•The mean concentrations of PM1 and PM2.5 decreased with floors as a whole.•Trace metals in the first floor were mainly concentrated in the coarse particles.•Minerals, soot, fly ash, sulfate, biogenic particles, Fe-rich and Zn particles were observed in the hospital.Health risk of populations dwelling in the hospital has been a global concern, but has not been adequately examined. PM2.5 and PM1 samples were collected in two indoor locations (outpatient department and inpatient department) and one outdoor location (courtyard) of the hospital in Shanghai. The concentrations of size-fractionated trace metals and the morphology of single particles were determined to accurately assess the health risk for populations in the hospital. The results indicated that the mean concentrations of PM2.5 and PM1 were in the order of outpatient department > courtyard > inpatient department. The mean concentrations of PM1 decreased with floors (first floor: 78.0 μg/m3, second floor: 64.1 μg/m3, fourth floor: 48.4 μg/m3). However, the mean PM2.5 concentrations were in the order of first floor (124.0 μg/m3) > fourth floor (91.4 μg/m3) > second floor (90.6 μg/m3), which was likely associated with the number of patients. The PM2.5 and PM1 concentrations have begun to increase rapidly from 9:00 am and decreased after 15:00 pm in the first floor, whereas they remain relatively stable in the second and fourth floor. The abundance of Mg, Ca, Al and K in the fine particles and coarse particles were both higher than other elements for all floors. The concentrations of trace metals (e.g., Zn, Ba, Fe, Mn, Cr, Ca, Ti, Na, and K) except Mg and Al in the coarse particles (> 2.5 μm) decreased with floors, whereas Zn, Ba, Fe, and Cr in the fine particles (< 2.5 μm) displayed opposite variation. Trace metals in the first floor were mainly concentrated in the > 2.5 μm and 1–2.5 μm, whereas they chiefly peaked at 0.25–0.5 μm and below 0.25 μm in the second and fourth floor. Single particles analysis showed that mineral particles, soot, and Fe-rich particles were mainly concentrated in the first floor, indicating the impacts of walking of patients, traffic emissions, and food cooking, respectively. Sulfate particles were internally mixed with soot, fly ash and Fe-rich particles in the second floor, which suggested that these sulfate particles probably underwent aging processes during the atmospheric long-range transport. In the fourth floor, fly ash, sulfate particles, Zn-rich particles, and biogenic particles were identified under the transmission electron microscopy (TEM). Higher abundance of sulfates and absence of chlorate hinted existence of heterogeneous reactions during long-range transport with the Cl− replaced by SO42 −. The index of average daily intake (ADI), hazard quotient (HQ), and carcinogenic risks (CR) indicated that Cr pose carcinogenic risks to the surrounding populations, while non-carcinogenic risks of Mn, Zn, and Cr were not remarkable.Mineral particles, soot, and Fe-rich particles were mainly concentrated in the first floor, indicating the impacts of walking of patients, traffic emissions, and food cooking. Sulfate particles were internally mixed with soot, fly ash and Fe-rich particles in the second floors, which suggested that these sulfate particles probably underwent aging processes during atmospheric long-range transport. In the fourth floor, fly ash, sulfate particles, Zn-rich particles, and biogenic particles were identified under the TEM.Download high-res image (247KB)Download full-size image

•The emissions of Cu and Zn from coal increased from 1995 to 2014.•The Cu and Zn emissions from industrial sector rank as primary source.•The trace metal emissions are closely associated with mortality and LE.China has become the largest coal consumer and important emitter of trace metals in the world. A multiple-year inventory of atmospheric copper (Cu) and zinc (Zn) emissions from coal combustion in 30 provinces of China and 4 economic sectors (power plant, industry sector, residential sector, and others) for the period of 1995–2014 has been calculated. The results indicated that the total emissions of Cu and Zn increased from 5137.70 t and 11484.16 t in 1995–7099.24 t and 14536.61 t in 2014, at an annual average growth rate of 1.90% and 1.33%, respectively. The industrial sector ranked as the leading source, followed by power plants, the residential use, and other sectors. The emissions of Cu and Zn were predominantly concentrated in the northern and eastern regions of China due to the enormous consumption of coal by the industrial and the power sectors. The emissions of Cu and Zn were closely associated with mortality and life expectancy (LE) on the basis of multiple regression analysis. Spatial econometric models suggested that Cu and Zn emissions displayed significantly positive relevance with mortality, while they exhibited negative correlation with LE. The influence of the Cu emission peaked in the north of China for both mortality and LE, while the impacts of the Zn emission on mortality and LE reached a maximum value in Xinjiang Province. The results of the grey prediction model suggested that the Cu emission would decrease to 5424.73 t, whereas the Zn emissions could reach 17402.13 t in 2020. Analysis of more specific data are imperative in order to estimate the emissions of both metals, to assess their human health effects, and then to adopt effective measures to prevent environmental pollution.The total emissions of Cu and Zn increased from 5137.70 t and 11484.16 t in 1995–7099.24 t and 14536.61 t in 2014, at an annual average growth rate of 1.90% and 1.33%, respectively. The industrial sector ranks as the leading source, followed by power plants, residential use, and other sectors in sequence.Download high-res image (197KB)Download full-size image

•Metal-containing particles were hosted by sulfates, nitrates, and oxides.•Six main types of Fe-containing particles could be observed by ATOFMS.•TEM and ATOFMS can supplement one another for single particle analysis.Aerosol particles were collected during three heavy haze episodes at Shanghai in the winter of 2013. Transmission electron microscopy (TEM) coupled with energy dispersive X-ray spectroscopy was used to study the morphology and speciation of typical metal particles at a single-particle level. In addition, time-of-flight aerosol mass spectrometry (ATOFMS) was applied to identify the speciation of the Fe-containing particles. TEM analysis indicated that various metal-containing particles were hosted by sulfates, nitrates, and oxides. Fe-bearing particles mainly originated from vehicle emissions and/or steel production. Pb-, Zn-, and Sb-bearing particles were mainly contributed by anthropogenic sources. Fe-bearing particles were clustered into six groups by ATOFMS: Fe-Carbon, Fe-Inorganic, Fe-Trace metal, Fe-CN, Fe-PO3, and Fe-NO3. ATOFMS data suggested that Fe-containing particles corresponded to different origins, including industrial activities, resuspension of dusts, and vehicle emissions. Fe-Carbon and Fe-CN particles displayed significant diurnal variation, and high levels were observed during the morning rush hours. Fe-Inorganic and Fe-Trace metal particle levels peaked at night. Furthermore, Fe-Carbon and Fe-PO3 were mainly concentrated in the fine particles. Fe-CN, Fe-Inorganic, and Fe-Trace metal exhibited bimodal distribution. The mixing state of the particles revealed that all Fe-bearing particles tended to be mixed with sulfate and nitrate. The data presented herein is essential for elucidating the origin, evolution processes, and health effects of metal-bearing particles.

•All of the pollutants except O3 decreased slightly during 2014–2016.•All of the pollutants except O3 displayed the highest levels in the winter.•PM10 is a major pollutant affecting the air quality of China.China is experiencing severe air pollution due to rapid economic development and accelerated urbanization. High-resolution temporal and spatial air pollution data are imperative to understand the physical and chemical processes affecting air quality of China. The data of PM2.5, PM10, SO2, CO, NO2, and O3 in 187 Chinese cities during January 2014 and November 2016 were collected to uncover the spatial and temporal variation of the pollutants in China. The annual mean concentrations of PM2.5 exceeded the Grade I standard of Chinese Ambient Air Quality (CAAQS) for all of the cities except several cities in Hainan, and more than 100 cities exceeded the CAAQS Grade II standard. The concentrations of PM2.5, PM10, SO2, CO, and NO2 decreased from 2014 to 2016, whereas the O3 level increased dramatically during this period. The concentrations of PM2.5, PM10, SO2, CO and NO2 exhibited the highest levels in winter and the lowest in summer, and evidently decreased from 2014 to 2016, whereas the O3 concentration peaked in spring and summer, and dramatically increased from 2014 to 2016. The non-attainment ratios were highest in winters, while high pollution days were also frequently observed in the Southeast region in autumn and in the Northwest region in spring. Pearson correlation analysis indicated that all of the pollutants exhibited significant correlation one another. PM10 was a major pollutant affecting the air quality of China in all of the seasons. Both SO2 and NO2 exerted significantly adverse effects on the air quality in spring and autumn, but CO played an important role on the air quality in winter. O3 was found to be the dominant species among the pollutants affecting the air quality in summer, suggesting that photochemical O3 formation should be paid more attention to improve the air quality in summer. The results of geographical weight regression (GWR) showed that more significant correlations among the pollutants and the highest air quality index (AQI) appeared in the south of China. The impacts of PM10 and NO2 on the air quality increased from the east to the west of China, while SO2 and O3 exhibited the opposite variation. The data presented herein supplied an important support for the future source apportionment and intra- and inter-regional transport modeling of pollutants.

Recent evidence suggested that organic ligands in atmosphere water play an important role in the mobilization of iron from mineral aerosol. In this study, the dissolution of goethite (α-FeOOH) was investigated in the presence of three low-molecular dicarboxylates enriched in the atmosphere, as well as a reference organic acid of methanesulfonate (MSA), which is especially abundant in marine atmospheric boundary layer. Iron mobilized from α-FeOOH was promoted under the irradiation and the deaerated condition, and the soluble Fe(II) concentration was enhanced greatly in the ligand-containing suspensions exposed to light. Irrespective of the reaction conditions, the capacities of the dicarboxylates on Fe mobilization were in the following order: oxalate > malonate > succinate, which were closely correlated with the carbon chain length of dicarboxylates: n = 2 > 3 > 4. The space barrier action of carbon atoms inhibited ligand-promoted Fe dissolution by affecting the structure and stability of the complexes. MSA also acted as an organic ligand to mobilize iron and showed weak capacity to reduce Fe(III) under the irradiation. The reactive oxygen species (ROS) analysis indicated that ·OH, O2·–, and H2O2 could be involved in the Fe(II)–Fe(III) redox circle, and the ligand-promoted photoreductive dissolution process could be an important source of ROS in atmosphere water. Both transmission electron microscopy analysis and zeta potential data supported that the adsorption of oxalate molecules onto the surface would change the aggregation state of goethite nanoparticles, which increased the effective surface area, and therefore facilitated Fe mobilization from the oxide. The data shown herein deepens our understanding on the ligand-promoted dissolution mechanisms, which could be an important formation pathway of bioavailable Fe in the atmosphere.

In this study, iron solubility from six combustion source particles was investigated in acidic media. For comparison, a Chinese loess (CL) dust was also included. The solubility experiments confirmed that iron solubility was highly variable and dependent on particle sources. Under dark and light conditions, the combustion source particles dissolved faster and to a greater extent relative to CL. Oil fly ash (FA) yielded the highest soluble iron as compared to the other samples. Total iron solubility fractions measured in the dark after 12 h ranged between 2.9 and 74.1% of the initial iron content for the combustion-derived particles (Oil FA > biomass burning particles (BP) > coal FA). Ferrous iron represented the dominant soluble form of Fe in the suspensions of straw BP and corn BP, while total dissolved Fe presented mainly as ferric iron in the cases of oil FA, coal FA, and CL. Mössbauer measurements and TEM analysis revealed that Fe in oil FA was commonly presented as nanosized Fe3O4 aggregates and Fe/S-rich particles. Highly labile source of Fe in corn BP could be originated from amorphous Fe form mixed internally with K-rich particles. However, Fe in coal FA was dominated by the more insoluble forms of both Fe-bearing aluminosilicate glass and Fe oxides. The data presented herein showed that iron speciation varies by source and is an important factor controlling iron solubility from these anthropogenic emissions in acidic solutions, suggesting that the variability of iron solubility from combustion-derived particles is related to the inherent character and origin of the aerosols themselves. Such information can be useful in improving our understanding on iron solubility from combustion aerosols when they undergo acidic processing during atmospheric transport.

C60 molecules with monomolecular layer state dispersed on the surface of ZnO and formed the hybridized interaction between ZnO and C60. C60-hybridized ZnO photocatalyst showed enhanced photocatalytic activity for the degradation of the organic dye and the photocorrosion of ZnO was successfully inhibited by the hybridization of C60 molecules. The photocorrosion inhibition of ZnO by C60 molecule could be attributed to the reduced activation of surface oxygen atom. The enhanced photocatalytic activity for C60-hybridized ZnO was originated from the high migration efficiency of photoinduced electrons on the interface of C60 and ZnO, which was produced by the interaction of C60 and ZnO with a conjugative π-system. The enhancement degree of photocatalytic activity was strongly depended on the coverage of C60 molecules on the surface of ZnO nanoparticles, and the optimum hybridization effect was found at a weight ratio of 1.5% (C60/ZnO). The hybridization of C60 with semiconductors could be used to improve the photocatalytic activity as well as the photostability.