Abstract. In January 2013, Beijing experienced several serious haze events. To achieve a better understanding of the characteristics, sources and processes of aerosols during this month, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed at an urban site between 1 January and 1 February 2013 to obtain the size-resolved chemical composition of non-refractory submicron particles (NR-PM1). During this period, the mean measured NR-PM1 mass concentration was 89.3 ± 85.6 μg m−3, and it peaked at 423 μg m−3. Positive matrix factorization (PMF) differentiated the organic aerosol into five components, including a highly oxidized, low-volatility oxygenated organic aerosol (LV-OOA), a less oxidized, semi-volatile oxygenated OA (SV-OOA), a coal combustion OA (CCOA), a cooking-related OA (COA), and a hydrocarbon-like OA (HOA), which on average accounted for 28%, 26%, 15%, 20% and 11% of the total organic mass, respectively. A detailed comparison between the polluted days and unpolluted days found many interesting results. First, the organic fraction was the most important NR-PM1 species during the unpolluted days (58%), while inorganic species were dominant on polluted days (59%). The OA composition also experienced a significant change; it was dominated by primary OA (POA), including COA, HOA and CCOA, on unpolluted days. The contribution of secondary OA (SOA) increased from 35% to 63% between unpolluted and polluted days. Second, meteorological effects played an important role in the heavy pollution in this month and differed significantly between the two types of days. The temperature and relative humidity (RH) were all increased on polluted days and the wind speed and air pressure were decreased. Third, the diurnal variation trend in NR-PM1 species and OA components showed some differences between the two types of days, and the OA was more highly oxidized on polluted days. Fourth, the effects of air masses were significantly different between the two types of days; air was mainly transported from contaminated areas on the polluted days. The comparison also found that the aerosol was more acidic on polluted days. Additionally, the variation trends of the mass concentration and mass fractions of NR-PM1 species and OA components were more dramatic when the NR-PM1 mass loading was at a higher level. The serious pollution observed in this month can be attributed to the synergy of unfavorable meteorological factors, the transport of air masses from high-pollution areas, emission by local sources, and other factors.
Abstract. 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, threeyear 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 NH 3 , comprised a dominant portion of the total flux. The contribution of NO − 3 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 NH 3 dry deposition. Taken together, these findings show that NH 3 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.
Additional size-resolved chemical information is needed before the physicochemical characteristics and sources of airborne particles can be understood; however, this information remains unavailable in most regions of China due to lacking measurement data. In this study, we report observations of various chemical species in size-segregated particle samples that were collected over 1 year in the urban area of Beijing, a megacity that experiences severe haze episodes. In addition to fine particles, high concentrations of coarse particles were measured during the periods of haze. The abundance and chemical compositions of the particles in this study were temporally and spatially variable, with major contributions from organic matter and secondary inorganic aerosols. The contributions of organic matter to the particle mass decreased from 37.9 to 31.2 %, and the total contribution of sulfate, nitrate and ammonium increased from 19.1 to 33.9 % between non-haze and haze days, respectively. Due to heterogeneous reactions and hygroscopic growth, the peak concentrations of the organic carbon, cadmium and sulfate, nitrate, ammonium, chloride and potassium shifted from 0.43 to 0.65 µm on non-haze days to 0.65-1.1 µm on haze days. Although the size distributions of lead and thallium were similar during the observation period, their concentrations increased by a factor of more than 1.5 on haze days compared with non-haze days. We observed that sulfate and ammonium, which have a size range of 0.43-0.65 µm, sulfate and nitrate, which have a size range of 0.65-1.1 µm, calcium, which has a size range of 5.8-9 µm, and the meteorological factors of relative humidity and wind speed were responsible for haze pollution when the visibility was less than 10 km. Source apportionment using Positive Matrix Factorization showed six PM 2.1 sources and seven PM 2.1−9 common sources: secondary inorganic aerosol (25.1 % for fine particles vs. 9.8 % for coarse particles), coal combustion (17.7 % vs. 7.8 %), biomass burning (11.1 % vs. 11.8 %), industrial pollution (12.1 % vs. 5.1 %), road dust (8.4 % vs. 10.9 %), vehicle emissions (19.6 % for fine particles), mineral dust (22.6 % for coarse particles) and organic aerosol (23.6 % for coarse particles). The contributions of the first four factors and vehicle emissions were higher on haze days than non-haze days, while the reverse is true for road dust and mineral dust. The sources' contribution generally increased as the size decreased, with the exception of mineral dust. However, two peaks were consistently found in the fine and coarse particles. In addition, the sources' contribution varied with the wind direction, with coal and oil combustion products increasing during southern flows. This result suggests that future air pollution control strategies should consider wind patterns, especially during episodes of haze. Furthermore, the findings of this study indicated that the PM 2.5based data set is insufficient for determining source control policies for haze in China and that detailed size-resolve...
Abstract. Atmospheric deposition is considered to be a major process that removes pollutants from the atmosphere and an important source of nutrients and contaminants for ecosystems. Trace elements (TEs), especially toxic metals deposited on plants and into soil or water, can cause substantial damage to the environment and human health due to their transfer and accumulation in food chains. Despite public concerns, quantitative knowledge of metal deposition from the atmosphere to ecosystems remains scarce. To advance our understanding of the spatiotemporal variations in the magnitudes, pathways, compositions and impacts of atmospherically deposited TEs, precipitation (rain and snow) and dry-deposited particles were collected simultaneously at 10 sites in Northern China from December 2007 to November 2010. The measurements showed that the wet and dry depositions of TEs in the target areas were orders of magnitude higher than previous observations within and outside China, generating great concern over the potential risks. The spatial distribution of the total (wet plus dry) deposition flux was consistent with that of the dry deposition, with a significant decrease from industrial and urban areas to suburban, agricultural and rural sites, while the wet deposition exhibited less spatial variation. In addition, the seasonal variation of wet deposition was also different from that of dry deposition, although they were both governed by the precipitation and emission patterns. For the majority of TEs that exist as coarse particles, dry deposition dominated the total flux at each site. This was not the case for potassium, nickel, arsenic, lead, zinc, cadmium, selenium, silver and thallium, for which the relative importance between wet and dry deposition fluxes varied by site. Whether wet deposition is the major atmospheric cleansing mechanism for the TEs depends on the size distribution of the particles. We found that atmospheric inputs of copper, lead, zinc, cadmium, arsenic and selenium were of the same magnitude as their increases in the topsoil of agricultural systems. At a background forest site in Northern China, the total deposition flux of lead observed in this study (14.1 mg m−2 yr−1) was twice that of the critical load calculated for temperate forest ecosystems in Europe. These findings provide baseline data needed for future targeting policies to protect various ecosystems from long-term heavy metal input via atmospheric deposition.
We present the X-ray timing results of the new black hole candidate (BHC) MAXI J1535-571 during its 2017 outburst from Hard X-ray Modulation Telescope (Insight -HXMT) observations taken from 2017 September 6 to 23. Following the definitions given by Belloni (2010), we find that the source exhibits state transitions from Low/Hard state (LHS) to Hard Intermediate state (HIMS) and eventually to Soft Intermediate state (SIMS). Quasi-periodic oscillations (QPOs) are found in the intermediate states, which suggest different types of QPOs. With the large effective area of Insight -HXMT at high energies, we are able to present the energy dependence of the QPO amplitude and centroid frequency up to 100 keV which is rarely explored by previous satellites. We also find that the phase lag at the type-C QPOs centroid frequency is negative (soft lags) and strongly correlated with the centroid frequency. By assuming a geometrical origin of type-C QPOs, the source is consistent with being a high inclination system.
Abstract. The evolution of physical, chemical and optical properties of urban aerosol particles was characterized during an extreme haze episode in Beijing, PRC, from 24 through 31 January 2013 based on in situ measurements. The average mass concentrations of PM1, PM2.5 and PM10 were 99 ± 67 μg m−3 (average ± SD), 188 ± 128 μg m−3 and 265 ± 157 μg m−3, respectively. A significant increase in PM1-2.5 fraction was observed during the most heavily polluted period. The average scattering coefficient at 550 nm was 877 ± 624 Mm−1. An increasing relative amount of coarse particles can be deduced from the variations of backscattering ratios, asymmetry parameter and scattering Ångström exponent. Particle number-size distributions between 14 and 2500 nm diameter showed high number concentrations, particularly in the nucleation mode and accumulation mode. Size-resolved chemical composition of submicron aerosol from a high-resolution time-of-flight aerosol mass spectrometer showed that the mass concentrations of organic, sulfate, nitrate, ammonium and chlorine mainly resided on particles between 500 and 800 nm (vacuum diameter), and nitrate and ammonium contributed greatly to particle growth during the heavily polluted day (28 January). Increasing relative humidity and stable synoptic conditions on 28 January combined with heavy pollution on 28 January, leading to enhanced water uptake by the hygroscopic submicron particles and formation of secondary aerosol, which might be the main reasons for the severity of the haze episode. Light-scattering apportionment showed that organic, sulfate, ammonium nitrate and ammonium chloride compounds contributed to light-scattering fractions of 54, 24, 12 and 10%, respectively. This study indicated that the organic component in submicron aerosol played an important role in visibility degradation during the haze episode in Beijing.
Abstract. Atmospheric sulfur (S) deposition via precipitation, particles and gases was investigated at ten sites in Northern China. Measurements were performed continuously between December 2007 and November 2010. The total S deposition flux in the target area ranged from 35.0 to 100.7 kg S ha −1 yr −1 , noticeably higher than the values documented in Europe, North America, and East Asia. The tensite, 3-yr average total S deposition was 64.8 kg S ha −1 yr −1 , with 68 % attributed to dry deposition (mainly SO 2 ) and the rest to wet deposition. Consequently, the spatial distribution of the total flux was consistent to that of dry deposition, that is, higher values were observed at industrial and urban sites than at agricultural and rural sites. However, the seasonal variation in the total S deposition was not obvious across the entire year because of opposite seasonal trends in wet and dry deposition. It was found that the wet deposition, without significant spatial and interannual differences, was influenced by the volume of precipitation, the air-column concentrations of S compounds and in-cloud scavenging. Similar to the wet deposition, the dry-deposited sulfate was also less dependent on the surface concentration. Nevertheless, the regional differences in SO 2 dry deposition were mostly explained by the ambient concentration, which is closely associated with local emissions. As expected, the spatial pattern of total S deposition resembled that of the emission inventory, indicating the dramatic anthropogenic imprints on the regional S budget. Although at most of the study sites the "acid equivalents" deposition of S was comparable to that of nitrogen (N), the importance of S in the acidification risks was more pronounced at the industrial sites. The ten-site, 3-yr mean total "acid equivalents" deposition of S and N was estimated to be 8.4 (range: 4.2-11.6) keq ha −1 yr −1 , which exceeds the critical loads for natural ecosystems in Northern China. Taking these findings and our previous studies together, a multipollutant perspective and joint mitigation strategies to abate SO 2 and NH 3 simultaneously in the target area are recommended to protect natural ecosystems from excess acid deposition.
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