Anthropogenic atmospheric emissions of typical toxic heavy metals have caused worldwide concern due to their adverse effects on human health and the ecosystem. By determining the best available representation of time-varying emission factors with S-shape curves, we establish the multiyear comprehensive atmospheric emission inventories of 12 typical toxic heavy metals (Hg, As, Se, Pb, Cd, Cr, Ni, Sb, Mn, Co, Cu, and Zn) from primary anthropogenic activities in China for the period of 1949–2012 for the first time. Further, we allocate the annual emissions of these heavy metals in 2010 at a high spatial resolution of 0.5° × 0.5° grid with ArcGIS methodology and surrogate indexes, such as regional population and gross domestic product (GDP). Our results show that the historical emissions of Hg, As, Se, Cd, Cr, Ni, Sb, Mn, Co, Cu, and Zn, during the period of 1949–2012, increased by about 22–128 times at an annual average growth rate of 5.1–8.0 %, reaching about 526.9–22 319.6 t in 2012. Nonferrous metal smelting, coal combustion of industrial boilers, brake and tyre wear, and ferrous metal smelting represent the dominant sources of heavy metal emissions. In terms of spatial variation, the majority of emissions are concentrated in relatively developed regions, especially for the northern, eastern, and southern coastal regions. In addition, because of the flourishing nonferrous metal smelting industry, several southwestern and central-southern provinces play a prominent role in some specific toxic heavy metals emissions, like Hg in Guizhou and As in Yunnan. Finally, integrated countermeasures are proposed to minimize the final toxic heavy metals discharge on account of the current and future demand of energy-saving and pollution reduction in China.

The main objective of this study is to investigate the formation and evolution mechanism of the regional haze in megacity Beijing by analyzing the process of a severe haze that occurred 20–27 September 2011. Mass concentration and size distribution of aerosol particles as well as aerosol optical properties were concurrently measured at the Beijing urban atmospheric environment monitoring station. Gaseous pollutants (SO₂, NO-NO₂-NO_x, O₃, CO) and meteorological parameters (wind speed, wind direction, and relative humidity) were simultaneously monitored. Meanwhile, aerosol spatial distribution and the height of planetary boundary layer (PBL) were retrieved from the signal of satellite and LIDAR (light detection and ranging). Concentrations of NO, NO₂, SO₂, O₃, and CO observed during 23–27 September had exceeded the national ambient air quality standards for residents. The mass concentration of PM_2.5 gradually accumulated during the measurement and reached at 220 μg m⁻³ on 26 September, and the corresponding atmospheric visibility was only 1.1 km. The daily averaged AOD in Beijing increased from ~ 0.16 at λ = 500 nm on 22 September and reached ~ 3.5 on 26 September. The key factors that affected the formation and evolution of this haze episode were stable anti-cyclone synoptic conditions at the surface, decreasing of the height of PBL, heavy pollution emissions from urban area, number and size evolution of aerosols, and hygroscopic growth for aerosol scattering. This case study may provide valuable information for the public to recognize the formation mechanism of the regional haze event over the megacity, which is also useful for the government to adopt scientific approach to forecast and eliminate the occurrence of regional haze in China.

The formation mechanism of aerosol sulfate during wintertime haze events in China is still largely unknown. As companions, SO₂ and transition metals are mainly emitted from coal combustion. Here, we argue that the transition metal-catalyzed oxidation of SO₂ on aerosol surfaces could be the dominant sulfate formation pathway and investigate this hypothesis by integrating chamber experiments, numerical simulations and in-field observations. Our analysis shows that the contribution of the manganese-catalyzed oxidation of SO₂ on aerosol surfaces is approximately one to two orders of magnitude larger than previously known routes, and contributes 69.2% ± 5.0% of the particulate sulfur production during haze events. This formation pathway could explain the missing source of sulfate and improve the understanding of atmospheric chemistry and climate change.

Emissions of hazardous trace elements in China are of great concern because of their negative impacts on local air quality as well as on regional environmental health and ecosystem risks. In this paper, the atmospheric emissions of mercury (Hg), arsenic (As), and selenium (Se) from coal combustion in China for the period 1980–2007 are estimated on the basis of coal consumption data and emission factors, which are specified by different categories of combustion facilities, coal types, and the equipped air pollution control devices configuration (Dust collectors, FGD, etc.). Specifically, multi-year emission inventories of Hg, As, and Se from 30 provinces and 4 economic sectors (thermal power, industry, residential use, and others) are evaluated and analyzed in detail. Furthermore, the gridded distribution of provincial-based Hg, As, and Se emissions in 2005 at a resolution of 1° × 1° is also plotted. It shows that the calculated national total atmospheric emissions of Hg, As, and Se from coal combustion have rapidly increased from 73.59 t, 635.57 t, and 639.69 t in 1980 to 305.95 t, 2205.50 t, and 2352.97 t in 2007, at an annually averaged growth rate of 5.4%, 4.7%, and 4.9%, respectively. The industrial sector is the largest source for Hg, As, and Se, accounting for about 50.8%, 61.2%, and 56.2% of the national totals, respectively. The share of power plants is 43.3% for mercury, 24.9% for arsenic, and 33.4% for selenium, respectively. Also, it shows remarkably different regional contribution characteristics of these 3 types of trace elements, the top 5 provinces with the heaviest mercury emissions in 2007 are Shandong (34.40 t), Henan (33.63 t), Shanxi (21.14 t), Guizhou (19.48 t), and Hebei (19.35 t); the top 5 provinces with the heaviest arsenic emissions in 2007 are Shandong (219.24 t), Hunan (213.20 t), Jilin (141.21 t), Hebei (138.54 t), and Inner Mongolia (127.49 t); while the top 5 provinces with the heaviest selenium emissions in 2007 are Shandong (289.11 t), Henan (241.45 t), Jiangsu (175.44 t), Anhui (168.89 t), and Hubei (163.96 t). Between 2000 and 2007, provinces always rank at the top five largest Hg, As, and Se emission sources are: Shandong, Hebei, Shanxi, Henan, and Jiangsu, most of which are located in the east and are traditional industry-based or economically energy intensive areas in China. Notably, Hg, As, and Se emissions from coal combustion in China begin to grow at a more moderate pace since 2005. Emissions from coal-fired power plants sector began to decrease though the coal use had been increasing steadily, which can be mainly attributed to the increasing use of wet flue gas desulfurization (WFGD) in power plants, thus the further research and control orientations of importance for these hazardous trace elements should be the industrial sector.