Atmospheric mercury in an eastern Chinese metropolis (Jinan).

Urban emissions are a major contributor to atmospheric Hg budgets. Continuous measurements of total gaseous mercury (TGM) and particulate-bound mercury (PHg) in PM2.5 were conducted from October 2015 to July 2016 in a metropolis, Jinan, in eastern China. Average TGM and PHg concentrations were 4.91 ± 3.66 ng m-3 and 451.9 ± 433.4 pg m-3, respectively, in the entire study period. During the winter heating period (HP), mean concentrations of TGM and PHg were 5.79 ng m-3 and 598.7 pg m-3, respectively, twice higher than those during the non-heating periods (NHPs). During the HP, TGM exhibited a distinct diurnal pattern with a peak in the morning and a minimum in the afternoon on less polluted days but a singular peak at midday on heavily polluted days. The diurnal variation of TGM during the NHPs was predominantly influenced by the variation in boundary layer height while during the HP by anthropogenic emissions. The ratio of PHg/PM2.5 in Jinan was one to two orders of magnitude larger than those elsewhere worldwide and those in soil and coal, which suggested the high enrichment of PHg in PM2.5 in Jinan. Correlation and principle component analysis results suggested that PHg and TGM had common combustion sources during the HP, whereas PHg resulted mainly from biomass burning and meteorological variations during the NHPs. High Hg concentrations in Jinan were mostly caused by emissions from coal-fired power plants, especially for those situated east of the sampling site. In addition, TGM and PHg concentrations significantly increased during haze and fog episodes, but decreased during a dust episode due possibly to strong ventilation conditions combined with partitioning of Hg between adsorption to PM2.5 and coarse dust particles.

Insights on Chemistry of Mercury Species in Clouds over Northern China: Complexation and Adsorption.

Cloud effects on heterogeneous reactions of atmospheric mercury (Hg) are poorly understood due to limited knowledge of cloudwater Hg chemistry. Here we quantified Hg species in cloudwater at the summit of Mt. Tai in northern China. Total mercury (THg) and methylmercury (MeHg) in cloudwater were on average 70.5 and 0.15 ng L-1, respectively, and particulate Hg (PHg) contributed two-thirds of THg. Chemical equilibrium modeling simulations suggested that Hg complexes by dissolved organic matter (DOM) dominated dissolved Hg (DHg) speciation, which was highly pH dependent. Hg concentrations and speciation were altered by cloud processing, during which significant positive correlations of PHg and MeHg with cloud droplet number concentration ( Nd) were observed. Unlike direct contribution to PHg from cloud scavenging of aerosol particles, abiotic DHg methylation was the most likely source of MeHg. Hg adsorption coefficients Kad (5.9-362.7 L g-1) exhibited an inverse-power relationship with cloud residues content. Morphology analyses indicated that compared to mineral particles, fly ash particles could enhance Hg adsorption due to more abundant carbon binding sites on the surface. Severe particulate air pollution in northern China may bring substantial Hg into cloud droplets and impact atmospheric Hg geochemical cycling by aerosol-cloud interactions.

Distribution and sources of particulate mercury and other trace elements in PM2.5 and PM10 atop Mount Tai, China.

The concentrations of particulate mercury (PHg) and other trace elements in PM2.5 and PM10 in the atmosphere were measured at the summit of Mount Tai during the time period of 15 June - 11 August 2015. The average PHg concentrations were 83.33 ±â€¯119.1 pg/m3 for PM2.5 and 174.92 ±â€¯210.5 pg/m3 for PM10. Average concentrations for other trace elements, including Al, Ca, Fe, K, Mg, Na, Pb, As, Se, Cu, Cd, Cr, V, Mo, Co, Ag, Ba, Mn, Zn and Ni ranged from 0.06 ng/m3 (Ag) to 354.33 ng/m3 (Ca) in PM2.5 and 0.11 ng/m3 (Co) to 592.66 ng/m3 (Ca) in PM10. The average concentrations of PHg were higher than those at other domestic mountain sites and cities in other counties, lower than those at domestic city sites. Other trace elements showed concentrations lower than those at the domestic mountain sites. Due possibly to increased control of emissions and the proportion of new energy, the PHg and trace element concentrations decreased, but the PHg showed concentrations higher than those at the Mountain sites, this showed that the reasons was not only severely affected by anthropogenic emissions, but also associated with other sources. The concentration changed trend of the main trace elements indicated that PHg, trace elements and particle matters present positive correlation and fine particulate matter has a greater surface area which was conductive to adsorption of Hg and trace elements to particles. On June 19, June 27 and July 6, according to the peak of mercury and trace elements, we can predict the potential sources of these three days. The results of principal component analysis (PCA) suggested that, crustal dust, coal combustion, and vehicle emissions were the main emission sources of PHg and other trace elements in Mount Tai. The 24-h backward trajectories and potential source contribution function (PSCF) analysis revealed that air masses arriving at Mount Tai were mainly affected by Shandong province. Mount Tai was subjected to five main airflow trajectories. Clusters 1, 2, 3, and 5 represented four pathways for local and regional sources and cluster 4 originated long-distance transportation. Central Shandong was the main source regions of PHg, Pb, Se, As, Cu and Cd. Southeastern and northwestern Shandong province and northern Jiangsu province were the most polluted source regions of Mn, Zn, and Ni. The crustal elements Fe and Ca had similar distributions of potential source regions, suggested by the highest PSCF values in southeastern Shandong and northern Jiangsu.

Polycyclic aromatic hydrocarbons (PAHs) associated with PM2.5 within boundary layer: Cloud/fog and regional transport.

A study of PM2.5-associated PAHs analysis at Mount Lushan (1165m) was conducted to investigate the distributions of PAHs in PM2.5 and influences of cloud/fog. The main purpose was to quantify the main emission sources of PAHs and estimate regional transport effects within the boundary layer. Mount Lushan is located between the boundary layer and troposphere, which is an ideal site for atmosphere transport investigation. The concentrations of PAHs in PM2.5 were analyzed with GC-MS. The results showed that the volume concentration was 6.98ng/m3 with a range from 1.47 to 25.17ng/m3 and PAHs mass were 160.24µg/g (from 63.86 to 427.97µg/g) during the sampling time at Mount Lushan. The dominant compounds are BbF, Pyr and BP. In terms of aromatic-ring PAHs distributions, 4-6-ring PAHs are predominant, indicating that the high-ring PAHs tend to contribute more than low-ring PAHs in particulates. Due to frequent cloud/fog days at Mount Lushan, PAHs concentrations in the PM2.5 were determined before and after cloud/fog weather. The results demonstrated that the cloud/fog and rain conditions cause lower PAHs levels. Regression analysis was used for studying the relationship of PAHs distributions with meteorological conditions like temperature, humidity and wind. The results showed that the temperature and wind speed were inversely related with PAHs concentration but humidity had no significant relationship. Furthermore, backward trajectories and PCA combined with DR (diagnostic ratio analysis) were employed to identify the influences of regional transport and main emission sources. The results revealed that PAHs in PM2.5 were mainly affected by regional transport with the main emissions by mobile vehicle and steel industry, which contributed about 56.0% to the total PAHs in the area of Mount Lushan. In addition, backward trajectories revealed that the dominant air masses were from the northwest accounting for about one third of total PAHs.

Characteristics and potential sources of atmospheric particulate mercury in Jinan, China.

Measurements of atmospheric particulate mercury (PHg) were conducted at a suburban site in Jinan, China from June 2014 to December 2015. The average PHg concentration was 508.5±402.7pgm-3, and the average Hg content in PM2.5 (particles with a diameter of 2.5µm or less) was 6.60±5.82µgg-1. Both PHg and Hg content in PM2.5 aerosols were comparable to levels in some cities in China and were much higher than in cities in North America and Europe. Weak correlations were found between PHg and meteorological parameters. The correlations between PHg and other pollutants in ambient air, including SO2, CO and NOχ, together with their wind dependence were used for source analysis, which suggested coal-fired industries, cement plants and traffic emissions as potential local sources for the site. Cluster analysis of 36-h backward trajectories suggested that the regional transport from southwestern Shandong Province also contributed to PHg in Jinan.