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  • 1
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    Significant increase of summertime ozone at Mount Tai in Central Eastern China
    Copernicus GmbH ; 2016
    In:  Atmospheric Chemistry and Physics Vol. 16, No. 16 ( 2016-08-26), p. 10637-10650
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 16 ( 2016-08-26), p. 10637-10650
    Abstract: Abstract. Tropospheric ozone (O3) is a trace gas playing important roles in atmospheric chemistry, air quality and climate change. In contrast to North America and Europe, long-term measurements of surface O3 are very limited in China. We compile available O3 observations at Mt. Tai – the highest mountain over the North China Plain – during 2003–2015 and analyze the decadal change of O3 and its sources. A linear regression analysis shows that summertime O3 measured at Mt. Tai has increased significantly by 1.7 ppbv yr−1 for June and 2.1 ppbv yr−1 for the July–August average. The observed increase is supported by a global chemistry-climate model hindcast (GFDL-AM3) with O3 precursor emissions varying from year to year over 1980–2014. Analysis of satellite data indicates that the O3 increase was mainly due to the increased emissions of O3 precursors, in particular volatile organic compounds (VOCs). An important finding is that the emissions of nitrogen oxides (NOx) have diminished since 2011, but the increase of VOCs appears to have enhanced the ozone production efficiency and contributed to the observed O3 increase in central eastern China. We present evidence that controlling NOx alone, in the absence of VOC controls, is not sufficient to reduce regional O3 levels in North China in a short period.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-16-10637-2016
    DOI: 10.5194/acp-16-10637-2016-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
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  • 2
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    Volatility of mixed atmospheric humic-like substances and ammonium sulfate particles
    Copernicus GmbH ; 2017
    In:  Atmospheric Chemistry and Physics Vol. 17, No. 5 ( 2017-03-15), p. 3659-3672
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 5 ( 2017-03-15), p. 3659-3672
    Abstract: Abstract. The volatility of organic aerosols remains poorly understood due to the complexity of speciation and multiphase processes. In this study, we extracted humic-like substances (HULIS) from four atmospheric aerosol samples collected at the SORPES station in Nanjing, eastern China, and investigated the volatility behavior of particles at different sizes using a Volatility Tandem Differential Mobility Analyzer (VTDMA). In spite of the large differences in particle mass concentrations, the extracted HULIS from the four samples all revealed very high-oxidation states (O : C 〉 0.95), indicating secondary formation as the major source of HULIS in Yangtze River Delta (YRD). An overall low volatility was identified for the extracted HULIS, with the volume fraction remaining (VFR) higher than 55 % for all the regenerated HULIS particles at the temperature of 280 °C. A kinetic mass transfer model was applied to the thermodenuder (TD) data to interpret the observed evaporation pattern of HULIS, and to derive the mass fractions of semi-volatile (SVOC), low-volatility (LVOC) and extremely low-volatility components (ELVOC). The results showed that LVOC and ELVOC dominated (more than 80 %) the total volume of HULIS. Atomizing processes led to a size-dependent evaporation of regenerated HULIS particles, and resulted in more ELVOC in smaller particles. In order to understand the role of interaction between inorganic salts and atmospheric organic mixtures in the volatility of an organic aerosol, the evaporation of mixed samples of ammonium sulfate (AS) and HULIS was measured. The results showed a significant but nonlinear influence of ammonium sulfate on the volatility of HULIS. The estimated fraction of ELVOC in the organic part of the largest particles (145 nm) increased from 26 %, in pure HULIS samples, to 93 % in 1 : 3 (mass ratio of HULIS : AS) mixed samples, to 45 % in 2 : 2 mixed samples, and to 70 % in 3 : 1 mixed samples, suggesting that the interaction with ammonium sulfate tends to decrease the volatility of atmospheric organic compounds. Our results demonstrate that HULIS are important low-volatility, or even extremely low-volatility, compounds in the organic-aerosol phase. As important formation pathways of atmospheric HULIS, multiphase processes, including oxidation, oligomerization, polymerization and interaction with inorganic salts, are indicated to be important sources of low-volatility and extremely low-volatility species of organic aerosols.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-17-3659-2017
    DOI: 10.5194/acp-17-3659-2017-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 3
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    Two-way coupled meteorology and air quality models in Asia: a systematic review and meta-analysis of impacts of aerosol feedbacks on meteorology and air quality
    Copernicus GmbH ; 2022
    In:  Atmospheric Chemistry and Physics Vol. 22, No. 8 ( 2022-04-22), p. 5265-5329
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 8 ( 2022-04-22), p. 5265-5329
    Abstract: Abstract. Atmospheric aerosols can exert an influence on meteorology and air quality through aerosol–radiation interaction (ARI) and aerosol–cloud interaction (ACI), and this two-way feedback has been studied by applying two-way coupled meteorology and air quality models. As one of the regions with the highest aerosol loading in the world, Asia has attracted many researchers to investigate the aerosol effects with several two-way coupled models (WRF-Chem, WRF-CMAQ, GRAPES-CUACE, WRF-NAQPMS, and GATOR-GCMOM) over the last decade. This paper attempts to offer a bibliographic analysis regarding the current status of applications of two-way coupled models in Asia, related research focuses, model performances, and the effects of ARI and/or ACI on meteorology and air quality. There were a total of 160 peer-reviewed articles published between 2010 and 2019 in Asia meeting the inclusion criteria, with more than 79 % of papers involving the WRF-Chem model. The number of relevant publications has an upward trend annually, and East Asia, India, and China, as well as the North China Plain are the most studied areas. The effects of ARI and both ARI and ACI induced by natural aerosols (particularly mineral dust) and anthropogenic aerosols (bulk aerosols, different chemical compositions, and aerosols from different sources) are widely investigated in Asia. Through the meta-analysis of surface meteorological and air quality variables simulated by two-way coupled models, the model performance affected by aerosol feedbacks depends on different variables, simulation time lengths, selection of two-way coupled models, and study areas. Future research perspectives with respect to the development, improvement, application, and evaluation of two-way coupled meteorology and air quality models are proposed.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-22-5265-2022
    DOI: 10.5194/acp-22-5265-2022-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
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  • 4
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    Evaluating wildfire emissions projection methods in comparisons of simulated and observed air quality
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 23 ( 2019-12-13), p. 15157-15181
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 23 ( 2019-12-13), p. 15157-15181
    Abstract: Abstract. Climate warming has been implicated as a major driver of recent catastrophic wildfires worldwide but analyses of regional differences in US wildfires show that socioeconomic factors also play a large role. We previously leveraged statistical projections of annual areas burned (AAB) over the fast-growing southeastern US that include both climate and socioeconomic changes from 2011 to 2060 and developed wildfire emissions estimates over the region at 12 km × 12 km resolution to enable air quality (AQ) impact assessments for 2010 and selected future years. These estimates employed two AAB datasets, one using statistical downscaling (“statistical d-s”) and another using dynamical downscaling (“dynamical d-s”) of climate inputs from the same climate realization. This paper evaluates these wildfire emissions estimates against the U.S. National Emissions Inventory (NEI) as a benchmark in contemporary (2010) simulations with the Community Multiscale Air Quality (CMAQ) model and against network observations for ozone and particulate matter below 2.5 µm in diameter (PM2.5). We hypothesize that our emissions estimates will yield model results that meet acceptable performance criteria and are comparable to those using the NEI. The three simulations, which differ only in wildfire emissions, compare closely, with differences in ozone and PM2.5 below 1 % and 8 %, respectively, but have much larger maximum mean fractional biases (MFBs) against observations (25 % and 51 %, respectively). The largest biases for ozone are in the fire-free winter, indicating that modeling uncertainties other than wildfire emissions are mainly responsible. Statistical d-s, with the largest AAB domain-wide, is 7 % more positively biased and 4 % less negatively biased in PM2.5 on average than the other two cases, while dynamical d-s and the NEI differ only by 2 %–3 % partly because of their equally large summertime PM2.5 underpredictions. Primary species (elemental carbon and ammonium from ammonia) have good-to-acceptable results, especially for the downscaling cases, providing confidence in our emissions estimation methodology. Compensating biases in sulfate (positive) and in organic carbon and dust (negative) lead to acceptable PM2.5 performance to varying degrees (MFB between −14 % and 51 %) in all simulations. As these species are driven by secondary chemistry or non-wildfire sources, their production pathways can be fruitful avenues for CMAQ improvements. Overall, the downscaling methods match and sometimes exceed the NEI in simulating current wildfire AQ impacts, while enabling such assessments much farther into the future.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-15157-2019
    DOI: 10.5194/acp-19-15157-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 5
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    The effect of COVID-19 restrictions on atmospheric new particle formation in Beijing
    Copernicus GmbH ; 2022
    In:  Atmospheric Chemistry and Physics Vol. 22, No. 18 ( 2022-09-19), p. 12207-12220
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 18 ( 2022-09-19), p. 12207-12220
    Abstract: Abstract. During the COVID-19 lockdown, the dramatic reduction of anthropogenic emissions provided a unique opportunity to investigate the effects of reduced anthropogenic activity and primary emissions on atmospheric chemical processes and the consequent formation of secondary pollutants. Here, we utilize comprehensive observations to examine the response of atmospheric new particle formation (NPF) to the changes in the atmospheric chemical cocktail. We find that the main clustering process was unaffected by the drastically reduced traffic emissions, and the formation rate of 1.5 nm particles remained unaltered. However, particle survival probability was enhanced due to an increased particle growth rate (GR) during the lockdown period, explaining the enhanced NPF activity in earlier studies. For GR at 1.5–3 nm, sulfuric acid (SA) was the main contributor at high temperatures, whilst there were unaccounted contributing vapors at low temperatures. For GR at 3–7 and 7–15 nm, oxygenated organic molecules (OOMs) played a major role. Surprisingly, OOM composition and volatility were insensitive to the large change of atmospheric NOx concentration; instead the associated high particle growth rates and high OOM concentration during the lockdown period were mostly caused by the enhanced atmospheric oxidative capacity. Overall, our findings suggest a limited role of traffic emissions in NPF.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-22-12207-2022
    DOI: 10.5194/acp-22-12207-2022-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
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  • 6
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    Los Angeles megacity: a high-resolution land–atmosphere modelling system for urban CO〈sub〉2〈/sub〉 emissions
    Copernicus GmbH ; 2016
    In:  Atmospheric Chemistry and Physics Vol. 16, No. 14 ( 2016-07-22), p. 9019-9045
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 14 ( 2016-07-22), p. 9019-9045
    Abstract: Abstract. Megacities are major sources of anthropogenic fossil fuel CO2 (FFCO2) emissions. The spatial extents of these large urban systems cover areas of 10 000 km2 or more with complex topography and changing landscapes. We present a high-resolution land–atmosphere modelling system for urban CO2 emissions over the Los Angeles (LA) megacity area. The Weather Research and Forecasting (WRF)-Chem model was coupled to a very high-resolution FFCO2 emission product, Hestia-LA, to simulate atmospheric CO2 concentrations across the LA megacity at spatial resolutions as fine as  ∼  1 km. We evaluated multiple WRF configurations, selecting one that minimized errors in wind speed, wind direction, and boundary layer height as evaluated by its performance against meteorological data collected during the CalNex-LA campaign (May–June 2010). Our results show no significant difference between moderate-resolution (4 km) and high-resolution (1.3 km) simulations when evaluated against surface meteorological data, but the high-resolution configurations better resolved planetary boundary layer heights and vertical gradients in the horizontal mean winds. We coupled our WRF configuration with the Vulcan 2.2 (10 km resolution) and Hestia-LA (1.3 km resolution) fossil fuel CO2 emission products to evaluate the impact of the spatial resolution of the CO2 emission products and the meteorological transport model on the representation of spatiotemporal variability in simulated atmospheric CO2 concentrations. We find that high spatial resolution in the fossil fuel CO2 emissions is more important than in the atmospheric model to capture CO2 concentration variability across the LA megacity. Finally, we present a novel approach that employs simultaneous correlations of the simulated atmospheric CO2 fields to qualitatively evaluate the greenhouse gas measurement network over the LA megacity. Spatial correlations in the atmospheric CO2 fields reflect the coverage of individual measurement sites when a statistically significant number of sites observe emissions from a specific source or location. We conclude that elevated atmospheric CO2 concentrations over the LA megacity are composed of multiple fine-scale plumes rather than a single homogenous urban dome. Furthermore, we conclude that FFCO2 emissions monitoring in the LA megacity requires FFCO2 emissions modelling with  ∼  1 km resolution because coarser-resolution emissions modelling tends to overestimate the observational constraints on the emissions estimates.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-16-9019-2016
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
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  • 7
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    Significant reduction of PM〈sub〉2.5〈/sub〉 in eastern China due to regional-scale emission control: evidence from SORPES in 2011–2018
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 18 ( 2019-09-24), p. 11791-11801
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 18 ( 2019-09-24), p. 11791-11801
    Abstract: Abstract. Haze pollution caused by PM2.5 is the largest air quality concern in China in recent years. Long-term measurements of PM2.5 and the precursors and chemical speciation are crucially important for evaluating the efficiency of emission control, understanding formation and transport of PM2.5 associated with the change of meteorology, and accessing the impact of human activities on regional climate change. Here we reported long-term continuous measurements of PM2.5, chemical components, and their precursors at a regional background station, the Station for Observing Regional Processes of the Earth System (SORPES), in Nanjing, eastern China, since 2011. We found that PM2.5 at the station has experienced a substantial decrease (−9.1 % yr−1), accompanied by even a very significant reduction of SO2 (−16.7 % yr−1), since the national “Ten Measures of Air” took action in 2013. Control of open biomass burning and fossil-fuel combustion are the two dominant factors that influence the PM2.5 reduction in early summer and winter, respectively. In the cold season (November–January), the nitrate fraction was significantly increased, especially when air masses were transported from the north. More NH3 available from a substantial reduction of SO2 and increased oxidization capacity are the main factors for the enhanced nitrate formation. The changes of year-to-year meteorology have contributed to 24 % of the PM2.5 decrease since 2013. This study highlights several important implications on air pollution control policy in China.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-11791-2019
    DOI: 10.5194/acp-19-11791-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 8
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    Impacts of black carbon on the formation of advection–radiation fog during a haze pollution episode in eastern China
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 11 ( 2019-06-12), p. 7759-7774
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 11 ( 2019-06-12), p. 7759-7774
    Abstract: Abstract. Aerosols can not only participate in fog formation by acting as condensation nuclei of droplets but also modify the meteorological conditions such as air temperature and moisture, planetary boundary layer height (PBLH) and regional circulation during haze events. The impact of aerosols on fog formation, yet to be revealed, can be critical in understanding and predicting fog–haze events. In this study, we used the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to investigate a heavy fog event during a multiday intense haze pollution episode in early December 2013 in the Yangtze River Delta (YRD) region in eastern China. Using the WRF-Chem model, we conducted four parallel numerical experiments to evaluate the roles of aerosol–radiation interaction (ARI), aerosol–cloud interaction (ACI), black carbon (BC) and non-BC aerosols in the formation and maintenance of the heavy fog event. We find that only when the aerosols' feedback processes are considered can the model capture the haze pollution and the fog event well. And the effects of ARI during the fog–haze episode in early December 2013 played a dominant role, while the effects of ACI were negligible. Furthermore, our analyses show that BC was more important in inducing fog formation in the YRD region on 7 December than non-BC aerosols. The dome effect of BC leads to an increase in air moisture over the sea by reducing PBLH and weakening vertical mixing, thereby confining more water vapor to the near-surface layer. The strengthened daytime onshore flow by a cyclonic wind anomaly, induced by contrast temperature perturbation over land and sea, transported moister air to the YRD region, where the suppressed PBLH and weakened daytime vertical mixing maintained the high moisture level. Then heavy fog formed due to the surface cooling at night. This study highlights the importance of anthropogenic emissions in the formation of advection–radiation fog in the polluted coastal areas.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-7759-2019
    DOI: 10.5194/acp-19-7759-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 9
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    Diverse mixing states of amine-containing single particles in Nanjing, China
    Copernicus GmbH ; 2021
    In:  Atmospheric Chemistry and Physics Vol. 21, No. 23 ( 2021-12-08), p. 17953-17967
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 23 ( 2021-12-08), p. 17953-17967
    Abstract: Abstract. The mixing states of particulate amines with different chemical components are of great significance in studying the formation and evolution processes of amine-containing particles. In this work, the mixing states of single particles containing trimethylamine (TMA) and diethylamine (DEA) are investigated using a high-performance single-particle aerosol mass spectrometer located in Nanjing, China, in September 2019. TMA- and DEA-containing particles accounted for 22.8 % and 5.5 % of the total detected single particles, respectively. The particle count and abundance of the TMA-containing particles in the total particles notably increased with enhancement of ambient relative humidity (RH), while the DEA-containing particles showed no increase under a high RH. This result suggested the important role of RH in the formation of particulate TMA. Significant enrichments of secondary organic species, including 43C2H3O+, 26CN−, 42CNO−, 73C3H5O2-, and 89HC2O4-, were found in DEA-containing particles, indicating that DEA-containing particles were closely associated with the aging of secondary organics. The differential mass spectra of the DEA-containing particles showed a much higher abundance of nitrate and organic nitrogen species during the nighttime than during the daytime, which suggested that the nighttime production of particulate DEA might be associated with reactions of gaseous DEA with HNO3 and/or particulate nitrate. In the daytime, the decrease in DEA-containing particles was observed with the enrichment of oxalate and glyoxylate, which suggested a substantial impact of photochemistry on the aging process of DEA-containing particles. Furthermore, more than 80 % of TMA- and DEA-containing particles internally mixed with nitrate, while the abundance of sulfate was higher in the DEA-containing particles (79.3 %) than in the TMA-containing particles (55.3 %). This suggested that particulate DEA existed both as nitrate and sulfate aminium salts, while the particulate TMA primarily presented as nitrate aminium salt. The different mixing states of the TMA- and DEA-containing particles suggested their different formation processes and various influencing factors, which are difficult to investigate using bulk analysis. These results provide insights into the discriminated fates of organics during the evolution process in aerosols, which helps to illustrate the behavior of secondary organic aerosols.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-21-17953-2021
    DOI: 10.5194/acp-21-17953-2021-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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