Shaojie Song

Chemical characteristics of size-resolved PM2.5 at a roadside environment in Beijing, China

Size-resolved particulate matter in the three size ranges (0.2-0.5 μm, 0.5-1.0 μm, and 1.0-2.5 μm) were collected at a roadside site in Beijing during and after the 2008 Olympic Games. The concentrations of PM mass, 14 elements, 3 major inorganic ions, and carbonaceous species were determined. The main contributors to PM(2.5) were crustal sources, vehicle emissions, secondary aerosol formation along with coal combustion, biomass from burning, and industrial processes, with vehicle emissions contributing more to roadside PM(2.5) than in the urban areas. The peaks at 0.5-1.0 μm in summer for PM mass and inorganic ions were most likely due to secondary aerosol formation, whereas the peaks at 0.2-0.5 μm in winter for PM mass and some elements were probably attributed to combustion from heating sources. The temporary control measures applied during the Olympics showed different effects on various emission sources and chemical species.

Trend analysis from 1970 to 2008 and model evaluation of EDGARv4 global gridded anthropogenic mercury emissions

The Emission Database for Global Atmospheric Research (EDGAR) provides a time-series of man-made emissions of greenhouse gases and short-lived atmospheric pollutants from 1970 to 2008. Mercury is included in EDGARv4.tox1, thereby enriching the spectrum of multi-pollutant sources in the database. With an average annual growth rate of 1.3% since 1970, EDGARv4 estimates that the global mercury emissions reached 1,287 tonnes in 2008. Specifically, gaseous elemental mercury (GEM) (Hg(0)) accounted for 72% of the global total emissions, while gaseous oxidised mercury (GOM) (Hg(2+)) and particle bound mercury (PBM) (Hg-P) accounted for only 22% and 6%, respectively. The less reactive form, i.e., Hg(0), has a long atmospheric residence time and can be transported long distances from the emission sources. The artisanal and small-scale gold production, accounted for approximately half of the global Hg(0) emissions in 2008 followed by combustion (29%), cement production (12%) and other metal industry (10%). Given the local-scale impacts of mercury, special attention was given to the spatial distribution showing the emission hot-spots on gridded 0.1°×0.1° resolution maps using detailed proxy data. The comprehensive ex-post analysis of the mitigation of mercury emissions by end-of-pipe abatement measures in the power generation sector and technology changes in the chlor-alkali industry over four decades indicates reductions of 46% and 93%, respectively. Combined, the improved technologies and mitigation measures in these sectors accounted for 401.7 tonnes of avoided mercury emissions in 2008. A comparison shows that EDGARv4 anthropogenic emissions are nearly equivalent to the lower estimates of the United Nations Environment Programme (UNEP)s mercury emissions inventory for 2005 for most sectors. An evaluation of the EDGARv4 global mercury emission inventory, including mercury speciation, was performed using the GEOS-Chem global 3-D mercury model. The model can generally reproduce both spatial variations and long-term trends in total gaseous mercury concentrations and wet deposition fluxes.

Characterization and source apportionment of particulate PAHs in the roadside environment in Beijing.

The profiles of particulate polycyclic aromatic hydrocarbons (PAHs) near a major road and relative major sources were determined based on five 1-week intensive field campaigns in 2008 and 2009, and the impacts of temporary control measures on roadside PAHs during the Beijing Olympics are discussed. The annual average concentration of PAHs in the non-Olympic period was 42.3 ± 52.4 ng/m(3) and clear seasonal variation was present. Diesel vehicles, gasoline vehicles and coal combustion were identified as the three possible major sources of roadside PAHs using positive matrix factorization analysis. During the Olympics, the average total PAH concentration decreased to 4.8 ± 2.7 ng/m(3), which was attributed primarily to the reduction of local emissions. Temporary traffic control measures significantly changed the diurnal pattern of particulate PAHs at the roadside site. Diesel vehicle contribution, in particular, decreased to a negligible fraction because heavy-duty diesel vehicles were strictly banned.

Oxidation of mercury by bromine in the subtropical Pacific free troposphere

Mercury is a global toxin that can be introduced to ecosystems through atmospheric deposition. Mercury oxidation is thought to occur in the free troposphere by bromine radicals, but direct observational evidence for this process is currently unavailable. During the 2013 Nitrogen, Oxidants, Mercury and Aerosol Distributions, Sources and Sinks campaign, we measured enhanced oxidized mercury and bromine monoxide in a free tropospheric air mass over Texas. We use trace gas measurements, air mass back trajectories, and a chemical box model to confirm the origin and chemical history of the sampled air mass. We find the presence of elevated oxidized mercury to be consistent with oxidation of elemental mercury by bromine atoms in this subsiding upper tropospheric air mass within the subtropical Pacific High, where dry atmospheric conditions are conducive to oxidized mercury accumulation. Our results support the role of bromine as the dominant oxidant of mercury in the upper troposphere.

Characteristics of On-road Diesel Vehicles: Black Carbon Emissions in Chinese Cities Based on Portable Emissions Measurement

Black carbon (BC) emissions from heavy-duty diesel vehicles (HDDVs) are rarely continuously measured using portable emission measurement systems (PEMSs). In this study, we utilize a PEMS to obtain real-world BC emission profiles for 25 HDDVs in China. The average fuel-based BC emissions of HDDVs certified according to Euro II, III, IV, and V standards are 2224 ± 251, 612 ± 740, 453 ± 584, and 152 ± 3 mg kg(-1), respectively. Notably, HDDVs adopting mechanical pump engines had significantly higher BC emissions than those equipped with electronic injection engines. Applying the useful features of PEMSs, we can relate instantaneous BC emissions to driving conditions using an operating mode binning methodology, and the average emission rates for Euro II to Euro IV diesel trucks can be constructed. From a macroscopic perspective, we observe that average speed is a significant factor affecting BC emissions and is well correlated with distance-based emissions (R(2) = 0.71). Therefore, the average fuel-based and distance-based BC emissions on congested roads are 40 and 125% higher than those on freeways. These results should be taken into consideration in future emission inventory studies.

Synthesis of the Southeast Atmosphere Studies: Investigating Fundamental Atmospheric Chemistry Questions

AbstractThe Southeast Atmosphere Studies (SAS), which included the Southern Oxidant and Aerosol Study (SOAS); the Southeast Nexus (SENEX) study; and the Nitrogen, Oxidants, Mercury and Aerosols: Distributions, Sources and Sinks (NOMADSS) study, was deployed in the field from 1 June to 15 July 2013 in the central and eastern United States, and it overlapped with and was complemented by the Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. SAS investigated atmospheric chemistry and the associated air quality and climate-relevant particle properties. Coordinated measurements from six ground sites, four aircraft, tall towers, balloon-borne sondes, existing surface networks, and satellites provide in situ and remotely sensed data on trace-gas composition, aerosol physicochemical properties, and local and synoptic meteorology. Selected SAS findings indicate 1) dramatically reduced NOx concentrations have altered ozone production regimes; 2) indica...

Mass concentrations and temporal profiles of PM10, PM2.5 and PM1 near major urban roads in Beijing

Mass concentrations of PM10, PM2.5 and PM1 were measured near major roads in Beijing during six periods: summer and winter of 2001, winter of 2007, and periods before, during and after the 2008 Beijing Olympic Games. Since the control efforts for motor vehicles helped offset the increase of emissions from the rapid growth of vehicles, the averaged PM2.5 concentrations at roadsides during the sampling period between 2001 and 2008 fluctuated over a relatively small range. With the implementation of temporary traffic control measures during the Olympics, a clear “V” shaped curve showing the concentrations of particulate matter and other gaseous air pollutants at roadsides over time was identified. The average concentrations of PM10, PM2.5, CO and NO decreased by 31.2%, 46.3%, 32.3% and 35.4%, respectively, from June to August; this was followed by a rebound of all air pollutants in December 2008. Daily PM10 concentrations near major roads exceeded the National Ambient Air Quality Standard (Grade II) for 61.2% of the days in the non-Olympic periods, while only for 12.5% during the Olympics. The mean ratio of PM2.5/ PM10 near major roads remained relatively stable at 0.55 (±0.108) on non-Olympic days. The ratio decreased to 0.48 (±0.099) during the Olympics due to a greater decline in fine particles than in coarse-mode PM. The ratios PM1/ PM2.5 fluctuated over a wide range and were statistically different from each other during the sampling periods. The average ratios of PM1/PM2.5 on non-Olympic days were 0.71.

Chemical characterization of roadside PM2.5 and black carbon in Macao during a summer campaign

Air pollution is the leading environmental concern in Macao. The temporal variations of particulate matter (PM) and black carbon (BC) mass concentrations and the size-resolved PM2.5 chemical compositions, including trace elements and carbonaceous species, were measured in Macao during a near-road summer campaign. The average concentra- tions for PM10, PM2.5 and BC at a roadside measurement site were 37.8 μg m -3 , 31.4 μg m -3 and 5.6 μg m -3 , respectively. Results showed that local emissions contributed at least 35% to PM2.5 mass in Macao. Higher BC concentrations were observed in the daytime than at night, consistent with the diurnal variations of traffic flow. Factor analysis classified trace elements into three categories, representing crustal sources (Mg, Si, Al, Na, Fe, Ca and K), road traffic sources (Cu and Co) and secondary inorganic particle formation (S). Crustal elements and road traffic elements were enriched in the size ranges of >1.0 μm and <0.2 μm, respectively. The unimodal distribution pattern with a peak at <0.2 μm for organic carbon (OC) was probably due to secondary organic aerosol formation, whereas about 70% of elemental carbon (EC) was in the size range of 0.2-1.0 μm. Secondary organic aerosols were found to be a strong contributor to PM in the size ranges of <0.2 μm and 1.0-2.5 μm.

The impact of power generation emissions on ambient PM2.5 pollution and human health in China and India

Emissions from power plants in China and India contain a myriad of fine particulate matter (PM2.5, PM ≤ 2.5 μm in diameter) precursors, posing significant health risks among large, densely settled populations. Studies isolating the contributions of various source classes and geographic regions are limited in China and India, but such information could be helpful for policy makers attempting to identify efficient mitigation strategies. We quantified the impact of power generation emissions on annual mean PM2.5 concentrations using the state-of-the-art atmospheric chemistry model WRF-Chem (Weather Research Forecasting model coupled with Chemistry) in China and India. Evaluations using nationwide surface measurements show the model performs reasonably well. We calculated province-specific annual changes in mortality and life expectancy due to power generation emissions generated PM2.5 using the Integrated Exposure Response (IER) model, recently updated IER parameters from Global Burden of Disease (GBD) 2015, population data, and the World Health Organization (WHO) life tables for China and India. We estimate that 15 million (95% Confidence Interval (CI): 10 to 21 million) years of life lost can be avoided in China each year and 11 million (95% CI: 7 to 15 million) in India by eliminating power generation emissions. Priorities in upgrading existing power generating technologies should be given to Shandong, Henan, and Sichuan provinces in China, and Uttar Pradesh state in India due to their dominant contributions to the current health risks.