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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, 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 ( N) 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 K (5.9-362.7 L g) 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.

Concentrations of PM2.5-bound trace elements have increased in China, with increasing anthropogenic emissions. In this study, long-term measurements of PM2.5-bound trace elements were conducted from January 2014 to January 2015 in the urban city of Jinan, east China. A positive matrix factorization model (PMF) and health risk assessment were used to evaluate the sources and health risks of these elements, respectively. Compared with most Chinese megacities, there were higher levels of arsenic, manganese, lead, chromium, and zinc in this city. Coal combustion, the smelting industry, vehicle emission, and soil dust were identified as the primary sources of all the measured elements. Heating activities during the heating period led to a factor of 1.3–2.8 higher concentrations for PM2.5 and all measured elements than those during the non-heating period. Cumulative non-carcinogenic and carcinogenic risks of the toxic elements exceeded the safety levels by 8–15 and 10–18 times, respectively. Arsenic was the critical element having the greatest health risk. Coal combustion caused the highest risk among the four sources. This work provides scientific data for making targeted policies to control air pollutants and protect human health.

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, and the average Hg content in PM (particles with a diameter of 2.5μm or less) was 6.60±5.82μgg. Both PHg and Hg content in PM 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 SO, CO and NO, 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.

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