the formation of particles. To assess the impact of the GLP on haze, sensitivity studies were conducted by applying a regional chemical–dynamical model (WRF-CHEM). The model results suggest that in the case of lower-limit emission reduction, the PM2.5 concentration decreased by 2–5 µg m−3 in large areas of the NCP. In the case of upper-limit emission reduction, there was much more remarkable decrease in PM2.5 concentration (4–10 µg m−3). This study is a good example to illustrate that scientific innovation can induce important benefits for environment issues such as haze.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-11185-2019
    DOI: 10.5194/acp-19-11185-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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