Caiqing Yan

Regionally-Varying Combustion Sources of the January 2013 Severe Haze Events over Eastern China

Thick haze plagued northeastern China in January 2013, strongly affecting both regional climate and human respiratory health. Here, we present dual carbon isotope constrained (Δ(14)C and δ(13)C) source apportionment for combustion-derived black carbon aerosol (BC) for three key hotspot regions (megacities): North China Plain (NCP, Beijing), the Yangtze River Delta (YRD, Shanghai), and the Pearl River Delta (PRD, Guangzhou) for January 2013. BC, here quantified as elemental carbon (EC), is one of the most health-detrimental components of PM2.5 and a strong climate warming agent. The results show that these severe haze events were equally affected (∼ 30%) by biomass combustion in all three regions, whereas the sources of the dominant fossil fuel component was dramatically different between north and south. In the NCP region, coal combustion accounted for 66% (46-74%, 95% C.I.) of the EC, whereas, in the YRD and PRD regions, liquid fossil fuel combustion (e.g., traffic) stood for 46% (18-66%) and 58% (38-68%), respectively. Taken together, these findings suggest the need for a regionally-specific description of BC sources in climate models and regionally-tailored mitigation to combat severe air pollution events in East Asia.

Chemical composition of PM2.5 from two tunnels with different vehicular fleet characteristics.

The chemical compositions of PM2.5 including OC, EC, water soluble ions, elements, and organic components such as polycyclic aromatic hydrocarbons (PAHs), hopanes, and steranes, emitted in Wuzushan (WZS) and Kuixinglou (KXL) tunnels were determined. WZS tunnel is a major route for diesel vehicles traveling, while KXL tunnel has limited to diesel vehicles. The results showed that the proportions of the different constituents of PM2.5 in the Wuzushan (WZS) tunnel were OC (27.7%), EC (32.1%), elements (13.9%), and water soluble ions (9.2%). Whereas the chemical profile of PM2.5 in the Kuixinglou (KXL) tunnel was OC (17.7%), EC (10.4%), elements (8.90%), and water soluble ions (8.87%). The emission factors (EFs) of PM2.5 and proportions of SO4(2-) and Pb were decreased by vehicle emission standards and fuel quality policy in China, and the higher molecular weight PAHs (4+5+6 rings) were more abundant than the lower molecular weight PAHs (2+3 rings) in the two tunnels. The proportions of 17A(H)-21B(H)-30-Norhopane and 17A(H)-21B(H)-Hopane in the hopane and sterane were not dependent on the vehicles types. In addition, specific composition profiles for PM2.5 from gasoline-fueled vehicles (GV) and diesel-fueled vehicles (DV) emissions were drafted, which indicated that OC (0.974mg·veh(-1)·km(-1)) was the most abundant component in PM2.5, followed by Fe, Cl(-), and Mg for GV. The relative proportions of the different constituents in the PM2.5 for DV were EC (35.9%), OC (27.2%), elements (12.8%), and water soluble ions (11.7%). Both the PM2.5 EFs and EC proportions in DV were higher than those in GV, and the HMW PAHs were the dominant PAHs for both GV and DV. The PM2.5 emissions from the vehicles in Yantai were 581±513tons to 1353±1197tons for GV, and 19,627±2477tons to 23,042±2887tons for DV, respectively.

Important fossil source contribution to brown carbon in Beijing during winter

Organic aerosol (OA) constitutes a substantial fraction of fine particles and affects both human health and climate. It is becoming clear that OA absorbs light substantially (hence termed Brown Carbon, BrC), adding uncertainties to global aerosol radiative forcing estimations. The few current radiative-transfer and chemical-transport models that include BrC primarily consider sources from biogenic and biomass combustion. However, radiocarbon fingerprinting here clearly indicates that light-absorbing organic carbon in winter Beijing, the capital of China, is mainly due to fossil sources, which contribute the largest part to organic carbon (OC, 67 ± 3%) and its sub-constituents (water-soluble OC, WSOC: 54 ± 4%, and water-insoluble OC, WIOC: 73 ± 3%). The dual-isotope (Δ14C/δ13C) signatures, organic molecular tracers and Beijing-tailored emission inventory identify that this fossil source is primarily from coal combustion activities in winter, especially from the residential sector. Source testing on Chinese residential coal combustion provides direct evidence that intensive coal combustion could contribute to increased light-absorptivity of ambient BrC in Beijing winter. Coal combustion is an important source to BrC in regions such as northern China, especially during the winter season. Future modeling of OA radiative forcing should consider the importance of both biomass and fossil sources.

Sources and spatial distribution of particulate polycyclic aromatic hydrocarbons in Shanghai, China

Atmospheric particulate polycyclic aromatic hydrocarbons (PAHs) have been drawing sustained attention due to their health risk and effects on air pollution. It is essential to determine the main sources and reduce atmospheric levels of PAHs to protect human health. PAHs in PM2.5 have been detected at five sites located in five districts in Shanghai, a modern metropolitan city in China. Spatial and temporal variations of composition profiles and sources of PAHs at each site in each season were investigated. The results showed that atmospheric particulate PAHs level in Shanghai was the lowest in summer and the highest in winter, dominated by high molecular weight (HMW) PAHs. Analysis with a combination of coefficients of Pearsons correlation and coefficient of divergences indicated heterogeneous spatial and temporal distribution for LMW PAHs and homogenous distribution for HMW PAHs. Diagnostic ratios and positive matrix factorization (PMF) model both identified pyrogenic sources as the main contributor of PAHs in Shanghai, with vehicular source contribution of 32-43% to the total PAHs annually and around 20% from biomass burning emissions in urban and urban buildup areas. While in winter, coal combustion and biomass burning could act as two major sources of PAHs in suburban areas, which could contribute to >70% of total PAHs measured in PM2.5 in Shanghai.

Comparison and overview of PM2.5 source apportionment methods

Serious air pollution in China now has great influence and threat on air quality, visibility, and human health. Accurate identification and quantification of sources play an important role in establishing relative policies, laws and control measures. This study briefly introduces development history and characteristics of three main methods to apportion sources of particles (emission inventory, source- oriented model and receptor model). Based on data platform of PM2.5 and chemical components conducted in Atlanta, USA, this study summarizes characteristics of major source apportionment methods of source-oriented model and receptor model and their performance towards different sources (i.e. vehicle emission, coal combustion, biomass burning, dust and secondary sources), points out the differences of various methods and potential reasons and analyzes their weakness and strength in application, suggesting that developing ensemble method should be an important direction for future source apportionment research.当前我国PM 2.5 污染严重, 空气质量、大气能见度和人体健康均受到影响和威胁, 准确判定解析和定量确定PM 2.5 的来源是有针对性地制定相关政策法规和控制措施的重要科学前提. 本文简要总结目前3大主要颗粒物源解析方法——源清单法、扩散模型法和受体模型法的发展历程和应用特征; 以美国亚特兰大采集的PM 2.5 及化学成分为公共数据平台, 评述了目前几种主要PM 2.5 源解析模型(受体模型和扩散模型)的方法特点以及适用性, 分析了不同源解析方法对机动车源、燃煤源、生物质燃烧源、道路尘以及二次源等多种源类的解析特点、结果差异以及可能原因, 总结了各种源解析方法在方法及应用上的优势和局限, 提出多种方法集成应用和发展混合模型是未来开展颗粒物源解析工作的方向.

Sources of primary and secondary organic aerosol and their diurnal variations.

PM(2.5), as one of the criteria pollutants regulated in the U.S. and other countries due to its adverse health impacts, contains more than hundreds of organic pollutants with different sources and formation mechanisms. Daytime and nighttime PM2.5 samples from the August Mini-Intensive Gas and Aerosol Campaign (AMIGAS) in the southeastern U.S. were collected during summer 2008 at one urban site and one rural site, and were analyzed for organic carbon (OC), elemental carbon (EC), water soluble organic carbon (WSOC), and various individual organic compounds including some important tracers for carbonaceous aerosol sources by gas chromatography-mass spectrometry. Most samples exhibited higher daytime OC concentration, while higher nighttime OC was found in a few events at the urban site. Sources, formation mechanisms and composition of organic aerosol are complicated and results of this study showed that it exhibited distinct diurnal variations. With detailed organic tracer information, sources contributing to particulate OC were identified: higher nighttime OC concentration occurring in several occasions was mainly contributed by the increasing primary emissions at night, especially diesel exhaust and biomass burning; whereas sources responsible for higher daytime OC concentration included secondary organic aerosol (SOA) formation (e.g., cis-pinonic acid and non-biomass burning WSOC) together with traffic emissions especially gasoline engine exhaust. Primary tracers from combustion related sources such as EC, polycyclic aromatic hydrocarbons, and hopanes and steranes were significantly higher at the urban site with an urban to rural ratio between 5 and 8. However, this urban-rural difference for secondary components was less significant, indicating a relatively homogeneous distribution of SOA spatially. We found cholesterol concentrations, a typical tracer for meat cooking, were consistently higher at the rural site especially during the daytime, suggesting the likely additional sources for this tracer at rural site and that it should be used with caution as meat cooking tracer in rural areas in the future.

Sources and characteristics of fine particles over the Yellow Sea and Bohai Sea using online single particle aerosol mass spectrometer

Marine aerosols over the East China Seas are heavily polluted by continental sources. During the Chinese Comprehensive Ocean Experiment in November 2012, size and mass spectra of individual atmospheric particles in the size range from 0.2 to 2.0 μm were measured on board by a single particle aerosol mass spectrometer (SPAMS). The average hourly particle number (PN) was around 4560±3240 in the South Yellow Sea (SYS), 2900±3970 in the North Yellow Sea (NYS), and 1700±2220 in the Bohai Sea (BS). PN in NYS and BS varied greatly over 3 orders of magnitude, while that in SYS varied slightly. The size distributions were fitted with two log-normal modes. Accumulation mode dominated in NYS and BS, especially during episodic periods. Coarse mode particles played an important role in SYS. Particles were classified using an adaptive resonance theory based neural network algorithm (ART-2a). Six particle types were identified with secondary-containing, aged sea-salt, soot-like, biomass burning, fresh sea-salt, and lead-containing particles accounting for 32%, 21%, 18%, 16%, 4%, and 3% of total PN, respectively. Aerosols in BS were relatively enriched in particles from anthropogenic sources compared to SYS, probably due to emissions from more developed upwind regions and indicating stronger influence of continental outflow on marine environment. Variation of source types depended mainly on origins of transported air masses. This study examined rapid changes in PN, size distribution and source types of fine particles in marine atmospheres. It also demonstrated the effectiveness of high-time-resolution source apportionment by ART-2a.

Application and Progress of Single Particle Aerosol Time-of-Flight Mass Spectrometry in Fine Particulate Matter Research

Abstract The idea of single particle aerosol mass spectrometry was first proposed in the 1970s and then developed quickly in recent two decades. Because it can simultaneously provide much information including particle size distribution, composition of multiple chemical species and mixing state for each single particle with high-time resolution, single particle aerosol mass spectrometry has been widely applied in the area of environmental monitoring and fine particulate matter research. This review aims to (1) provide an introduction of the development history and progress of single particle aerosol time-of-flight mass spectrometry, (2) summarize its principle, methods for data analysis, output of results and its applications in environmental measurement and research using two major commercialized instruments (ATOFMS and SPAMS), and (3) provide suggestions for future research.

Residential Coal Combustion as a Source of Levoglucosan in China

Levoglucosan (LG) has been widely identified as a specific marker for biomass burning (BB) sources and frequently utilized in estimating the BB contribution to atmospheric fine particles all over the world. However, this study provides direct evidence to show that coal combustion (CC) is also a source of LG, especially in the wintertime in Northern China, based on both source testing and ambient measurement. Our results show that low-temperature residential CC could emit LG with emission factors (EF) ranging from 0.3 to 15.9 mg kg-1. Ratios of LG to its isomers, mannosan and galactosan, differ between CC and BB emissions, and the wintertime ratios in Beijing ambient PM2.5 and source-specific tracers including carbon isotopic signatures all indicated a significant contribution from CC to ambient levoglucosan in winter in Beijing. The results suggest that LG cannot be used as a distinct source marker for biomass burning in special cases such as some cities in the northern China, where coal is still widely used in the residential and industrial sectors. Biomass burning sources could be overestimated, although such an over-estimation could vary spatially and temporally.

PM2.5 Source Apportionment in China

China has been facing a severe air pollution challenge in recent years. It is known that fine particulate matter is closely linked to haze. It is very important to have a good understanding of the formation mechanisms and sources of haze in China. This study provides long-term variation trends of meteorology and emissions during the past decades, reviews methodologies used in source apportionment of fine particulate matter based on published literature, and presents most recent source apportionment results from different cities in China, especially Beijing, the capital of China. Directions and key challenges in current source apportionment research are also discussed and suggestions are provided.