scholarly journals Emission characteristics of CO, NOx, SO2and indications of biomass burning observed at a rural site in eastern China

Author(s):  
T. Wang
2018 ◽  
Author(s):  
Yunhua Chang ◽  
Yanlin Zhang ◽  
Chongguo Tian ◽  
Shichun Zhang ◽  
Xiaoyan Ma ◽  
...  

Abstract. Atmospheric fine-particle (PM2.5) pollution is frequently associated with the formation of particulate nitrate (pNO3−), the end product of the oxidation of NOx gases (= NO + NO2) in the upper troposphere. The application of stable nitrogen (N) (and oxygen) isotope analyses of pNO3− to constrain NOx source partitioning in the atmosphere requires the knowledge of the isotope fractionation during the reactions leading to NO3− formation. Here we determined the δ15N values of fresh pNO3− (δ15N-pNO3−) in PM2.5 at a rural site in Northern China, where atmospheric pNO3− can be attributed exclusively to biomass burning. The observed δ15N-pNO3− (12.17 ± 1.55 ‰; n = 8) was much higher than the N isotopic source signature of NOx from biomass burning (1.04 ± 4.13 ‰). The large difference between δ15N-pNO3− and δ15N-NOx (Δ(δ15N)) can be reconciled by the net N isotope effect (ԑN) associated with the gas-particle conversion from NOx to NO3−. For the biomass-burning site, a mean ԑN (≈ Δ(δ15N)) of 10.99 ± 0.74 ‰ was assessed through a newly-developed computational quantum chemistry (CQC) module. ԑN depends on the relative importance of the two dominant N isotope exchange reactions involved (NO2 reaction with OH versus hydrolysis of dinitrogen pentoxide (N2O5) with H2O), and varies between regions, and on a diurnal basis. A second, slightly higher CQC-based mean value for ԑN (15.33 ± 4.90 ‰) was estimated for an urban site with intense traffic in Eastern China, and integrated in a Bayesian isotope mixing model to make isotope-based source apportionment estimates for NOx at this site. Based on the δ15N values (10.93 ± 3.32 ‰, n = 43) of ambient pNO3− determined for the urban site, and considering the location-specific estimate for ԑN, our results reveal that the relative contribution of coal combustion and road traffic to urban NOx are 32 ± 11 % and 68 ± 11 %, respectively. This finding agrees well with a regional bottom-up emission inventory of NOx. Moreover, the variation pattern of OH contribution to ambient pNO3− formation calculated by the CQC module is consistent with that simulated by the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), further confirming the robustness of our estimates. Our investigations also show that, without the consideration of the N isotope effect during pNO3− formation, the observed δ15N-pNO3− at the study site would erroneously imply that NOx is derived almost entirely from coal combustion. Similarly, reanalysis of reported δ15N-NO3− data throughout China suggests that, nationwide, NOx emissions from coal combustion may be substantively overestimated (by > 30 %) when the N isotope fractionation during atmospheric pNO3− formation is neglected.


2019 ◽  
Author(s):  
Jun Zhang ◽  
Xinfeng Wang ◽  
Rui Li ◽  
Shuwei Dong ◽  
Yingnan Zhang ◽  
...  

Abstract. Particulate organic nitrates (PONs) constitute a substantial fraction of secondary organic aerosols and have important effects on the reactive nitrogen budget and air quality. Laboratory studies have revealed the non-negligible influence of the interactions between anthropogenic pollutants and biogenic volatile organic compounds (BVOCs) on the formation of PONs. In this study, the contents of specific PONs, including monoterpene hydroxyl nitrate (MHN215), pinene keto nitrate (PKN229), limonene di-keto nitrate (LDKN247), oleic acid keto nitrate (OAKN359), oleic acid hydroxyl nitrate (OAHN361), and pinene sulfate organic nitrate (PSON295), in fine particulate matters at four rural and urban sites in eastern China were determined, and the variation characteristics of PONs and the impacts of human activities on PONs formation were investigated. The average concentration of PONs ranged from 116 to 548 ng m−3 at these four sites. PONs were present in higher levels in summer than in other seasons, owing to the high emissions of precursors and intensive photochemical activities in this hottest season. Among the six species of PONs, MHN215 was dominant. In addition, the proportion of OAKN359 in PONs in urban areas was much higher than that in the rural site, indicating that OAKN359 primarily originated from anthropogenic activities. Slight diurnal differences existed in the concentration and secondary formation of specific PONs and varied with locations, seasons, and precursor VOCs. The measurement results showed that PONs in North China were clearly influenced by coal combustion and biomass burning, while meteorological conditions and biogenic emissions were the dominant contributing factors in the South China. Biomass burning significantly enhanced the formation of PONs due to the elevated concentrations of ozone and the released BVOCs. Sulfur dioxide (SO2) emitted from coal combustion was able to react rapidly with Criegee intermediates, the reaction products of BVOCs with ozone, to produce PONs at high rates, suggesting that there is a substantially greater role played by SO2 in organic nitrate chemistry than has previously been assumed.


2018 ◽  
Vol 18 (16) ◽  
pp. 11647-11661 ◽  
Author(s):  
Yunhua Chang ◽  
Yanlin Zhang ◽  
Chongguo Tian ◽  
Shichun Zhang ◽  
Xiaoyan Ma ◽  
...  

Abstract. Atmospheric fine-particle (PM2.5) pollution is frequently associated with the formation of particulate nitrate (pNO3−), the end product of the oxidation of NOx gases (NO + NO2) in the upper troposphere. The application of stable nitrogen (N) (and oxygen) isotope analyses of pNO3− to constrain NOx source partitioning in the atmosphere requires knowledge of the isotope fractionation during the reactions leading to nitrate formation. Here we determined the δ15N values of fresh pNO3− (δ15N–pNO3−) in PM2.5 at a rural site in northern China, where atmospheric pNO3− can be attributed exclusively to biomass burning. The observed δ15N–pNO3− (12.17±1.55 ‰; n = 8) was much higher than the N isotopic source signature of NOx from biomass burning (1.04±4.13 ‰). The large difference between δ15N–pNO3− and δ15N–NOx (Δ(δ15N)) can be reconciled by the net N isotope effect (εN) associated with the gas–particle conversion from NOx to NO3−. For the biomass burning site, a mean εN( ≈ Δ(δ15N)) of 10.99±0.74 ‰ was assessed through a newly developed computational quantum chemistry (CQC) module. εN depends on the relative importance of the two dominant N isotope exchange reactions involved (NO2 reaction with OH versus hydrolysis of dinitrogen pentoxide (N2O5) with H2O) and varies between regions and on a diurnal basis. A second, slightly higher CQC-based mean value for εN (15.33±4.90 ‰) was estimated for an urban site with intense traffic in eastern China and integrated in a Bayesian isotope mixing model to make isotope-based source apportionment estimates for NOx at this site. Based on the δ15N values (10.93±3.32 ‰; n = 43) of ambient pNO3− determined for the urban site, and considering the location-specific estimate for εN, our results reveal that the relative contribution of coal combustion and road traffic to urban NOx is 32 % ± 11 % and 68 %± 11 %, respectively. This finding agrees well with a regional bottom-up emission inventory of NOx. Moreover, the variation pattern of OH contribution to ambient pNO3− formation calculated by the CQC module is consistent with that simulated by the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), further confirming the robustness of our estimates. Our investigations also show that, without the consideration of the N isotope effect during pNO3− formation, the observed δ15N–pNO3− at the study site would erroneously imply that NOx is derived almost entirely from coal combustion. Similarly, reanalysis of reported δ15N–NO3− data throughout China and its neighboring areas suggests that NOx emissions from coal combustion may be substantively overestimated (by  > 30 %) when the N isotope fractionation during atmospheric pNO3− formation is neglected.


2018 ◽  
Author(s):  
Jian Wu ◽  
Shaofei Kong ◽  
Fangqi Wu ◽  
Yi Cheng ◽  
Shurui Zheng ◽  
...  

Abstract. Open biomass burning (OBB) has significant impacts on air pollution, climate change and potential human health. OBB has raised wide attention but with few focus on the annual variation of pollutant emission. Central and Eastern China (CEC) is one of the most polluted regions in China. This study aims to provide a state-of the-art estimation of the pollutant emissions from OBB in CEC from 2003 to 2015, by adopting the satellite observation dataset (the burned area product (MCD64Al) and the active fire product (MCD14 ML)), local biomass data (updated biomass loading data and high-resolution vegetation data) and local emission factors. Monthly emissions of pollutants were estimated and allocated into a 1 × 1 km spatial grid for four types of OBB including grassland, shrubland, forest and cropland. From 2003 to 2015, the emissions from forest, shrubland and grassland fire burning had a minor annual variation whereas the emissions from crop straw burning steadily increased. The cumulative emissions of OC, EC, CH4, NOX, NMVOC, SO2, NH3, CO, CO2 and PM2.5 were 3.64 × 103, 2.87 × 102, 3.05 × 103, 1.82 × 103, 6.4 × 103, 2.12 × 102, 4.67 × 103, 4.59 × 104, 9.39 × 105 and 4.13 × 102 Gg in these years, respectively. For cropland, corn straw burning was the largest contributor for all pollutant emissions, by 84 %–96 %. Among the forest, shrubland, grassland fire burning, forest fire burning emissions contributed the most and emissions from grassland fire was negligible due to few grass coverage in this region. High pollutant emissions were populated in the connection area of Shandong, Henan, Jiangsu and Anhui, with emission intensity higher than 100 ton per pixel, which was related to the frequent agricultural activities in these regions. The monthly emission peak of pollutants occurred in summer and autumn harvest periods including May, June, September and October, at which period ~ 50 % of pollutants were emitted for OBB. This study highlights the importance in controlling the crops straw burning emission. From December to March of the next year, the crop residue burning emissions decreased, while the emissions from forest, shrubland and grassland exhibited their highest values, leading to another small peak emissions of pollutants. Obvious regional differences in seasonal variations of OBB were observed due to different local biomass types and environmental conditions. Rural population, agricultural output, local burning habits, anthropological activities and management policies are all influence factors for OBB emissions. The successful adoption of double satellite dataset for long term estimation of pollutants from OBB with a high spatial resolution can support the assessing of OBB on regional air-quality, especially for harvest periods or dry seasons. It is also useful to evaluate the effects of annual OBB management policies in different regions.


2016 ◽  
Vol 16 (2) ◽  
pp. 1139-1160 ◽  
Author(s):  
L. Xu ◽  
L. R. Williams ◽  
D. E. Young ◽  
J. D. Allan ◽  
H. Coe ◽  
...  

Abstract. The composition of PM1 (particulate matter with diameter less than 1 µm) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between the two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer) only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS) at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have undergone similar chemical processing as rBC in the atmosphere. Although the atomic O : C ratio of OOA is substantially larger than that of solid fuel OA and hydrocarbon-like OA, these three factors have similar volatility, which is inferred from the change in mass concentration after heating at 120 °C. Finally, we discuss the relationship between the mass fraction remaining (MFR) of OA after heating in the TD and atomic O : C of OA and find that particles with a wide range of O : C could have similar MFR after heating. This analysis emphasizes the importance of understanding the distribution of volatility and O : C in bulk OA.


2018 ◽  
Vol 18 (22) ◽  
pp. 16345-16361 ◽  
Author(s):  
Derong Zhou ◽  
Ke Ding ◽  
Xin Huang ◽  
Lixia Liu ◽  
Qiang Liu ◽  
...  

Abstract. Anthropogenic fossil fuel (FF) combustion, biomass burning (BB) and desert dust are the main sources of air pollutants around the globe but are particularly intensive and important for air quality in Asia in spring. In this study, we investigate the vertical distribution, transport characteristics, source contribution and meteorological feedback of these aerosols in a unique pollution episode that occurred in eastern Asia based on various measurement data and modeling methods. In this episode, the Yangtze River Delta (YRD) in eastern China experienced persistent air pollution, dramatically changing from secondary fine particulate pollution to dust pollution in late March 2015. The Eulerian and Lagrangian models were conducted to investigate the vertical structure, transport characteristics and mechanisms of the multi-scale, multisource and multiday air pollution episode. The regional polluted continental aerosols mainly accumulated near the surface, mixed with dust aerosol downwash from the upper planetary boundary layer (PBL) and middle–lower troposphere (MLT), and further transported by large-scale cold fronts and warm conveyor belts. BB smoke from Southeast Asia was transported by westerlies around the altitude of 3 km from southern China, was further mixed with dust and FF aerosols in eastern China and experienced long-range transport over the Pacific. These pollutants could all be transported to the YRD region and cause a structure of multilayer pollution there. These pollutants could also cause significant feedback with MLT meteorology and then enhance local anthropogenic pollution. This study highlights the importance of intensive vertical measurement in eastern China and the downwind Pacific Ocean and raises the need for quantitative understanding of environmental and climate impacts of these pollution sources.


2021 ◽  
Vol 21 (4) ◽  
pp. 3181-3192
Author(s):  
Linlin Liang ◽  
Guenter Engling ◽  
Chang Liu ◽  
Wanyun Xu ◽  
Xuyan Liu ◽  
...  

Abstract. Biomass burning activities are ubiquitous in China, especially in northern China, where there is a large rural population and winter heating custom. Biomass burning tracers (i.e., levoglucosan, mannosan and potassium (K+)), as well as other chemical components, were quantified at a rural site (Gucheng, GC) in northern China from 15 October to 30 November, during a transition heating season, when the field burning of agricultural residue was becoming intense. The measured daily average concentrations of levoglucosan, mannosan and K+ in PM2.5 (particulate matter with aerodynamic diameters less than 2.5 µm) during this study were 0.79 ± 0.75, 0.03 ± 0.03 and 1.52 ± 0.62 µg m−3, respectively. Carbonaceous components and biomass burning tracers showed higher levels during nighttime than daytime, while secondary inorganic ions were enhanced during daytime. An episode with high levels of biomass burning tracers was encountered at the end of October 2016, with high levoglucosan at 4.37 µg m−3. Based on the comparison of chemical components during different biomass burning pollution periods, it appeared that biomass combustion can obviously elevate carbonaceous component levels, whereas there was essentially no effect on secondary inorganic aerosols in the ambient air. Moreover, the levoglucosan / mannosan ratios during different biomass burning pollution periods remained at high values (in the range of 18.3–24.9); however, the levoglucosan / K+ ratio was significantly elevated during the intensive biomass burning pollution period (1.67) when air temperatures were decreasing, which was substantially higher than in other biomass burning periods (averaged at 0.47).


2021 ◽  
Author(s):  
Simone M. Pieber ◽  
Dac-Loc Nguyen ◽  
Hendryk Czech ◽  
Stephan Henne ◽  
Nicolas Bukowiecki ◽  
...  

&lt;p&gt;Open biomass burning (BB) is a globally widespread phenomenon. The fires release pollutants, which are harmful for human and ecosystem health and alter the Earth's radiative balance. Yet, the impact of various types of BB on the global radiative forcing remains poorly constrained concerning greenhouse gas emissions, BB organic aerosol (OA) chemical composition and related light absorbing properties. Fire emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation-type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. Here we investigate the influence of seasonally recurring BB on trace gas concentration and air quality at the regional Global Atmosphere Watch (GAW) station Pha Din (PDI) in rural Northwestern Vietnam. PDI is located in a sparsely populated area on the top of a hill (1466 m a.s.l.) and is well suited to study the large-scale fires on the Indochinese Peninsula, whose pollution plumes are frequently transported towards the site [1]. We present continuous trace gas observations of CO&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;4&lt;/sub&gt;, CO, and O&lt;sub&gt;3&lt;/sub&gt; conducted at PDI since 2014 and interpret the data with atmospheric transport simulations. Annually recurrent large scale BB leads to hourly time-scale peaks CO mixing ratios at PDI of 1000 to 1500 ppb around every April since the start of data collection in 2014. We complement this analysis with carbonaceous PM&lt;sub&gt;2.5 &lt;/sub&gt;chemical composition analyzed during an intensive campaign in March-April 2015. This includes measurements of elemental and organic carbon (EC/OC) and more than 50 organic markers, such as sugars, PAHs, fatty acids and nitro-aromatics [2]. For the intensive campaign, we linked CO, CO&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;4&lt;/sub&gt; and O&lt;sub&gt;3&lt;/sub&gt; mixing ratios to a statistical classification of BB events, which is based on OA composition. We found increased CO and O&lt;sub&gt;3&lt;/sub&gt; levels during medium and high BB influence during the intensive campaign. A backward trajectory analysis confirmed different source regions for the identified periods based on the OA cluster. Typically, cleaner air masses arrived from northeast, i.e., mainland China and Yellow sea during the intensive campaign. The more polluted periods were characterized by trajectories from southwest, with more continental recirculation of the medium cluster, and more westerly advection for the high cluster. These findings highlight that BB activities in Northern Southeast Asia significantly enhances the regional OA loading, chemical PM&lt;sub&gt;2.5 &lt;/sub&gt;composition and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on air quality in a region of scarce data availability.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;&lt;strong&gt;REFERENCES&lt;/strong&gt;&lt;/p&gt;&lt;p&gt;[1] Bukowiecki, N. et al. Effect of Large-scale Biomass Burning on Aerosol Optical Properties at the GAW Regional Station Pha Din, Vietnam. AAQR. 19, 1172&amp;#8211;1187 (2019).&lt;/p&gt;&lt;p&gt;[2] Nguyen, D. L, et al. Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case-study in Northwestern Vietnam. ACPD., https://doi.org/10.5194/acp-2020-1027, in review, 2020.&lt;/p&gt;


2019 ◽  
Author(s):  
Marco Paglione ◽  
Stefania Gilardoni ◽  
Matteo Rinaldi ◽  
Stefano Decesari ◽  
Nicola Zanca ◽  
...  

Abstract. The Po Valley (Italy) is a well-known air quality hotspot characterized by Particulate Matter (PM) levels well above the limit set by the European Air Quality Directive and by the World Health Organization, especially during the colder season. In the framework of the Emilia-Romagna regional project SUPERSITO, the southern Po Valley submicron aerosol chemical composition was characterized by means of High-Resolution Aerosol Mass Spectroscopy (HR-AMS) with the specific aim of organic aerosol (OA) characterization and source apportionment. Eight intensive observation periods (IOPs) were carried out over four years (from 2011 to 2014) at two different sites (Bologna, BO, urban background and San Pietro Capofiume, SPC, rural background), to characterize the spatial variability and seasonality of the OA sources, with a special focus on the cold season. On the multi-year basis of the study, the AMS observations show that OA accounts for an average 45 ± 8 % (ranging 33–58 %) and 46 ± 7 % (ranging 36–50 %) of the total non-refractory submicron particle mass (PM1-NR) at the urban and at the rural site, respectively. Primary organic aerosol (POA) comprises biomass burning (23 ± 13 % of OA) and fossil fuel (12 ± 7 %) contributions with a marked seasonality in concentration. As expected, the biomass burning contribution to POA is more significant at the rural site (urban/rural concentrations ratio of 0.67), but it is also an important source of POA at the urban site during the cold season, with contributions ranging from 14 to 38 % of the total OA mass. Secondary organic aerosol (SOA) contribute to OA mass to a much larger extent than POA at both sites throughout the year (69 ± 16 % and 83 ± 16 % at urban and rural, respectively), with important implications for public health. Within the secondary fraction of OA, the measurements highlight the importance of biomass burning ageing products during the cold season, even at the urban background site. This biomass burning SOA fraction represents 14–44 % of the total OA mass in the cold season, indicating that in this region a major contribution of combustion sources to PM mass is mediated by environmental conditions and atmospheric reactivity. Among the environmental factors controlling the formation of SOA in the Po Valley, the availability of liquid water in the aerosol was shown to play a key role in the cold season. We estimate that organic fraction originating from aqueous reactions of biomass burning products (bb-aqSOA) represents 21 % (14–28 %) and 25 % (14–35 %) of the total OA mass and 44 % (32–56 %) and 61 % (21–100 %) of the SOA mass at the urban and rural sites, respectively.


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