Although much attention has been paid to investigating and controlling air pollution in China, the trends of air-pollutant concentrations on a national scale have remained unclear. Here, we quantitatively investigated the variation of air pollutants in China using long-term comprehensive data sets from 2013 to 2017, during which Chinese government made major efforts to reduce anthropogenic emission in polluted regions. Our results show a significant decreasing trend in the PM_2.5 concentration in heavily polluted regions of eastern China, with an annual decrease of ∼7% compared with measurements in 2013. The measured decreased concentrations of SO₂, NO₂ and CO (a proxy for anthropogenic volatile organic compounds) could explain a large fraction of the decreased PM_2.5 concentrations in different regions. As a consequence, the heavily polluted days decreased significantly in corresponding regions. Concentrations of organic aerosol, nitrate, sulfate, ammonium and chloride measured in urban Beijing revealed a remarkable reduction from 2013 to 2017, connecting the decreases in aerosol precursors with corresponding chemical components closely. However, surface-ozone concentrations showed increasing trends in most urban stations from 2013 to 2017, which indicates stronger photochemical pollution. The boundary-layer height in capital cities of eastern China showed no significant trends over the Beijing–Tianjin–Hebei, Yangtze River Delta and Pearl River Delta regions from 2013 to 2017, which confirmed the reduction in anthropogenic emissions. Our results demonstrated that the Chinese government was successful in the reduction of particulate matter in urban areas from 2013 to 2017, although the ozone concentration has increased significantly, suggesting a more complex mechanism of improving Chinese air quality in the future.

Haze in China has been increasing in frequency of occurrence as well as the area of the affected region. Here, we report on a new mechanism of haze formation, in which coexistence with NOx can reduce the environmental capacity for SO₂, leading to rapid conversion of SO₂ to sulfate because NO₂ and SO₂ have a synergistic effect when they react on the surface of mineral dust. Monitoring data from five severe haze episodes in January of 2013 in the Beijing-Tianjin-Hebei regions agreed very well with the laboratory simulation. The combined air pollution of motor vehicle exhaust and coal-fired flue gases greatly reduced the atmospheric environmental capacity for SO₂, and the formation of sulfate was found to be a main reason for the growth of fine particles, which led to the occurrence of haze. These results indicate that the impact of motor vehicle exhaust on the atmospheric environment might be underestimated.

The mixing layer is an important meteorological factor that affects air pollution. In this study, the atmospheric mixing layer height (MLH) was observed in Beijing from July 2009 to December 2012 using a ceilometer. By comparison with radiosonde data, we found that the ceilometer underestimates the MLH under conditions of neutral stratification caused by strong winds, whereas it overestimates the MLH when sand-dust is crossing. Using meteorological, PM_2.5, and PM₁₀ observational data, we screened the observed MLH automatically; the ceilometer observations were fairly consistent with the radiosondes, with a correlation coefficient greater than 0.9. Further analysis indicated that the MLH is low in autumn and winter and high in spring and summer in Beijing. There is a significant correlation between the sensible heat flux and MLH, and the diurnal cycle of the MLH in summer is also affected by the circulation of mountainous plain winds. Using visibility as an index to classify the degree of air pollution, we found that the variation in the sensible heat and buoyancy term in turbulent kinetic energy (TKE) is insignificant when visibility decreases from 10 to 5 km, but the reduction of shear term in TKE is near 70 %. When visibility decreases from 5 to 1 km, the variation of the shear term in TKE is insignificant, but the decrease in the sensible heat and buoyancy term in TKE is approximately 60 %. Although the correlation between the daily variation of the MLH and visibility is very poor, the correlation between them is significantly enhanced when the relative humidity increases beyond 80 %. This indicates that humidity-related physicochemical processes is the primary source of atmospheric particles under heavy pollution and that the dissipation of atmospheric particles mainly depends on the MLH. The presented results of the atmospheric mixing layer provide useful empirical information for improving meteorological and atmospheric chemistry models and the forecasting and warning of air pollution.

Emissions of reactive nitrogen (N) species can affect surrounding ecosystems via atmospheric deposition. However, few long-term and multi-site measurements have focused on both the wet and the dry deposition of individual N species in large areas of Northern China. Thus, the magnitude of atmospheric deposition of various N species in Northern China remains uncertain. In this study, the wet and dry atmospheric deposition of different N species was investigated during a three-year observation campaign at ten selected sites in Northern China. The results indicate that N deposition levels in Northern China were high with a ten-site, three-year average of 60.6 kg N ha⁻¹ yr⁻¹. The deposition levels showed spatial and temporal variation in the range of 28.5–100.4 kg N ha⁻¹ yr⁻¹. Of the annual total deposition, 40% was deposited via precipitation, and the remaining 60% was comprised of dry-deposited forms. Compared with gaseous N species, particulate N species were not the major contributor of dry-deposited N; they contributed approximately 10% to the total flux. On an annual basis, oxidized species accounted for 21% of total N deposition, thereby implying that other forms of gaseous N, such as NH₃, comprised a dominant portion of the total flux. The contribution of NO₃⁻ to N deposition was enhanced in certain urban and industrial areas, possibly due to the fossil fuse combustion. As expected, the total N deposition in Northern China was significantly larger than the values reported by national scale monitoring networks in Europe, North America and East Asia because of high rates of wet deposition and gaseous NH₃ dry deposition. Taken together, these findings show that NH₃ emissions should be abated to mitigate high N deposition and associated potential impacts on ecosystems in Northern China. The present results improve our understanding of spatio-temporal variations of magnitudes, pathways and species of deposited N in the target areas, and are important not only to inform conservation and regulatory bodies but also to initiate further detailed studies. Uncertainties among current observations underscore the need to quantify the impact of vegetation on dry deposition and to refine the simulation of dry deposition velocity.

The simultaneous observation and analysis of atmospheric fine particles (PM_2.5) on a regional scale is an important approach to develop control strategies for haze pollution. In this study, samples of filtered PM_2.5 were collected simultaneously at three urban sites (Beijing, Tianjin, and Shijiazhuang) and at a regional background site (Xinglong) in the Beijing–Tianjin–Hebei (BTH) region from June 2014 to April 2015. The PM_2.5 at the four sites was mainly comprised of organic matter, secondary inorganic ions, and mineral dust. Positive matrix factorization (PMF) demonstrated that, on an annual basis, secondary inorganic aerosol was the largest PM_2.5 source in this region, accounting for 29.2–40.5 % of the PM_2.5 mass at the urban sites; the second-largest PM_2.5 source was motor vehicle exhaust, particularly in Beijing (24.9 %), whereas coal combustion was also a large source in Tianjin (12.4 %) and Shijiazhuang (15.5 %), with particular dominance in winter. Secondary inorganic aerosol plays a vital role in the haze process, with the exception of the spring haze in Shijiazhuang and Tianjin, for which the dust source was crucial. In addition to secondary transformations, local direct emissions (coal combustion and motor vehicle exhaust) significantly contribute to the winter haze at the urban sites. Moreover, with the aggravation of haze pollution, the OC ∕ EC mass ratio of PM_2.5 decreased considerably and the nitrate-rich secondary aerosol increased during all four seasons in Beijing, both of which indicate that local motor vehicle emissions significantly contribute to the severe haze episodes in Beijing. To assess the impacts of regional transport on haze pollution, the PMF results were further processed with backward-trajectory cluster analysis, revealing that haze pollution usually occurred when air masses originating from polluted industrial regions in the south prevailed and is characterized by high PM_2.5 loadings with considerable contributions from secondary aerosols. This study suggests that control strategies to mitigate haze pollution in the BTH region should focus on the reduction of gaseous precursor emissions from fossil fuel combustion (motor vehicle emissions in Beijing and coal combustion in Tianjin, Hebei, and nearby provinces).