Journal of Atmospheric Chemistry最新文献

To explore the freezing effect on iron (Fe) solubility in natural environments, especially in Polar regions, event based freshly fallen snow samples were collected at Newark, New Jersey on the US East Coast for two consecutive winter seasons (2014–2015 and 2015–2016). These samples were analyzed for the concentrations of soluble iron (Fe_sol) using UV-Vis Spectroscopy and filterable iron (Fe_fil) and total iron (Fe_tot) using Atomic Absorption Spectroscopy. The average fractional solubility of the Fe_sol (the portion that passes through a 0.22?μm pore-size filter) with respect to the total Fe in the samples was 23.3?±?12.2%, with the majority of the soluble Fe being present as Fe(III). Approximately 48.5% of the total Fe existed as Fe_fil (the portion that passes through 0.45?μm pore size filter media). No significant correlation was found between the soluble ionic species and soluble Fe. Six snow events were kept frozen for 10?days, and analyzed in periodic intervals to study the post-freezing modification in Fe solubility. Events 1 and 2 showed increasing trend in the soluble Fe concentrations; however, the events 5, 6, 7, and 8 showed no noticeable increments. The pattern shown in Events 1 and 2 is associated with high fraction of Fe_fil and one unit pH drop, suggesting that the freeze-induced modification in Fe solubility could be linked with the amount of Fe_fil and the acidity change in the samples. To further investigate the freeze-induced compaction of particles, samples from three events 6, 7, and 10 were analyzed by SEM-STEM-EDS microscopy, and the results showed that due to freezing, in general, the particles in the ice-melt counterparts tend to compact and cluster and form larger aggregates compared to the particles in snow-melt. These results show, despite the freeze-induced compaction in snow was observed from STEM images, the snow freezing might not have significant effect in increasing Fe solubility from materials in the snow. These results further suggest that freezing process with fresh snow in high-latitude regions may not impose significant modification on Fe solubility in snow.

APEC blue was coined to describe the impact of short-term curbs on air pollution during the Asian-Pacific Economic Cooperation (APEC) Summit organized in Beijing in November 2014 and has been a hot topic among both general public and scientific sector in China. The consensus that gaseous agents NO₂ and SO₂ are greatly reduced in response to the control and restriction strategies implemented during the Summit period is shared by earlier literature. However, the re-examination of APEC blue conducted in the present study comes to a more contrasted conclusion. The remarkable drop in NO₂ abundances is confirmed in terms of both surface concentration and vertical column, whereas corresponding SO₂ changes are found to be marginal and not statistically significant, indicating that the decline of SO₂ was more tied to natural or random variability rather than externally forced. To explain the contrasted responses of NO₂ and SO₂ during the APEC summit, short-term variations of these species are further placed in the context of a longer term perspective, which reveals a striking contrast in the pathways of the secular tendency in NO₂ and SO₂ emissions and corresponding measured abundances of both pollutants. On the one hand, NO₂ emissions exhibit a sharp rise by 30–50% from 2006-2010 to 2011–2014; on the other hand, SO₂ emissions have undergone a gradual decrease in the last decade and have currently returned to their pre-2000 level. Therefore, short-term control measures are expected to be more effective in reducing the levels of NO₂ than SO₂.

Ambient concentrations of organic carbon (OC), elemental carbon (EC) and water soluble inorganic ionic components (WSIC) of PM₁₀ were studied at Giridih, Jharkhand, a sub-urban site near the Indo Gangatic Plain (IGP) of India during two consecutive winter seasons (November 2011–February 2012 and November 2012–February 2013). The abundance of carbonaceous and water soluble inorganic species of PM₁₀ was recorded at the study site of Giridih. During winter 2011–12, the average concentrations of PM₁₀, OC, EC and WSIC were 180.2?±?46.4; 37.2?±?6.2; 15.2?±?5.4 and 18.0?±?5.1?μg m^?3, respectively. Similar concentrations of PM₁₀, OC, EC and WSIC were also recorded during winter 2012–13. In the present case, a positive linear trend is observed between OC and EC at sampling site of Giridih indicates the coal burning, as well as dispersed coal powder and vehicular emissions may be the source of carbonaceous aerosols. The principal components analysis (PCA) also identifies the contribution of coal burning??+?soil dust, vehicular emissions?+?biomass burning and seconday aerosol to PM₁₀ mass concentration at the study site. Backward trajectoy and potential source contributing function (PSCF) analysis indicated that the aerosols being transported to Giridih from upwind IGP (Punjab, Haryana, Uttar Pradesh and Bihar) and surrounding region.

Nitrogen-containing organic compounds (NOC) formed from secondary organic aerosols (SOA) age via reaction with reduced nitrogen species are a vital class of brown carbon compounds. NOC compounds from ammonia (NH₃) gas-aging of benzene SOA were investigated in present study, and the experiments were performed by irradiating benzene/CH₃ONO/NO/NH₃ air mixtures in a home-made smog chamber. The particulate NOC products of aged benzene SOA in the presence of NH₃ were measured by UV-Vis spectrophotometer, attenuated total reflectance-Fourier transform infrared (ATR-FTIR), and aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with Fuzzy C-Means (FCM) clustering algorithm, respectively. Experimental results demonstrated that NH₃ has significant promotion effect on benzene SOA formation. Organic ammonium salts, such as ammonium glyoxylate, ammonium 6-oxo-2,4-hexadienoiclate, which are formed from NH₃ reactions with gaseous organic acids were detected as the major particulate NOC products of NH₃-aged benzene SOA. 1H–imidazole, 1H–imidazole-2-carbaldehyde and other imidazole products via the heterogeneous reactions between NH₃ and dialdehydes of benzene SOA were successfully detected as important brown carbon constituents. The formation of imidazole products suggests that some ambient particles contained organonitrogen compounds may be come from this mechanism. The results of this study may provide valuable information for discussing NH₃ deposition and SOA aging mechanisms.

Three online coupled chemical transport model simulations were analyzed for three summer months of 2015 in Poland. One of them was run with default emission inventory, the other two with NO_x and VOC emissions reduced by 30%, respectively. Obtained ozone concentrations were evaluated with data from air quality measurement stations and ozone sensitivity to precursor emissions was estimated by ozone concentration differences between simulations and with the use of indicator ratios. They were calculated based on modeled mixing ratios of ozone, total reactive nitrogen and its components, nitric acid and hydrogen peroxide. The results show that the model overestimates ozone concentrations with the largest errors in the morning and evening, which is primarily related to the way vertical mixing is resolved by the model. Better model performance for ozone is achieved in rural than urban environment, as PBL and mixing mechanisms play more significant role in urban areas. Modeled ozone shows mixed sensitivity to precursor concentrations, similarly to other European regions, but indicator ratios have different values than are found in literature, particularly H₂O₂/HNO₃ is larger than in southern Europe. However, indicator ratios often differ between locations and transition values need to be established individually for a given region.

During the MILAGRO campaign, March 2006, eight-stage cut impactors were used to sample atmospheric particles at Tecámac (T1 supersite), towards the northeast edge of the Mexico City Metropolitan Area, collecting fresh local emissions and aged pollutants produced in Mexico City. Particle samples were analyzed to determine total mass concentrations of Ca²⁺, Mg²⁺, NH₄ ⁺, K⁺, Cl^?, SO₄ ^2?, and NO₃ ^?. Average concentrations were 22.1?±?7.2?μg m^?3 for PM₁₀ and 18.3?±?6.2?μg m^?3 for PM_1.8. A good correlation between PM₁₀ and PM_1.8, without influence from wind patterns, indicates that local emissions are more important than the city’s pollution transported to the site, despite the fact that Tecámac is just 40?km away from Mexico City. A lack of diurnal patterns in the PM_2.5/PM_1.8 ratio supports this conclusion. The inorganic composition of particles suggests that vehicles, soil resuspension, and industries are the main pollutant sources. Finally, the particles were found to be neutralized, in agreement with observations in the Mexico City Metropolitan Area.

Dibromomethane (CH₂Br₂), a natural stratospheric ozone depleting substance, is mostly emitted from the ocean, but the relative importance of coastal (or macroalgae) and open ocean emissions is unknown. We made long-term high-frequency measurements of CH₂Br₂ concentrations at two remote coastal sites in Japan, on the subtropical Hateruma Island (poor in macroalgae) and at Cape Ochiishi (rich in macroalgae). CH₂Br₂ concentrations at Hateruma showed prominent seasonal variation, being lower in summer (around 0.94 ppt) than in winter (around 1.23 ppt). In contrast, CH₂Br₂ concentrations at Ochiishi were highly variable, often exceeding 2 ppt in the summer but with minimum baseline concentrations close to those from Hateruma; in the winter the concentrations were almost constant at about 1.3 ppt. Analysis of the data suggested that (1) emissions from macroalgae were not likely to extend offshore, but instead were localized near the shore, (2) strong macroalgal emissions of CH₂Br₂ were almost limited to the summer, but it was not reflected in the seasonality of the baseline concentrations of CH₂Br₂ in the atmosphere, and therefore (3) macroalgal or coastal emissions of CH₂Br₂ in the temperate zone might have a rather limited contribution to the global CH₂Br₂ sources. These findings are especially important for the understanding of the tropospheric and stratospheric bromine budget.

Measurements of the concentrations of H₂O₂ and methyl hydroperoxide (MHP), O₃, and SO₂ over Imizu City, Toyama Prefecture, Japan were performed in March using a helicopter. H₂O₂ concentrations were higher at an altitude of approximately 2,400 m (8,000 ft). The H₂O₂ concentrations (< 0.8 ppb) in the spring were much lower than those observed during the summer observations. MHP was also higher in the high-altitude atmosphere. Lower concentrations of H₂O₂ were observed when high air pollutants were actively transported from Asian continent. The concentrations of H₂O₂ were mostly lower than those of SO₂; this condition is called oxidant limitation. If H₂O₂ concentration rises in cold months, the acidification of cloud water may be accelerated at high elevations in central Japan where air pollution is actively transported.

To determine the effects of long-range transport of aerosols from an upwind area in East Asia to a downwind area in Japan, we chemically analyzed aerosols collected simultaneously on Tuoji Island (Shandong Province, China), Fukue Island (Nagasaki Prefecture, Japan), and Cape Hedo (Okinawa Prefecture, Japan). We focused on changes in the metallic composition of PM_2.5 aerosols during long-range transport. The average mass concentrations of PM_2.5 at the three sites decreased in the order Tuoji Island > Fukue Island ≈ Cape Hedo (48.3 ± 4.5, 13.9 ± 1.5, and 13.2 ± 0.9 μg/m³, respectively). The fraction of coarse particles in total suspended particles estimated by (1–PM_2.5/TSP) was highest on Cape Hedo, indicating that the contribution of sea salts was increased by long-range transport of the aerosols over the ocean. Enrichment factor analysis revealed that at all three sites, Al, K, Ca, Mn, Fe, Co, Sr, and Ba originated from soil; whereas Cr, Ni, Cu, Zn, As, Mo, Ag, Cd, Sn, Sb, Tl, and P appeared to be of anthropogenic origin. Na was the most abundant element on Cape Hedo, indicating the addition of sea salts during aerosol transport. The V concentration was highest at Fukue Island, which was ascribed to V emission from ships. Sixty-one percent of the V on Fukue Island and 62% of the V on Cape Hedo were determined to have originated from ships, implicating of data obtained on dates during which backward trajectory analysis indicated that the same air mass passed over Tuoji Island, Fukue Island, and Cape Hedo in that order.