Speciation of “brown” carbon in cloud water impacted by agricultural biomass burning in eastern China

2013 ◽  
Vol 118 (13) ◽  
pp. 7389-7399 ◽  
Author(s):  
Yury Desyaterik ◽  
Yele Sun ◽  
Xinhua Shen ◽  
Taehyoung Lee ◽  
Xinfeng Wang ◽  
...  
2019 ◽  
Vol 19 (17) ◽  
pp. 11213-11233 ◽  
Author(s):  
Xiaoyan Liu ◽  
Yan-Lin Zhang ◽  
Yiran Peng ◽  
Lulu Xu ◽  
Chunmao Zhu ◽  
...  

Abstract. Biomass burning can significantly impact the chemical and optical properties of carbonaceous aerosols. Here, the biomass burning impacts were studied during wintertime in a megacity of Nanjing, eastern China. The high abundance of biomass burning tracers such as levoglucosan (lev), mannosan (man), galactosan (gal) and non-sea-salt potassium (nss-K+) was found during the studied period with the concentration ranges of 22.4–1476 ng m−3, 2.1–56.2 ng m−3, 1.4–32.2 ng m−3 and 0.2–3.8 µg m−3, respectively. The significant contribution of biomass burning to water-soluble organic carbon (WSOC; 22.3±9.9 %) and organic carbon (OC; 20.9±9.3 %) was observed in this study. Backward air mass origin analysis, potential emission sensitivity of elemental carbon (EC) and MODIS fire spot information indicated that the elevations of the carbonaceous aerosols were due to the transported biomass-burning aerosols from southeastern China. The characteristic mass ratio maps of lev∕man and lev∕nss-K+ suggested that the biomass fuels were mainly crop residuals. Furthermore, the strong correlation (p < 0.01) between biomass burning tracers (such as lev) and light absorption coefficient (babs) for water-soluble brown carbon (BrC) revealed that biomass burning emissions played a significant role in the light-absorption properties of carbonaceous aerosols. The solar energy absorption due to water-soluble brown carbon and EC was estimated by a calculation based on measured light-absorbing parameters and a simulation based on a radiative transfer model (RRTMG_SW). The solar energy absorption of water-soluble BrC in short wavelengths (300–400 nm) was 0.8±0.4 (0.2–2.3) W m−2 (figures in parentheses represent the variation range of each parameter) from the calculation and 1.2±0.5 (0.3–1.9) W m−2 from the RRTMG_SW model. The absorption capacity of water-soluble BrC accounted for about 20 %–30 % of the total absorption of EC aerosols. The solar energy absorption of water-soluble BrC due to biomass burning was estimated as 0.2±0.1 (0.0–0.9) W m−2, considering the biomass burning contribution to carbonaceous aerosols. Potential source contribution function model simulations showed that the solar energy absorption induced by water-soluble BrC and EC aerosols was mostly due to the regionally transported carbonaceous aerosols from source regions such as southeastern China. Our results illustrate the importance of the absorbing water-soluble brown carbon aerosols in trapping additional solar energy in the low-level atmosphere, heating the surface and inhibiting the energy from escaping the atmosphere.


2019 ◽  
Vol 19 (19) ◽  
pp. 12221-12234 ◽  
Author(s):  
Yunhua Chang ◽  
Yan-Lin Zhang ◽  
Jiarong Li ◽  
Chongguo Tian ◽  
Linlin Song ◽  
...  

Abstract. Predicting tropospheric cloud formation and subsequent nutrient deposition relies on understanding the sources and processes affecting aerosol constituents of the atmosphere that are preserved in cloud water. However, this challenge is difficult to address quantitatively based on the sole use of bulk chemical properties. Nitrogenous aerosols, mainly ammonium (NH4+) and nitrate (NO3-), play a particularly important role in tropospheric cloud formation. While dry and wet (mainly rainfall) deposition of NH4+ and NO3- are regularly assessed, cloud water deposition is often underappreciated. Here we collected cloud water samples at the summit of Mt. Tai (1545 m above sea level) in eastern China during a long-lasting biomass burning (BB) event and simultaneously measured for the first time the isotopic compositions (mean ±1σ) of cloud water nitrogen species (δ15N-NH4+ = −6.53 ‰ ± 4.96 ‰, δ15N-NO3- = −2.35 ‰ ± 2.00 ‰, δ18O-NO3- = 57.80 ‰ ± 4.23 ‰), allowing insights into their sources and potential transformation mechanism within the clouds. Large contributions of BB to the cloud water NH4+ (32.9 % ± 4.6 %) and NO3- (28.2 % ± 2.7 %) inventories were confirmed through a Bayesian isotopic mixing model, coupled with our newly developed computational quantum chemistry module. Despite an overall reduction in total anthropogenic NOx emission due to effective emission control actions and stricter emission standards for vehicles, the observed cloud δ15N-NO3- values suggest that NOx emissions from transportation may have exceeded emissions from coal combustion. δ18O-NO3- values imply that the reaction of OH with NO2 is the dominant pathway of NO3- formation (57 % ± 11 %), yet the contribution of heterogeneous hydrolysis of dinitrogen pentoxide was almost as important (43 % ± 11 %). Although the limited sample set used here results in a relatively large uncertainty with regards to the origin of cloud-associated nitrogen deposition, the high concentrations of inorganic nitrogen imply that clouds represent an important source of nitrogen, especially for nitrogen-limited ecosystems in remote areas. Further simultaneous and long-term sampling of aerosol, rainfall, and cloud water is vital for understanding the anthropogenic influence on nitrogen deposition in the study region.


2017 ◽  
Vol 122 (4) ◽  
pp. 2304-2324 ◽  
Author(s):  
Yonghua Wu ◽  
Yong Han ◽  
Apostolos Voulgarakis ◽  
Tijian Wang ◽  
Mengmeng Li ◽  
...  

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.


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.


Atmosphere ◽  
2017 ◽  
Vol 8 (12) ◽  
pp. 88 ◽  
Author(s):  
Hongmei Zhao ◽  
Xuelei Zhang ◽  
Shichun Zhang ◽  
Weiwei Chen ◽  
Daniel Tong ◽  
...  

2020 ◽  
Vol 20 (10) ◽  
pp. 6177-6191 ◽  
Author(s):  
Rong Tang ◽  
Xin Huang ◽  
Derong Zhou ◽  
Aijun Ding

Abstract. Biomass burning has attracted great concerns for the emission of particular matters and trace gases, which substantially impacts air quality, human health, and climate change. Meanwhile, large areas of dark char, carbon residue produced in incomplete combustion, can stick to the surface over fire-prone areas after open burning, leading to a sharp drop in surface albedo, so-called “surface darkening”. However, exploration into such surface albedo declines and the radiative and meteorological effects is still fairly limited. As one of the highest-yield agricultural areas, eastern China features intensive straw burning every early summer, the harvest season for winter wheat, which was particularly strong in 2012. Satellite retrievals show that the surface albedo decline over fire-prone areas was significant, especially in the near-infrared band, which can reach −0.16. Observational evidence of abnormal surface warming was found by comparing radiosonde and reanalysis data. Most sites around intensive burned scars show a positive deviation, extending especially in the downwind area. Comparisons between “pre-fire” and “post-fire” from 2007 to 2015 indicated a larger temperature bias of the forecast during the post-fire stage. The signal becomes more apparent between 14:00 and 20:00 LT. Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) simulations suggest that including surface darkening can decrease model bias and well-captured temperature variation after burning at sites in fire areas and their adjacent area. This work highlights the importance of biomass burning induced albedo change in weather forecast and regional climate.


2020 ◽  
Vol 20 (4) ◽  
pp. 2017-2030 ◽  
Author(s):  
Can Wu ◽  
Gehui Wang ◽  
Jin Li ◽  
Jianjun Li ◽  
Cong Cao ◽  
...  

Abstract. To investigate the characteristics of atmospheric brown carbon (BrC) in the semiarid region of East Asia, PM2.5 and size-resolved particles in the urban atmosphere of Xi'an, inland China, during the winter and summer of 2017 were collected and analyzed for optical properties and chemical compositions. Methanol extracts (MeOH extracts) were more light-absorbing than water extracts (H2O extracts) in the optical wavelength of 300–600 nm and well correlated with nitrophenols, polycyclic aromatic hydrocarbons (PAHs) and oxygenated PAHs (r > 0.78). The light absorptions (absλ=365 nm) of H2O extracts and MeOH extracts in winter were 28±16 and 49±32 M m−1, respectively, which are about 10 times higher than those in summer, mainly due to the enhanced emissions from biomass burning for house heating. Water-extracted BrC predominately occurred in the fine mode (< 2.1 µm) during winter and summer, accounting for 81 % and 65 % of the total absorption of BrC, respectively. The light absorption and stable carbon isotope composition measurements showed an increasing ratio of absλ=365 nm-MeOH to absλ=550 nm-EC along with an enrichment of 13C in PM2.5 during the haze development, indicating an accumulation of secondarily formed BrC (e.g., nitrophenols) in the aerosol aging process. Positive matrix factorization (PMF) analysis showed that biomass burning, fossil fuel combustion, secondary formation, and fugitive dust are the major sources of BrC in the city, accounting for 55 %, 19 %, 16 %, and 10 % of the total BrC of PM2.5, respectively.


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