Journal of Atmospheric Chemistry最新文献

Hygroscopicity measurements of secondary organic aerosol (SOA) particles often show inconsistent results between the supersaturated and subsaturated regimes, with higher activity as cloud condensation nucleus (CCN) than indicated by hygroscopic growth. In this study, we have investigated the discrepancy between the two regimes in the Lund University (LU) smog chamber. Various anthropogenic SOA were produced from mixtures of different precursors: anthropogenic light aromatic precursors (toluene and m-xylene), exhaust from a diesel passenger vehicle spiked with the light aromatic precursors, and exhaust from two different gasoline-powered passenger vehicles. Three types of seed particles were used: soot aggregates from a diesel vehicle, soot aggregates from a flame soot generator and ammonium sulphate (AS) particles. The hygroscopicity of seed particles with condensed, photochemically produced, anthropogenic SOA was investigated with respect to critical supersaturation (s_c) and hygroscopic growth factor (gf) at 90% relative humidity. The hygroscopicity parameter κ was calculated for the two regimes: κ_sc and κ_gf, from measurements of s_c and gf, respectively. The two κ showed significant discrepancies, with a κ_gf /κ_sc ratio closest to one for the gasoline experiments with ammonium sulphate seed and lower for the soot seed experiments. Empirical observations of s_c and gf were compared to theoretical predictions, using modified K?hler theory where water solubility limitations were taken into account. The results indicate that the inconsistency between measurements in the subsaturated and supersaturated regimes may be explained by part of the organic material in the particles produced from anthropogenic precursors having a limited solubility in water.

This study reports for the first-time the ambient concentrations of HULIS mass (HULIS-OM, Humic-like substances) and HULIS-C (carbon) in PM₁₀ (particulate matter with aerodynamic diameter?≤?10?μm) from the Indo-Gangetic Plain (IGP at Kanpur, wintertime). HULIS extraction followed by purification and isolation protocol with methanol: acetonitrile (1:1?v/v) on HLB (Hydrophilic-Lipophilic Balanced) cartridge has been established. Quantification of HULIS-C was achieved on a total organic carbon (TOC) analyser whereas HULIS-OM was determined gravimetrically. Consistently high recovery (> 90%) of HULIS-C based on analysis of Humic standard (sodium salt of Humic acid) suggested suitability of our established analytical protocol involving solvent extraction, purification and accurate quantification of HULIS. HULIS-OM varied from 17.3–38?μg?m^?3 during daytime and from 19.8–40.6?μg?m^?3 during night in this study. During daytime the HULIS-OM constituted 20–30% mass fraction of OM_Total and 10–15% of PM₁₀ mass. However, a relatively low contribution of HULIS-OM has been observed during the night. This observation has been attributed to higher concentrations of OM and PM₁₀ in night owing to nighttime chemical reactivity and condensation of organics in conjunction with shallower planetary boundary layer height. Strong correlation of HULIS-C with K⁺_BB (R²?>?0.80) and significant day-night variability of HULIS-C/WSOC ratio in conjunction with air-mass back trajectories (showing transport of pollutants from upwind IGP) suggest biomass burning emission and secondary transformations as important sources of HULIS over IGP. High-loading of atmospheric PM₁₀ (as high as 440?μg?m^?3) with significant contribution of water-soluble organic aerosols (WSOC/OC: ~ 0.40–0.80) during wintertime highlights their plausible potential role in fog and haze formation and their impact on regional-scale atmospheric radiative forcing over the IGP.

Temporal variations in atmospheric hydrogen sulphide concentrations and its biosphere-atmosphere exchanges were studied in the World’s largest mangrove ecosystem, Sundarbans, India. The results were used to understand the possible contribution of H₂S fluxes in the formation of atmospheric aerosol of different size classes (e.g. accumulation, nucleation and coarse mode). The mixing ratio of hydrogen sulphide (H₂S) over the Sundarban mangrove atmosphere was found maximum during the post-monsoon season (October to January) with a mean value of 0.59?±?0.02?ppb and the minimum during pre-monsoon (February to May) with a mean value of 0.26?±?0.01?ppb. This forest acted as a perennial source of H₂S and the sediment-air emission flux ranged between 1213?±?276?μg?S?m^?2 d^?1(December) and 457?±?114?μg?S?m^?2 d^?1 (August) with an annual mean of 768?±?240?μg?S?m^?2d^?1. The total annual emissions of H₂S from the Indian Sundarban were estimated to be 1.2?±?0.6 Tg S. The accumulation mode of aerosols was found to be more enriched with non-sea salt sulfate with an average loading of 5.74?μg?m^?3 followed by the coarse mode (5.18?μg?m^?3) and nucleation mode (1.18?μg?m^?3). However, the relative contribution of Non-sea salt sulfate aerosol to total sulfate aerosol was highest in the nucleation mode (83%) followed by the accumulation (73%) and coarse mode (58%). Significant positive relations between H₂S flux and different modes of NSS indicated the likely link between H₂S, a dominant precursor for the non-sea salt sulfate, and non-sea sulfate aerosol particles. An increase in H₂S emissions from the mangrove could result in an increase in enhanced NSS in aerosol and associated cloud albedo, and a decrease in the amount of incoming solar radiation reaching the Sundarban mangrove forest.

PM₁₀ samples were collected to characterize the seasonal and annual trends of carbonaceous content in?PM₁₀ at an urban site of megacity Delhi, India from January 2010 to December 2017. Organic carbon (OC) and elemental carbon (EC) concentrations were quantified by thermal-optical transmission (TOT) method of PM₁₀ samples collected at Delhi. The average concentrations of PM₁₀, OC, EC and TCA (total carbonaceous aerosol) were 222?±?87 (range: 48.2–583.8?μg?m^?3), 25.6?±?14.0 (range: 4.2–82.5?μg?m^?3), 8.7?±?5.8 (range: 0.8–35.6?μg?m^?3) and 54.7?±?30.6?μg?m^?3 (range: 8.4–175.2?μg?m^?3), respectively during entire sampling period. The average secondary organic carbon (SOC) concentration ranged from 2.5–9.1 μg?m^?3 in PM₁₀, accounting from 14 to 28% of total OC mass concentration of PM₁₀. Significant seasonal variations were recorded in concentrations of PM₁₀, OC, EC and TCA with maxima during winter and minima during monsoon seasons. In the present study, the positive linear trend between OC and EC were recorded during winter (R²?=?0.53), summer (R²?=?0.59) and monsoon (R²?=?0.78) seasons. This behaviour suggests the contribution of similar sources and common atmospheric processes in both the fractions. OC/EC weight?ratio suggested that vehicular emissions, fossil fuel combustion and biomass burning could be the major sources of carbonaceous aerosols of PM₁₀ at the megacity Delhi, India. Trajectory analysis indicates that the air mass approches to the sampling site is mainly from Indo Gangetic plain (IGP) region (Uttar Pradesh, Haryana and Punjab etc.), Thar desert, Afghanistan, Pakistan and surrounding areas.

Aerosols consist of organic and inorganic species, and the composition and concentration of these species depends on their sources, chemical transformation and sinks. In this study an assessment of major inorganic ions determined in three aerosol particle size ranges collected for 1?year at Welgegund in South Africa was conducted. SO₄^2? and ammonium (NH₄⁺) dominated the PM₁ size fraction, while SO₄^2? and nitrate (NO₃) dominated the PM_1–2.5 and PM_2.5–10 size fractions. SO₄^2? had the highest contribution in the two smaller size fractions, while NO₃^? had the highest contribution in the PM_2.5–10 size fraction. SO₄^2? and NO₃^? levels were attributed to the impacts of aged air masses passing over major anthropogenic source regions. Comparison of inorganic ion concentrations to levels thereof within a source region influencing Welgegund, indicated higher levels of most species within the source region. However, the comparative ratio of SO₄^2? was significantly lower due to SO₄^2? being formed distant from SO₂ emissions and submicron SO₄^2? having longer atmospheric residencies. The PM at Welgegund was determined to be acidic, mainly due to high concentrations of SO₄^2?. PM₁ and PM_1–2.5 fractions revealed a seasonal pattern, with higher inorganic ion concentrations measured from May to September. Higher concentrations were attributed to decreased wet removal, more pronounced inversion layers trapping pollutants, and increases in household combustion and wild fires during winter. Back trajectory analysis also revealed higher concentrations of inorganic ionic species corresponding to air mass movements over anthropogenic source regions.

Atmospheric particle-bound mercury levels were measured in PM₁₀ aerosols (HgP) at a rural site (Mahasar, Haryana) during winter 2014–15 and summer 2015. The PM₁₀ HgP was determined by?using Differential Pulse Anodic Stripping Voltammetry through standard addition methods while the trace metals were determined by using an Atomic Absorption Spectroscopy. The mass concentrations of HgP varied from 591 to 1533?pg/m³ with an average of 1009?±?306?pg/m³ during the winter, while the mass concentrations of HgP varied from 43 to 826?pg/m³ with an average of 320?±?228?pg/m³ during the summer. However, it is difficult to assess whether these levels are harmful or not because there is no standard value available as National Ambient Air Quality Standard. The higher concentrations of HgP during winters were possibly due to favourable local meteorological conditions for the stagnation of particulate matter in the lower atmosphere and the increased emissions from existing natural or anthropogenic sources, regional sources and long-range transportation. Relatively low concentrations of HgP during summer might be due to increased mixing heights as well as scavenging effect because some light to heavy rain events were observed during summer time sampling. However, among other metals determined, the concentration of HgP was the lowest during both the seasons. The study may be useful in assessing the health impacts of PM₁₀ HgP and other metals.

In this work, the X-ray Photoelectron Spectroscopy (XPS) technique is utilized to analyze the surface chemical composition of particulate matter (PM) which was collected from various locations at Jeddah, Saudi Arabia. The main elements found on the surface of PM are carbon (C), oxygen (O) and silicon (Si) with combined percentage of 89.4–94.9 while traces of nitrogen (N), calcium (Ca), aluminum (Al), sodium (Na), chlorine (Cl), manganese (Mg), and sulfur (S) were also present. The analyzed XPS chemical state of C, O and Si was further used to determine their bonding with other elements occurring over the surface of PM. Carbon was found in the form of carbides (18.86%), fluorides (2.39%) and carbonates (78.75%); oxygen was observed as oxides (21.05%) and hydroxides (73.42%) of other metals; and silicon was detected as silicones (12.16%), nitrides (82.53%) and silicates (5.25%). The particle size of a PM is also of great concern for health issues, and thus has been investigated by the Field Emission Scanning Electron Microscope (FESEM). The Energy Dispersive X-ray Spectroscopy (EDS) was employed for cross verification of detected elements by XPS.

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.