Relative effects of open biomass and crop straw burning on haze formation over central and eastern China: modelling study driven by constrained emissions

Author(s):  
Pengfei Li ◽  
Shaocai Yu ◽  
Yujie Wu ◽  
khalid Mehmood ◽  
Liqiang Wang ◽  
...  

<p><span>Open biomass burning (OBB) has large potential in triggering local and regional severe haze with elevated fine particulate matter (PM<sub>2.5</sub>) concentrations and could thus deteriorate ambient air quality and threaten human health. Open crop straw burning (OCSB), as a critical part of OBB, emits abundant gaseous and particulate pollutants, especially in fields with intensive agriculture, such as central and eastern China (CEC).  However, uncertainties in current OCSB and other types of OBB emissions in </span><span>chemical transport models (CTMs) lead to inaccuracies in evaluating their impacts on haze formations. Satellite retrievals provide </span><span>an alternative that can be used to simultaneously quantify emissions of </span><span>OCSB and other types of OBB, such as </span><span>the Fire INventory from NCAR version 1.5 (FINNv1.5), which, nevertheless, generally underestimate their magnitudes due to unresolved small fires. In this study, we selected June in 2014 as our study period, which exhibited a complete evolution process of OBB (from June 1 to 19) over CEC. During this period, OBB was dominated by OCSB in terms of the number of fire hotspot and associated emissions, most of which were located at Henan and Anhui with intensive enhancements from June 5 to 14. OCSB generally exhibits spatiotemporal correlation with regional haze over the central part of CEC (Henan, Anhui, Hubei, and Hunan), while other types of OBB emissions had influences on Jiangxi, Zhejiang, and Fujian. Based on these analyses, we establish a constraining method that integrates </span><span>ground-level PM<sub>2.5</sub> measurements with </span><span>a state-of-art fully coupled regional meteorological and chemical transport model (the two-way coupled WRF-CMAQ) in order to derive optimal OBB emissions based on FINNv1.5. It is demonstrated that these emissions allow the model to reproduce meteorological and chemical fields over CEC during the study period, whereas the original FINNv1.5 underestimated OBB emissions by 2 ~ 7 times, depending on specific spatiotemporal scales. The results show that OBB had substantial impacts on surface PM<sub>2.5</sub> concentrations over CEC. Most of the OBB contributions were dominated by OCSB, especially in Henan, Anhui, Hubei, and Hunan, while other types of OBB emissions also exerted influence in Jiangxi, Zhejiang, and Fujian. With the </span><span>concentration-weighted trajectory (CWT) method, potential OCSB sources leading to severe haze in Henan, Anhui, Hubei, and Hunan were pinpointed. The results show that the OCSB emissions in Henan and Anhui can cause haze not only locally but also regionally through regional transport. </span><span>Combining with meteorological analyses, we can find that surface weather patterns played a cardinal role in reshaping spatial and temporal characteristics of PM<sub>2.5</sub> concentrations. Stationary high-pressure systems over CEC enhanced local PM<sub>2.5</sub> concentrations in Henan and Anhui. Then, with the evolution of meteorological patterns, Hubei and Hunan in the low-pressure system were impacted by areas enveloped in the high-pressure system. These results suggest that policymakers should strictly undertake interprovincial joint enforcement actions to prohibit irregular OBB, especially OCSB over CEC. Constrained OBB emissions can, to a large extent, supplement estimations derived from satellite retrievals as well as reduce overestimates of bottom-up methods.</span></p>

2019 ◽  
Author(s):  
Khalid Mehmood ◽  
Yujie Wu ◽  
Liqiang Wang ◽  
Shaocai Yu ◽  
Pengfei Li ◽  
...  

Abstract. Open biomass burning (OBB) has large potential in triggering local and regional severe haze with elevated fine particulate matter (PM2.5) concentrations and could thus deteriorate ambient air quality and threaten human health. Open crop straw burning (OCSB), as a critical part of OBB, emits abundant gaseous and particulate pollutants, especially in fields with intensive agriculture, such as central and eastern China (CEC). However, there are high uncertainties in current OCSB and other types of OBB emissions that could drive chemical transport models (CTMs) to fail to evaluate their respective impacts on haze formations accurately. Satellite retrievals provide an attractive alternative that can be used to simultaneously quantify emissions of OCSB and other types of OBB, such as the Fire INventory from NCAR version 1.5 (FINNv1.5), which yet generally underestimate their magnitudes due to unresolved small fires. In this study, we selected June in 2014 as our study period, which exhibited a complete evolution process of OBB (from June 1 to 19) over CEC. During this period, OBB was dominated by OCSB in terms of the number of fire hotspot and associated emissions (74 ~ 94 %), most of which were located at Henan and Anhui (> 60 %) with intensive enhancements from June 5 to 14 (> 80 %). It is found that OCSB presented a generally strong spatiotemporal correlation with regional haze over the central part of CEC (Henan, Anhui, Hubei, and Hunan), while other types of OBB emissions had certain influences on Jiangxi, Zhejiang, and Fujian. Based on these analyses, we established a constraining method that integrates ground PM2.5 measurements with a state-of-art fully coupled regional meteorological and chemical transport model (the two-way coupled WRF-CMAQ) in order to derive optimal OBB emissions based on FINNv1.5. It is demonstrated that these emissions could allow the model to reproduce meteorological and chemical fields over CEC during the study period, whereas original FINNv1.5 underestimated OBB emissions by 2 ~ 7 times, depending on specific spatiotemporal scales. The results show that OBB had substantial impacts on surface PM2.5 concentrations over CEC. Most of OBB contributions were dominated by OCSB, especially in Henan, Anhui, Hubei, and Hunan, while other types of OBB emissions also exerted certain influence in Jiangxi, Zhejiang, and Fujian. With the concentration-weighted trajectory (CWT) method, potential OCSB sources leading to severe haze in Henan, Anhui, Hubei, and Hunan were pinpointed. The results illustrated that the OCSB emissions in Henan and Anhui can cause haze not only locally but also regionally through regional transport. Combining with meteorological analyses, we can find that surface weather patterns played a cardinal role in reshaping spatial and temporal characteristics of PM2.5 concentrations. Stationary high-pressure systems over CEC enhanced local PM2.5 concentrations in Henan and Anhui. Then, with the evolution of meteorological patterns, Hubei and Hunan in the low-pressure system were forced to receive the pollution from areas (i.e., Henan and Anhui) enveloped in the high-pressure system. These results highlight that policymakers should strictly undertake interprovincial joint enforcement actions to prohibit irregular OBB, especially OCSB over CEC. By comparison, the constrained OBB emissions can, to a large extent, not only supplement insufficient estimations derived from satellite retrievals but also reduce overestimations of bottom-up methods.


2020 ◽  
Vol 20 (4) ◽  
pp. 2419-2443 ◽  
Author(s):  
Khalid Mehmood ◽  
Yujie Wu ◽  
Liqiang Wang ◽  
Shaocai Yu ◽  
Pengfei Li ◽  
...  

Abstract. Open biomass burning (OBB) has a high potential to trigger local and regional severe haze with elevated fine particulate matter (PM2.5) concentrations and could thus deteriorate ambient air quality and threaten human health. Open crop straw burning (OCSB), as a critical part of OBB, emits abundant gaseous and particulate pollutants, especially in fields with intensive agriculture, such as in central and eastern China (CEC). This region includes nine provinces, i.e., Hubei, Anhui, Henan, Hunan, Jiangxi, Shandong, Jiangsu, Shanghai, and Fujian. The first four ones are located inland, while the others are on the eastern coast. However, uncertainties in current OCSB and other types of OBB emissions in chemical transport models (CTMs) lead to inaccuracies in evaluating their impacts on haze formations. Satellite retrievals provide an alternative that can be used to simultaneously quantify emissions of OCSB and other types of OBB, such as the Fire INventory from NCAR version 1.5 (FINNv1.5), which, nevertheless, generally underestimates their magnitudes due to unresolved small fires. In this study, we selected June 2014 as our study period, which exhibited a complete evolution process of OBB (from 1 to 19 June) over CEC. During this period, OBB was dominated by OCSB in terms of the number of fire hotspots and associated emissions (74 %–94 %), most of which were located at Henan and Anhui (> 60 %) with intensive enhancements from 5 to 14 June (> 80 %). OCSB generally exhibits a spatiotemporal correlation with regional haze over the central part of CEC (Henan, Anhui, Hubei, and Hunan), while other types of OBB emissions had influences on Jiangxi, Zhejiang, and Fujian. Based on these analyses, we establish a constraining method that integrates ground-level PM2.5 measurements with a state-of-art fully coupled regional meteorological and chemical transport model (the two-way coupled WRF-CMAQ) in order to derive optimal OBB emissions based on FINNv1.5. It is demonstrated that these emissions allow the model to reproduce meteorological and chemical fields over CEC during the study period, whereas the original FINNv1.5 underestimated OBB emissions by 2–7 times, depending on specific spatiotemporal scales. The results show that OBB had substantial impacts on surface PM2.5 concentrations over CEC. Most of the OBB contributions were dominated by OCSB, especially in Henan, Anhui, Hubei, and Hunan, while other types of OBB emissions also exerted an influence in Jiangxi, Zhejiang, and Fujian. With the concentration-weighted trajectory (CWT) method, potential OCSB sources leading to severe haze in Henan, Anhui, Hubei, and Hunan were pinpointed. The results show that the OCSB emissions in Henan and Anhui can cause haze not only locally but also regionally through regional transport. Combining with meteorological analyses, we can find that surface weather patterns played a cardinal role in reshaping spatial and temporal characteristics of PM2.5 concentrations. Stationary high-pressure systems over CEC enhanced local PM2.5 concentrations in Henan and Anhui. Then, with the evolution of meteorological patterns, Hubei and Hunan in the low-pressure system were impacted by areas (i.e., Henan and Anhui) enveloped in the high-pressure system. These results suggest that policymakers should strictly undertake interprovincial joint enforcement actions to prohibit irregular OBB, especially OCSB over CEC. Constrained OBB emissions can, to a large extent, supplement estimations derived from satellite retrievals as well as reduce overestimates of bottom-up methods.


2010 ◽  
Vol 10 (11) ◽  
pp. 27853-27891 ◽  
Author(s):  
Y. Wang ◽  
Y. Zhang ◽  
J. Hao ◽  
M. Luo

Abstract. Both observations and a 3-D chemical transport model suggest that surface ozone over populated eastern China features a significant drop in mid-summer and that the peak month differs by latitude and region. Source-receptor analysis is used to quantify the contributions of background ozone and Chinese anthropogenic emissions on this variability. Annual mean background ozone over China shows a spatial gradient from 55 ppbv in the northwest to 20 ppbv in the southeast, corresponding with changes in topography and ozone lifetime. Anthropogenic background (annual mean of 12.6 ppbv) shows distinct troughs in the summer and peaks in the spring. On the monthly-mean basis, Chinese pollution ozone (CPO) has a peak of 20–25 ppbv in June north of the Yangtze River and in October south of it, which explains the peaks of surface ozone in these months. The mid-summer drop in ozone over eastern China is driven by the decrease of background ozone (−15 ppbv). Tagged simulations suggest that this decrease is driven by reduced transport from Europe and North America, whereas ozone from Southeast Asia and Pacific Ocean exhibits a maximum in the summer over eastern China. This contrast in seasonality provides clear evidence that the seasonal switch in monsoonal wind patterns plays a significant role in determining the seasonality of background ozone over China.


2016 ◽  
Vol 50 (7) ◽  
pp. 3695-3705 ◽  
Author(s):  
Mariel D. Friberg ◽  
Xinxin Zhai ◽  
Heather A. Holmes ◽  
Howard H. Chang ◽  
Matthew J. Strickland ◽  
...  

2014 ◽  
Vol 14 (8) ◽  
pp. 4065-4077 ◽  
Author(s):  
E. Galarneau ◽  
P. A. Makar ◽  
Q. Zheng ◽  
J. Narayan ◽  
J. Zhang ◽  
...  

Abstract. The offline Eulerian AURAMS (A Unified Regional Air quality Modelling System) chemical transport model was adapted to simulate airborne concentrations of seven PAHs (polycyclic aromatic hydrocarbons): phenanthrene, anthracene, fluoranthene, pyrene, benz[a]anthracene, chrysene + triphenylene, and benzo[a]pyrene. The model was then run for the year 2002 with hourly output on a grid covering southern Canada and the continental USA with 42 km horizontal grid spacing. Model predictions were compared to ~5000 24 h-average PAH measurements from 45 sites, most of which were located in urban or industrial areas. Eight of the measurement sites also provided data on particle/gas partitioning which had been modelled using two alternative schemes. This is the first known regional modelling study for PAHs over a North American domain and the first modelling study at any scale to compare alternative particle/gas partitioning schemes against paired field measurements. The goal of the study was to provide output concentration maps of use to assessing human inhalation exposure to PAHs in ambient air. Annual average modelled total (gas + particle) concentrations were statistically indistinguishable from measured values for fluoranthene, pyrene and benz[a]anthracene whereas the model underestimated concentrations of phenanthrene, anthracene and chrysene + triphenylene. Significance for benzo[a]pyrene performance was close to the statistical threshold and depended on the particle/gas partitioning scheme employed. On a day-to-day basis, the model simulated total PAH concentrations to the correct order of magnitude the majority of the time. The model showed seasonal differences in prediction quality for volatile species which suggests that a missing emission source such as air–surface exchange should be included in future versions. Model performance differed substantially between measurement locations and the limited available evidence suggests that the model's spatial resolution was too coarse to capture the distribution of concentrations in densely populated areas. A more detailed analysis of the factors influencing modelled particle/gas partitioning is warranted based on the findings in this study.


1999 ◽  
Vol 104 (D9) ◽  
pp. 11755-11781 ◽  
Author(s):  
Eugene V. Rozanov ◽  
Vladimir A. Zubov ◽  
Michael E. Schlesinger ◽  
Fanglin Yang ◽  
Natalia G. Andronova

2012 ◽  
Vol 12 (15) ◽  
pp. 7073-7085 ◽  
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
G. Nikulin ◽  
M. L. Santee ◽  
...  

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.


2016 ◽  
Vol 9 (8) ◽  
pp. 2741-2754 ◽  
Author(s):  
Elham Baranizadeh ◽  
Benjamin N. Murphy ◽  
Jan Julin ◽  
Saeed Falahat ◽  
Carly L. Reddington ◽  
...  

Abstract. The particle formation scheme within PMCAMx-UF, a three-dimensional chemical transport model, was updated with particle formation rates for the ternary H2SO4–NH3–H2O pathway simulated by the Atmospheric Cluster Dynamics Code (ACDC) using quantum chemical input data. The model was applied over Europe for May 2008, during which the EUCAARI-LONGREX (European Aerosol Cloud Climate and Air Quality Interactions–Long-Range Experiment) campaign was carried out, providing aircraft vertical profiles of aerosol number concentrations. The updated model reproduces the observed number concentrations of particles larger than 4 nm within 1 order of magnitude throughout the atmospheric column. This agreement is encouraging considering the fact that no semi-empirical fitting was needed to obtain realistic particle formation rates. The cloud adjustment scheme for modifying the photolysis rate profiles within PMCAMx-UF was also updated with the TUV (Tropospheric Ultraviolet and Visible) radiative-transfer model. Results show that, although the effect of the new cloud adjustment scheme on total number concentrations is small, enhanced new-particle formation is predicted near cloudy regions. This is due to the enhanced radiation above and in the vicinity of the clouds, which in turn leads to higher production of sulfuric acid. The sensitivity of the results to including emissions from natural sources is also discussed.


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