scholarly journals Enhancement of secondary aerosol formation by reduced anthropogenic emissions during Spring Festival 2019 and enlightenment for regional PM<sub>2.5</sub> control in Beijing

2021 ◽  
Vol 21 (2) ◽  
pp. 915-926
Author(s):  
Yuying Wang ◽  
Zhanqing Li ◽  
Qiuyan Wang ◽  
Xiaoai Jin ◽  
Peng Yan ◽  
...  

Abstract. A comprehensive field experiment measuring aerosol chemical and physical properties at a suburban site in Beijing around the 2019 Spring Festival was carried out to investigate the impact of reduced anthropogenic emissions on aerosol formation. Sharply reduced sulfur dioxide (SO2) and nitrogen dioxide (NO2) concentrations during the festival holiday resulted in an unexpected increase in the surface ozone (O3) concentration caused by the strong O3-titration phenomenon. Simultaneously, the reduced anthropogenic emissions resulted in massive decreases in particle number concentration at all sizes and the mass concentrations of organics and black carbon. However, the mass concentrations of inorganics (especially sulfate) decreased weakly. Detailed analyses of the sulfur oxidation ratio and the nitrogen oxidation ratio suggest that sulfate formation during the holiday could be promoted by enhanced nocturnal aqueous-phase chemical reactions between SO2 and O3 under moderate relative humidity (RH) conditions (40 % < RH < 80 %). Daytime photochemical reactions in winter in Beijing mainly controlled nitrate formation, which was enhanced a little during the holiday. A regional analysis of air pollution patterns shows that the enhanced formation of secondary aerosols occurred throughout the entire Beijing–Tianjin–Hebei (BTH) region during the holiday, partly offsetting the decrease in particle matter with an aerodynamic diameter less than 2.5 µm. Our results highlight the necessary control of O3 formation to reduce secondary pollution in winter under current emission conditions.

2020 ◽  
Author(s):  
Yuying Wang ◽  
Zhanqing Li ◽  
Qiuyan Wang ◽  
Xiaoai Jin ◽  
Peng Yan ◽  
...  

Abstract. A comprehensive field experiment measuring aerosol chemical and physical properties at a suburban site in Beijing around the 2019 Spring Festival was carried out to investigate the impact of reduced anthropogenic emissions on aerosol formation. Sharply reduced sulfur dioxide (SO2) and nitrogen dioxide (NO2) concentrations during the festival holiday resulted in an unexpected increase in the surface ozone (O3) concentration, leading to enhancement of the atmospheric oxidation capacity. Simultaneously, the reduced anthropogenic emissions resulted in massive decreases in particle number concentration at all sizes and the mass concentrations of organics and black carbon. However, the mass concentrations of inorganics (especially sulfate) decreased weakly. Detailed analyses of the sulfur oxidation ratio and the nitrogen oxidation ratio suggest that sulfate formation during the holiday could be promoted by enhanced nocturnal aqueous-phase chemical reactions between SO2 and O3 under moderate relative humidity (RH) conditions (40 % 


2015 ◽  
Vol 12 (5) ◽  
pp. 3943-3990
Author(s):  
S. Myriokefalitakis ◽  
N. Daskalakis ◽  
N. Mihalopoulos ◽  
A. R. Baker ◽  
A. Nenes ◽  
...  

Abstract. The global atmospheric iron (Fe) cycle is parameterized in the global 3-D chemical transport model TM4-ECPL to simulate the proton- and the organic ligand-promoted mineral Fe dissolution as well as the aqueous-phase photochemical reactions between the oxidative states of Fe(III/II). Primary emissions of total (TFe) and dissolved (DFe) Fe associated with dust and combustion processes are also taken into account. TFe emissions are calculated to amount to ~35 Tg Fe yr−1. The model reasonably simulates the available Fe observations, supporting the reliability of the results of this study. Accounting for proton- and organic ligand-promoted Fe-dissolution in present-day TM4-ECPL simulations, the total Fe-dissolution is calculated to be ~0.163 Tg Fe yr−1 that accounts for up to ~50% of the calculated total DFe emissions. The atmospheric burden of DFe is calculated to be ~0.012 Tg Fe. DFe deposition presents strong spatial and temporal variability with an annual deposition flux ~0.489 Tg Fe yr−1 from which about 25% (~0.124 Tg Fe yr−1) are deposited over the ocean. The impact of air-quality on Fe deposition is studied by performing sensitivity simulations using preindustrial (year 1850), present (year 2008) and future (year 2100) emission scenarios. These simulations indicate that an increase (~2 times) in Fe-dissolution may have occurred in the past 150 years due to increasing anthropogenic emissions and thus atmospheric acidity. On the opposite, a decrease (~2 times) of Fe-dissolution is projected for near future, since atmospheric acidity is expected to be lower than present-day due to air-quality regulations of anthropogenic emissions. The organic ligand contribution to Fe dissolution shows inverse relationship to the atmospheric acidity thus its importance has decreased since the preindustrial period but is projected to increase in the future. The calculated changes also show that the atmospheric DFe supply to High-Nutrient-Low-Chlorophyll oceanic areas (HNLC) characterized by Fe scarcity, has increased (~50%) since the preindustrial period. However, the DFe deposition flux is expected to decrease (~30%) to almost preindustrial levels over the Northern Hemisphere HNLC oceanic regions in the future. Significant reductions of ~20% over the Southern Ocean and the remote tropical Pacific Ocean are also projected which can further limit the primary productivity over HNLC waters.


2013 ◽  
Vol 13 (4) ◽  
pp. 11315-11355 ◽  
Author(s):  
Y. Gao ◽  
J. S. Fu ◽  
J. B. Drake ◽  
J.-F. Lamarque ◽  
Y. Liu

Abstract. Dynamical downscaling was applied in this study to link the global climate–chemistry model Community Atmosphere Model (CAM-Chem) with the regional models: Weather Research and Forecasting (WRF) Model and Community Multi-scale Air Quality (CMAQ). Two Representative Concentration Pathway (RCP) scenarios (RCP 4.5 and RCP 8.5) were used to evaluate the climate impact on ozone concentrations in 2050s. Ozone concentrations in the lower-mid troposphere (surface to ~ 300 hPa), from mid- to high latitudes in the Northern Hemisphere (NH), show decreasing trends in RCP 4.5 between 2000s and 2050s, with the largest decrease of 4–10 ppbv occurring in the summer and the fall; and increasing trends (2–12 ppbv) in RCP 8.5 resulting from the increased methane emissions. In RCP 8.5, methane emissions increase by ~ 60% by the end of 2050s, accounting for more than 90% of ozone increases in summer and fall, and 60–80% in spring and winter. Under the RCP 4.5 scenario, in the summer when photochemical reactions are the most active, the large ozone precursor emissions reduction leads to the greatest decrease of downscaled surface ozone concentrations, ranging from 6 to 10 ppbv. However, a few major cities show ozone increases of 3 to 7 ppbv due to weakened NO titration. Under the RCP 8.5 scenario, in winter, downscaled ozone concentrations increase across nearly the entire continental US in winter, ranging from 3 to 10 ppbv due to increased methane emissions and enhanced stratosphere-troposphere exchange (STE). More intense heat waves are projected to occur by the end of 2050s in RCP 8.5, leading to more than 8 ppbv of the maximum daily 8 h daily average (MDA8) ozone during the heat wave days than other days; this indicates the dramatic impact heat waves exert on high frequency ozone events.


2021 ◽  
Author(s):  
Jiani Tan ◽  
Joshua Fu ◽  
Gregory Carmichael ◽  
Hang Su ◽  
Yafang Cheng

&lt;p&gt;This study aims at comparing the gas-to-particle conversion mechanisms adopted by regional chemical transport models (CTMs). We use the results from twelve regional CTMs from the third phase of the Model Inter-Comparison Study for Asia (MICS-Asia III). The simulations are conducted over East Asia for the whole year of 2010. The models used are WRF-CMAQ (version 4.7.1 and v5.0.2), WRF-Chem (v3.6.1 and v3.7.1), GEOS-Chem, NHM-Chem, NAQPMS and NU-WRF. Measurements from 54 EANET sites, 86 sites of the Air Pollution Indices (API) and 35 local sites, remote sensing products from AERONET and satellite data from MODIS are used to evaluate model performance on PM&lt;sub&gt;10&lt;/sub&gt;, PM&lt;sub&gt;2.5&lt;/sub&gt; and its components and aerosol optical depth (AOD). To investigate the inter-model differences in secondary aerosol formation, we compare the Sulfur Oxidation Ratio (SOR) and Nitrogen Oxidation Ratio (NOR) values by different models with observations at the EANET sites. The preliminary results show that the inter-model differences in the oxidation ratio (50%) are almost of the same magnitude as those in simulating the concentrations of particles. The results suggest large uncertainties in the gas-particle conversion process in modelling secondary aerosol formation.&lt;/p&gt;


2013 ◽  
Vol 13 (18) ◽  
pp. 9607-9621 ◽  
Author(s):  
Y. Gao ◽  
J. S. Fu ◽  
J. B. Drake ◽  
J.-F. Lamarque ◽  
Y. Liu

Abstract. Dynamical downscaling was applied in this study to link the global climate-chemistry model Community Atmosphere Model (CAM-Chem) with the regional models Weather Research and Forecasting (WRF) Model and Community Multi-scale Air Quality (CMAQ). Two representative concentration pathway (RCP) scenarios (RCP 4.5 and RCP 8.5) were used to evaluate the climate impact on ozone concentrations in the 2050s. From the CAM-Chem global simulation results, ozone concentrations in the lower to mid-troposphere (surface to ~300 hPa), from mid- to high latitudes in the Northern Hemisphere, decreases by the end of the 2050s (2057–2059) in RCP 4.5 compared to present (2001–2004), with the largest decrease of 4–10 ppbv occurring in the summer and the fall; and an increase as high as 10 ppbv in RCP 8.5 resulting from the increased methane emissions. From the regional model CMAQ simulation results, under the RCP 4.5 scenario (2057–2059), in the summer when photochemical reactions are the most active, the large ozone precursor emissions reduction leads to the greatest decrease of downscaled surface ozone concentrations compared to present (2001–2004), ranging from 6 to 10 ppbv. However, a few major cities show ozone increases of 3 to 7 ppbv due to weakened NO titration. Under the RCP 8.5 scenario, in winter, downscaled ozone concentrations increase across nearly the entire continental US in winter, ranging from 3 to 10 ppbv due to increased methane emissions. More intense heat waves are projected to occur by the end of the 2050s in RCP 8.5, leading to a 0.3 ppbv to 2.0 ppbv increase (statistically significant except in the Southeast) of the mean maximum daily 8 h daily average (MDA8) ozone in nine climate regions in the US. Moreover, the upper 95% limit of MDA8 increase reaches 0.4 ppbv to 1.5 ppbv in RCP 4.5 and 0.6 ppbv to 3.2 ppbv in RCP 8.5. The magnitude differences of increase between RCP 4.5 and 8.5 also reflect that the increase of methane emissions may favor or strengthen the effect of heat waves.


2015 ◽  
Vol 12 (13) ◽  
pp. 3973-3992 ◽  
Author(s):  
S. Myriokefalitakis ◽  
N. Daskalakis ◽  
N. Mihalopoulos ◽  
A. R. Baker ◽  
A. Nenes ◽  
...  

Abstract. The global atmospheric iron (Fe) cycle is parameterized in the global 3-D chemical transport model TM4-ECPL to simulate the proton- and the organic ligand-promoted mineral-Fe dissolution as well as the aqueous-phase photochemical reactions between the oxidative states of Fe (III/II). Primary emissions of total (TFe) and dissolved (DFe) Fe associated with dust and combustion processes are also taken into account, with TFe mineral emissions calculated to amount to ~ 35 Tg-Fe yr−1 and TFe emissions from combustion sources of ~ 2 Tg-Fe yr−1. The model reasonably simulates the available Fe observations, supporting the reliability of the results of this study. Proton- and organic ligand-promoted Fe dissolution in present-day TM4-ECPL simulations is calculated to be ~ 0.175 Tg-Fe yr−1, approximately half of the calculated total primary DFe emissions from mineral and combustion sources in the model (~ 0.322 Tg-Fe yr−1). The atmospheric burden of DFe is calculated to be ~ 0.024 Tg-Fe. DFe deposition presents strong spatial and temporal variability with an annual flux of ~ 0.496 Tg-Fe yr−1, from which about 40 % (~ 0.191 Tg-Fe yr−1) is deposited over the ocean. The impact of air quality on Fe deposition is studied by performing sensitivity simulations using preindustrial (year 1850), present (year 2008) and future (year 2100) emission scenarios. These simulations indicate that about a 3 times increase in Fe dissolution may have occurred in the past 150 years due to increasing anthropogenic emissions and thus atmospheric acidity. Air-quality regulations of anthropogenic emissions are projected to decrease atmospheric acidity in the near future, reducing to about half the dust-Fe dissolution relative to the present day. The organic ligand contribution to Fe dissolution shows an inverse relationship to the atmospheric acidity, thus its importance has decreased since the preindustrial period but is projected to increase in the future. The calculated changes also show that the atmospheric DFe supply to the globe has more than doubled since the preindustrial period due to 8-fold increases in the primary non-dust emissions and about a 3-fold increase in the dust-Fe dissolution flux. However, in the future the DFe deposition flux is expected to decrease (by about 25 %) due to reductions in the primary non-dust emissions (about 15 %) and in the dust-Fe dissolution flux (about 55 %). The present level of atmospheric deposition of DFe over the global ocean is calculated to be about 3 times higher than for 1850 emissions, and about a 30 % decrease is projected for 2100 emissions. These changes are expected to impact most on the high-nutrient–low-chlorophyll oceanic regions.


2014 ◽  
Vol 14 (3) ◽  
pp. 1397-1412 ◽  
Author(s):  
E. J. Freney ◽  
K. Sellegri ◽  
F. Canonaco ◽  
A. Colomb ◽  
A. Borbon ◽  
...  

Abstract. The MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris, using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), giving detailed information on the non-refractory submicron aerosol species. The mass concentration of black carbon (BC), measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), BC, and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (−log(NOx / NOy)). Plotting the equivalent ratios of different organic aerosol species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA) formation. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in London, Mexico City, and in New England, USA. Using the measured SOA volatile organic compounds (VOCs) species together with organic aerosol formation yields, we were able to predict ~50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA and have an impact on aerosol composition on a regional scale.


2017 ◽  
Vol 17 (22) ◽  
pp. 13869-13890 ◽  
Author(s):  
Camilla Andersson ◽  
Heléne Alpfjord ◽  
Lennart Robertson ◽  
Per Erik Karlsson ◽  
Magnuz Engardt

Abstract. We have constructed two data sets of hourly resolution reanalyzed near-surface ozone (O3) concentrations for the period 1990–2013 for Sweden. Long-term simulations from a chemistry-transport model (CTM) covering Europe were combined with hourly ozone concentration observations at Swedish and Norwegian background measurement sites using retrospective variational data analysis. The reanalysis data sets show improved performance over the original CTM when compared to independent observations. In one of the reanalyses, we included all available hourly near-surface O3 observations, whilst in the other we carefully selected time-consistent observations. Based on the second reanalysis we investigated statistical aspects of the distribution of the near-surface O3 concentrations, focusing on the linear trend over the 24-year period. We show that high near-surface O3 concentrations are decreasing and low O3 concentrations are increasing, which is reflected in observed improvement of many health and vegetation indices (apart from those with a low threshold). Using the CTM we also conducted sensitivity simulations to quantify the causes of the observed change, focusing on three factors: change in hemispheric background concentrations, meteorology and anthropogenic emissions. The rising low concentrations of near-surface O3 in Sweden are caused by a combination of all three factors, whilst the decrease in the highest O3 concentrations is caused by European O3 precursor emissions reductions. While studying the impact of anthropogenic emissions changes, we identified systematic differences in the modeled trend compared to observations that must be caused by incorrect trends in the utilized emissions inventory or by too high sensitivity of our model to emissions changes.


2017 ◽  
Author(s):  
Qiongzhen Wang ◽  
Xinyi Dong ◽  
Joshua S. Fu ◽  
Jian Xu ◽  
Congrui Deng ◽  
...  

Abstract. Near surface and vertical in situ measurements of atmospheric aerosols were conducted in Shanghai during March 19–27, 2010 to explore the transport and chemical evolution of dust aerosols in a super dust storm. An air quality model with optimized physical dust emission scheme and newly implemented dust chemistry was utilized to study the impact of dust chemistry on regional air quality. Two discontinuous dust periods were observed with one travelling over Northern China (DS1) and the other passing over the coastal regions of Eastern China (DS2). Stronger mixing extents between dust and anthropogenic emissions were found in DS2, reflecting by the higher SO2/PM10 and NO2/PM10 ratios as well as typical pollution elemental species such as As, Cd, Pb, and Zn. As a result, the concentrations of SO42− and NO3− and the ratio of Ca2+/Ca were more elevated in DS2 than in DS1 but opposite for the [NH4+]/[SO42−+NO3−] ratio, suggesting the heterogeneous reactions between calcites and acid gases were significantly promoted in DS2 due to the higher level of relative humidity and gaseous pollution precursors. Lidar observation showed a columnar effect on the vertical structure of aerosol optical properties in DS1 that dust dominantly accounted for ~80–90 % of the total aerosol extinction from near the ground to ~700 m. In contrast, the dust plumes in DS2 were refrained within lower altitudes while the extinction from spheric particles exhibited maximum at a high altitude of ~800 m. The model simulation reproduced relatively consistent results with observations that strong impacts of dust heterogeneous reactions on secondary aerosol formation occurred in areas where the anthropogenic emissions were intensive. Compared to the sulfate simulation, the nitrate formation on dust is suggested to be improved in the future modeling efforts.


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