Abstract
Abstract. Field burning of crop residue in early summer releases a large amount of pollutants into the atmosphere with significant impacts on the air quality and aerosol properties in the North China Plain (NCP). In order to investigate the influence of this regional anthropogenic activity on molecular characteristics of organic aerosols, PM2.5 filter samples were collected with a 3 h interval at a rural site of NCP from 10 to 25 June 2013 and analyzed for more than 100 organic tracer compounds, including both primary (n-alkanes, fatty acids/alcohols, sugar compounds, polycyclic aromatic hydrocarbons, hopanes, and phthalate esters) and secondary organic aerosol (SOA) tracers (phthalic acids, isoprene-, α-/β-pinene, β-caryophyllene, and toluene-derived products), as well as organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC). Total concentrations of the measured organics ranged from 177 to 6248 ng m−3 (mean 1806±1308 ng m−3) during the study period, most of which were contributed by sugar compounds, followed by fatty acids and fatty alcohols. Levoglucosan (240±288 ng m−3) was the most abundant single compound and strongly correlated with OC and WSOC, suggesting that biomass burning (BB) is an important source of summertime organic aerosols in this rural region. Based on the analysis of fire spots and backward trajectories of air masses, two representative periods were classified, which are (1) Period 1 (P1), 13 June 21:00–16 June at 15:00 CST (China Standard Time), when air masses were uniformly distributed from the southeast part of NCP, where intensive open-field biomass burning occurred; and (2) Period 2 (P2), 22 June at 12:00 to 24 June at 06:00 CST, which is representative of local emission. Nearly all the measured PM components showed much higher concentrations in P1 than in P2. Although n-alkanes, fatty acids, and fatty alcohols presented similar temporal–diurnal variations as those of levoglucosan throughout the entire period, their molecular distributions were more dominated by high molecular weight (HMW) compounds in P1, demonstrating an enhanced contribution from BB emissions. In contrast, intensive BB emission in P1 seems to have limited influence on the concentrations of polycyclic aromatic hydrocarbons (PAHs), hopanes, and phthalate esters. Both 3-hydroxyglutaric acid and β-caryophyllinic acid showed strong linearly correlations with levoglucosan (R2=0.72 and 0.80, respectively), indicating that BB is also an important source for terpene-derived SOA formation. A tracer-based method was used to estimate the distributions of biomass-burning OC, fungal-spore OC, and secondary organic carbon (SOC) derived from isoprene, α-/β-pinene, β-caryophyllene, and toluene in the different periods. The results showed that the contribution of biomass-burning OC to total OC in P1 (27.6 %) was 1.7 times that in P2 (17.1 %). However, the contribution of SOC from oxidation of the four kinds of volatile organic compounds (VOCs) increased slightly from 16.3 % in P1 to 21.1 % in P2.
Highlights
Open-field burning is still a common activity for disposal of crop residue in the rural area of the North China Plain, especially during the wheat harvest period from the end of May to the middle of June (Fu et al, 2012). These extensive emissions from regional biomass burning in the provinces of Anhui, Jiangsu, Shandong, Henan, and Hebei in NCP can cause severe air pollution on a local and regional scale
Combining with information on air mass back-trajectories, the sampling period was divided into two sections: (1) 10–18 June, when air masses were mainly transported via long distances from the southeast part of NCP, where intensive emissions from wheat straw burning occurred; (2) 19–25 June, when air masses were mostly influenced by local emissions and regional emission from biomass burning decreased dramatically (Li et al, 2018)
Given that levoglucosan is a marker of biomass-burning emissions (Simoneit et al, 1999, 2004a), and many kinds of secondary organic aerosol (SOA) could be produced in the biomass-burning plumes during the long-range transport, these results indicate that particulate water-soluble organic carbon (WSOC) in the region is mostly derived from biomass-burning activities including direct emission and secondary oxidation
Summary
Organic aerosols (OAs, i.e., the organic fraction of particles) constitute a substantial fraction (∼ 10 %–90 %) of atmospheric particles (Jimenez et al, 2009; Q. Zhang et al, 2007; Hallquist et al, 2009) and have significant effects on global and regional climate (Venkataraman et al, 2005; Kanakidou et al, 2005), air quality (Aggarwal et al, 2013; Wang et al, 2006b), human health (Lelieveld et al, 2015), and ecosystems (Tie et al, 2016). Atmospheric secondary OAs (SOAs) are produced from photochemical oxidation products of volatile organic compounds (VOCs) via gas–particle conversion processes such as nucleation, condensation and heterogeneous chemical reactions (Hallquist et al, 2009). These organic species could modify physicochemical characteristics of atmospheric aerosols such as hygroscopicity, albedo, and oxidation state (Dinar et al, 2008; Chan et al, 2005; Fu et al, 2010).
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