Yongliang Ma

Trends in hazardous trace metal concentrations in aerosols collected in Beijing, China from 2001 to 2006

Daily observations of hazardous trace metal concentrations in aerosols in Beijing, China were made in the period from 2001 to 2006. We considered coal combustion as a major source of some anthropogenic metals by achieving a correlation analysis and by investigating enrichment factors and relative composition of metals. A possible extra source of some specific metals, such as Cu and Sb, was brake abrasion particles, however, we did not think the transport-related particle was a major source for the hazardous anthropogenic metals even though they could originate from vehicle exhaust and brake/tire abrasion particles. A time-trend model was used to describe temporal variations of chemical constituent concentrations during the five-year period. Several crustal elements, such as Al, Ti, V, Cr, Mn, Fe, and Co, did not show clear increases, with annual rates of change of -15.2% to 3.6%. On the other hand, serious increasing trends were noted from several hazardous trace metals. Cu, Zn, As, Cd, and Pb, which are derived mainly from anthropogenic sources, such as coal combustion, showed higher annual rate of change (4.9-19.8%, p<0.001) according to the regression model. In particular, the Cd and Pb concentrations increased remarkably. We hypothesize that the trend towards increasing concentrations of metals in the air reflects a change that has occurred in the process of burning coal, whereby the use of higher temperatures for coal combustion has resulted in increased emissions of these metals. The increasing use of low-rank coal may also explain the observed trends. In addition, nonferrous metal smelters are considered as a potential, albeit minor, reason for the increasing atmospheric concentrations of anthropogenic hazardous metals in Beijing city.

Measurement of humic-like substances in aerosols: a review.

Aerosol-phase humic-like substances (HULIS) have received increasingly attention due to their universal ambient presence, active participation in atmospheric chemistry and important environmental and health effects. In last decade, intensive field works have promoted development of quantification and analysis method, unearthed spatio-temporal variation, and proved evidence for source identification of HULIS. These important developments were summarized in this review to provide a global perspective of HULIS. The diverse operational HULIS definitions were gradually focused onto several versions. Although found globally in Europe, Asia, Australasia and North America, HULIS are far more typical in continental and near-ground aerosols. HULIS concentrations varied from <1 μg/m(3) to >13 μg/m(3), with their carbon fraction making up 9%-72% of water soluble organic carbon. Dominant HULIS source was suggested as secondary processes and biomass burning, with the detailed formation pathways suggested and verified in laboratory works.

Characteristics of Real-World Vehicular Emissions in Chinese Cities

Abstract On-board emission measurements were performed on 49 light-duty gasoline vehicles in seven cities of China. Vehicle-specific power mode distribution and emission characteristics were analyzed based on the data collected. The results of our study show that there were significant differences in different types of roads. The emission factors and fuel consumption rates on arterial roads and residential roads were approximately 1.4–2 times those on freeways. The carbon monoxide, hydrocarbon, and nitrogen oxides emission factors of Euro II vehicles were on average 86.2, 88.2, and 64.5% lower than those of carburetor vehicles, respectively. The new vehicle emission standards implemented in China had played an important role in reducing individual vehicle emissions. More comprehensive measures need to be considered to reduce the total amount of emissions from vehicles.

Review on recent progress in observations, source identifications and countermeasures of PM2.5.

Recently, PM2.5 (atmospheric fine particulate matter with aerodynamic diameter ≤ 2.5 μm) have received so much attention that the observations, source appointment and countermeasures of it have been widely studied due to its harmful impacts on visibility, mood (mental health), physical health, traffic safety, construction, economy and nature, as well as its complex interaction with climate. A review on the PM2.5 related research is necessary. We start with summary of chemical composition and characteristics of PM2.5 that contains both macro and micro observation results and analysis, wherein the temporal variability of concentrations of PM2.5 and major components in many recent reports is embraced. This is closely followed by an overview of source appointment, including the composition and sources of PM2.5 in different countries in the six inhabitable continents based on the best available results. Besides summarizing PM2.5 pollution countermeasures by policy, planning, technology and ideology, the World Air Day is proposed to be established to inspire and promote the crucial social action in energy-saving and emission-reduction. Some updated knowledge of the important topics (such as formation and evolution mechanisms of hazes, secondary aerosols, aerosol mass spectrometer, organic tracers, radiocarbon, emissions, solutions for air pollution problems, etc.) is also included in the present review by logically synthesizing the studies. In addition, the key research challenges and future directions are put forward. Despite our efforts, our understanding of the recent reported observations, source identifications and countermeasures of PM2.5 is limited, and subsequent efforts both of the authors and readers are needed.

Source of atmospheric heavy metals in winter in Foshan, China

Foshan is a ceramics manufacturing center in the world and the most polluted city in the Pearl River Delta (PRD) in southern China measured by the levels of atmospheric heavy metals. PM2.5 samples were collected in Foshan in winter 2008. Among the 22 elements and ions analyzed, 7 heavy metals (Zn, V, Mn, Cu, As, Cd and Pb) were studied in depth for their levels, spatiotemporal variations and sources. The ambient concentrations of the heavy metals were much higher than the reported average concentrations in China. The levels of Pb (675.7 ± 378.5 ng/m(3)), As (76.6 ± 49.1 ng/m(3)) and Cd (42.6 ± 45.2 ng/m(3)) exceeded the reference values of NAAQS (GB3095-2012) and the health guidelines of the World Health Organization. Generally, the levels of atmospheric heavy metals showed spatial distribution as: downtown site (CC, Chancheng District)>urban sites (NH and SD, Nanhai and Shunde Districts)>rural site (SS, Shanshui District). Two sources of heavy metals, the ceramic and aluminum industries, were identified during the sampling period. The large number of ceramic manufactures was responsible for the high levels of atmospheric Zn, Pb and As in Chancheng District. Transport from an aluminum industry park under light north-west winds contributed high levels of Cd to the SS site (Shanshui District). The average concentration of Cd under north-west wind was 220 ng/m(3), 20.5 times higher than those under other wind directions. The high daily maximum enrichment factors (EFs) of Cd, Pb, Zn, As and Cu at all four sites indicated extremely high contamination by local emissions. Back trajectory analysis showed that the heavy metals were also closely associated with the pathway of air mass. A positive matrix factorization (PMF) method was applied to determine the source apportionment of these heavy metals. Five factors (industry including the ceramic industry and coal combustion, vehicle emissions, dust, transportation and sea salt) were identified and industry was the most important source of atmospheric heavy metals. The present paper suggests a control policy on the four heavy metals Cd, Pb, Zn, and Cu, and suggests the inclusion of As in the ceramic industry emission standard in the future.

Humidity plays an important role in the PM2.5 pollution in Beijing

Heavily-polluted PM₂.₅ (fine particulate matter) episodes frequently impacting Beijing, especially during winter, have become a substantial concern. We found that during winter, the daily variation of PM2.5 in Beijing tracked the pattern of relative humidity (RH). With the increase of PM₂.₅ (or RH), water-soluble components (especially inorganic ions) became more abundant, and the water-soluble organic carbon to organic carbon ratios increased. The nitrate to sulfate ratios also exhibited dependence on RH, and were higher than those measured about a decade ago, consistent with the increasing trend of nitrogen oxides emissions. Surprisingly, the ratios of water-insoluble organic carbon to elemental carbon showed significant increase at high RH levels, presumably indicating the formation of secondary organic aerosol that is not soluble in water. In addition, humid winters were occasionally identified during 1996-2013 which are expected to be favorable for the formation of air pollution episodes with high PM₂.₅ concentrations.

The characteristics of Beijing aerosol during two distinct episodes: impacts of biomass burning and fireworks.

The chemical composition of Beijing aerosol was measured during summer and winter. Two distinct episodes were identified. Water-soluble potassium (K(+)) increased significantly during the firework episode in winter with an episode to non-episode ratio of 4.97, whereas the biomass burning (BB) episode in summer was characterized by high episode to non-episode ratios of levoglucosan (6.38) and K(+) (6.90). The BB and firework episodes had only a minor influence on the water-soluble OC (organic carbon) to OC ratio. Based on separate investigations of episode and non-episode periods, it was found that: (i) sulfate correlated strongly with both relative humidity and nitrate during the typical winter period presumably indicating the importance of the aqueous-phase oxidation of sulfur dioxide by nitrogen dioxide, (ii) oxalate and WSOC during both winter and summer in Beijing were mainly due to secondary formation, and (iii) high humidity can significantly enhance the formation potential of WSOC in winter.

Measurement of semivolatile carbonaceous aerosols and its implications: a review.

Measurement of carbonaceous aerosols is complicated by positive and negative artifacts. An organic denuder with high efficiency for removing gaseous organics is an effective approach to eliminate the positive artifact, and it is a precondition for the accurate determination of SVOC by an adsorbent backup filter. Evaluations of different configurations of the organic denuder, and SVOC determined by different denuder-based samplers, both integrated and semi-continuous, are reviewed. A new equation for determination of the denuder efficiency is estimated, considering the efficiency of removing both the gaseous organics that could be adsorbed by the quartz and the gaseous passing through the quartz that could be subsequently adsorbed by the backup adsorbent filter. The origin of OC on the backup quartz filter, behind either quartz or Teflon filter, is quantitatively evaluated by the denuder-based method based on the data published. The backup-OC is shown to be dominated by either gaseous organics passing through the front filter or the evaporated particulate organic carbon depending on the sampling environment.

Long-term trends of chemical characteristics and sources of fine particle in Foshan City, Pearl River Delta: 2008-2014.

Foshan is a major international ceramic center and the most polluted city in the Pearl River Delta (PRD). Here we present the results of the first long-term PM2.5 (particles <2.5μm) sampling and chemical characterization study of the city. A total of 2774 samples were collected at six sites from 2008 to 2014, and analyzed for water soluble species, elements and carbonaceous species. The major constituents of PM2.5 were sulfate, OC (Organic Carbon), nitrate, ammonium and EC (Elemental Carbon), which accounted for 50%-88% of PM2.5. PM2.5 and the most abundant chemical species decreased from 2008 to 2011, but rebounded in 2012-2013. After 2008, the chemical composition of PM2.5 changed dramatically due to the implementation of pollution control measures. From 2008 to 2011, SO4(2-) and NO3(-) were the two largest components; subsequently, however, OC was the largest component. The respective contributions of SO4(2-), NO3(-) and OC to the sum of water soluble species and carbonaceous species were 30.5%, 22.9% and 19.9% in 2008; and 20.2%, 16.5% and 30.2% in 2014. Distinct differences in nitrate and sulfate, and in mass ratio [NO3(-)]/[SO4(2-)] imply that mobile sources tended to more important in Foshan during 2012-2014. The results indicate that pollution control measures implemented during 2008-2014 had a large effect on anthropogenic elements (Pb, As, Cd, Zn and Cu) and water soluble species, but little influence on crustal elements (V, Mn, Ti, Ba and Fe) and carbonaceous species. The PMF method was used for source apportionment of PM2.5. Industry (including the ceramic industry and coal combustion), vehicles and dust were the three most important sources and comprised 39.2%, 20.0% and 18.4% of PM2.5 in 2008, respectively. However, secondary aerosols, vehicles and industry were the three most important sources and comprised 29.5%, 22.4% and 20.4% of PM2.5 in 2014, respectively. During the seven year study interval, the contributions of primary sources (industry and dust) decreased significantly, but secondary sources increased dramatically. Industry, dust and vehicles contributed 36.6μgm(-3), 13.9μgm(-3), and 9.2μgm(-3) to the reduction of PM2.5, respectively.

Episode-Based Evolution Pattern Analysis of Haze Pollution: Method Development and Results from Beijing, China

Haze episodes occurred in Beijing repeatedly in 2013, resulting in 189 polluted days. These episodes differed in terms of sources, formation processes, and chemical composition and thus required different control policies. Therefore, an overview of the similarities and differences among these episodes is needed. For this purpose, we conducted one-year online observations and developed a program that can simultaneously divide haze episodes and identify their shapes. A total of 73 episodes were identified, and their shapes were linked with synoptic conditions. Pure-haze events dominated in wintertime, whereas mixed haze-dust (PM2.5/PM10 < 60%) and mixed haze-fog (Aerosol Water/PM2.5 ∼ 0.3) events dominated in spring and summer-autumn, respectively. For all types, increase of ratio of PM2.5 in PM10 was typically achieved before PM2.5 reached ∼150 μg/m(3). In all PM2.5 species observed, organic matter (OM) was always the most abundant component (18-60%), but it was rarely the driving factor: its relative contribution usually decreased as the pollution level increased. The only OM-driven episode observed was associated with intensive biomass-burning activities. In comparison, haze evolution generally coincided with increasing sulfur and nitrogen oxidation ratios (SOR and NOR), indicating the enhanced production of secondary inorganic species. Applicability of these conclusions required further tests with simultaneously multisite observations.