Characterization of carbonaceous aerosols over Delhi in Ganga basin: seasonal variability and possible sources

The mass concentration of carbonaceous species, organic carbon (OC), and elemental carbon (EC) using a semicontinuous thermo-optical EC-OC analyzer, and black carbon (BC) using an Aethalometer were measured simultaneously at an urban mega city Delhi in Ganga basin from January 2011 to May 2012. The concentrations of OC, EC, and BC exhibit seasonal variability, and their concentrations were ～2 times higher during winter (OC 38.1?±?17.9 μg m^?3, EC 15.8?±?7.3 μg m^?3, and BC 10.1?±?5.3 μg m^?3) compared to those in summer (OC 14.1?±?4.3 μg m^?3, EC 7.5?±?1.5 μg m^?3, and BC 4.9?±?1.5 μg m^?3). A significant correlation between OC and EC (R?=?0.95, n?=?232) indicate their common emission sources with relatively lower OC/EC ratio (range 1.0–3.6, mean 2.2?±?0.5) suggests fossil fuel emission as a major source of carbonaceous aerosols over the station. On average, mass concentration of EC was found to be ～38 % higher than BC during the study period. The measured absorption coefficient (b_abs) was significantly correlated with EC, suggesting EC as a major absorbing species in ambient aerosols at Delhi. Furthermore, the estimated mass absorption efficiency (σ_abs) values are similar during winter (5.0?±?1.5 m² g^?1) and summer (4.8?±?2.8 m² g^?1). Significantly high aerosol loading of carbonaceous species emphasize an urgent need to focus on air quality management and proper impact assessment on health perspective in these regions.     

The characterization of water-soluble inorganic ions in PM2.5 during a winter period in Xi'an,China

The characteristics of water-soluble inorganic ions (WSIIs) during a winter period in a suburb of Xi'an, China, were investigated. Our results show that the total mass concentration of the dominant WSIIs (8) was 91.27 µg m^–3, accounting for 50.1% of the total mass concentration of PM_2.5 (particulates with a size of 2.5 µm or less). Secondary inorganic aerosols (SO₄^2?, NO₃^? and NH₄⁺) were the most abundant ions, accounting for up to 95.12% of the total ions. By using the anion and cation equivalence ratio method, PM_2.5 was shown to have weak alkalinity, and the chemical forms of WSIIs were mainly (NH₄)₂SO₄ and NH₄NO₃. The sulfur oxidation ratio (SOR) and nitrogen oxidation ratio (NOR) suggested that larger proportions of SO₄^2? and NO₃^? were formed by gas-phase SO₂ and NO₂ in the sampling site. Ratio analysis also indicated that anthropogenic sources significantly contributed to WSII pollution. Among the anthropogenic sources, fixed pollution sources were found to be dominant over mobile sources.     

Sources and characteristics of carbonaceous aerosols at Agra “World heritage site” and Delhi “capital city of India”

Agra, one of the oldest cities “World Heritage site”, and Delhi, the capital city of India are both located in the border of Indo-Gangetic Plains (IGP) and heavily loaded with atmospheric aerosols due to tourist place, anthropogenic activities, and its topography, respectively. Therefore, there is need for monitoring of atmospheric aerosols to perceive the scenario and effects of particles over northern part of India. The present study was carried out at Agra (AGR) as well as Delhi (DEL) during winter period from November 2011 to February 2012 of fine particulate (PM_2.5: d?<?2.5 μm) as well as associated carbonaceous aerosols. PM_2.5 was collected at both places using medium volume air sampler (offline measurement) and analyzed for organic carbon (OC) and elemental carbon (EC). Also, simultaneously, black carbon (BC) was measured (online) at DEL. The average mass concentration of PM_2.5 was 165.42?±?119.46 μg m^?3 at AGR while at DEL it was 211.67?±?41.94 μg m^?3 which is ~27 % higher at DEL than AGR whereas the BC mass concentration was 10.60 μg m^?3. The PM_2.5 was substantially higher than the annual standard stipulated by central pollution control board and United States Environmental Protection Agency standards. The average concentrations of OC and EC were 69.96?±?34.42 and 9.53?±?7.27 μm m^?3, respectively. Total carbon (TC) was 79.01?±?38.98 μg m^?3 at AGR, while it was 50.11?±?11.93 (OC), 10.67?±?3.56 μg m^?3 (EC), and 60.78?±?14.56 μg m^?3 (TC) at DEL. The OC/EC ratio was 13.75 at (AGR) and 5.45 at (DEL). The higher OC/EC ratio at Agra indicates that the formation of secondary organic aerosol which emitted from variable primary sources. Significant correlation between PM_2.5 and its carbonaceous species were observed indicating similarity in sources at both sites. The average concentrations of secondary organic carbon (SOC) and primary organic carbon (POC) at AGR were 48.16 and 26.52 μg m^?3 while at DEL it was 38.78 and 27.55 μg m^?3, respectively. In the case of POC, similar concentrations were observed at both places but in the case of SOC higher over AGR by 24 in comparison to DEL, it is due to the high concentration of OC over AGR. Secondary organic aerosol (SOA) was 42 % higher at AGR than DEL which confirms the formation of secondary aerosol at AGR due to rural environment with higher concentrations of coarse mode particles. The SOA contribution in PM_2.5 was also estimated and was ~32 and 12 % at AGR and DEL respectively. Being high loading of fine particles along with carbonaceous aerosol, it is suggested to take necessary and immediate action in mitigation of the emission of carbonaceous aerosol in the northern part of India.     

Identification and source apportionment of polycyclic aromatic hydrocarbons in ambient air particulate matter of Riyadh, Saudi Arabia

In an effort to assess the occurrence and sources of polycyclic aromatic hydrocarbons (PAHs) in the ambient air of Riyadh, Saudi Arabia, PM₁₀ samples were collected during December 2010. Diagnostic PAH concentration ratios were used as a tool to identify and characterize the PAH sources. The results reflect high PM₁₀ and PAH concentrations (particulate matter (PM)?=?270–1,270 μg/m³). The corresponding average PAH concentrations were in the range of 18?±?8 to 1,003?±?597 ng/m³ and the total concentrations (total PAHs (TPAHs) of 17 compounds) varied from 1,383 to 13,470 ng/m³ with an average of 5,871?±?2,830 ng/m³. The detection and quantification limits were 1–3 and 1–10 ng/ml, respectively, with a recovery range of 42–80 %. The ratio of the sum of the concentrations of the nine major non-alkylated compounds to the total (CPAHs/TPAHs) was 0.87?±?0.10, and other ratios were determined to apportion the PM sources. The PAHs found are characteristic for emissions from traffic with diesel being a predominant source.     

Carbonaceous and inorganic composition in long-range transported aerosols over northern Japan: Implication for aging of water-soluble organic fraction

To better understand the influence of sources and atmospheric processing on aerosol chemical composition, we collected atmospheric particles in Sapporo, northern Japan during spring and early summer 2005 under the air mass transport conditions from Siberia, China and surrounding seas. The aerosols were analyzed for inorganic ions, organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and the major water-soluble organic compound classes (i.e., dicarboxylic acids and sugars). SO₄^2? is the most abundant inorganic constituent (average 44% of the identified inorganic ion mass) followed by NH₄⁺ (21%) and NO₃^? (13%). Concentrations of OC, EC, and WSOC ranged from 2.0–16, 0.24–2.9, and 0.80–7.9 μg m^?3 with a mean of 7.4, 1.0, and 3.1 μg m^?3, respectively. High OC/EC ratios (range: 3.6–19, mean: 8.7) were obtained, however WSOC/OC ratios (0.23–0.69, 0.44) do not show any significant diurnal changes. These results suggest that the Sapporo aerosols were already aged, but were not seriously affected by local photochemical processes. Identified water-soluble organic compounds (diacids + sugars) account for <10% of WSOC. Based on some marker species and air mass back trajectory analyses, and using stable carbon isotopic compositions of shorter-chain diacids (i.e., C₂–C₄) as photochemical aging factor of organic aerosols, the present study suggests that a fraction of WSOC in OC is most likely influenced by aerosol aging, although the OC loading in aerosols may be more influenced by their sources and source regions.     

Photochemical production and loss of organic acids in high Arctic aerosols during long-range transport and polar sunrise ozone depletion events

Unique daily measurements of water-soluble organics in fine (<2 μm) and coarse (>2 μm) aerosols were conducted at Alert in the Canadian Arctic in winter to spring of 1992. They yield insight into photochemical production and loss of organics during long-range transport and ozone depletion events following polar sunrise. Comprehensive analyses of α, ω-dicarboxylic acids (C₂–C₁₂), ω-oxocarboxylic acids (C₂–C₉) and α-dicarbonyls (C₂, C₃) as well as pyruvic acid and aromatic (phthalic) diacid were conducted using GC and GC/MS techniques. Oxalic (C₂) acid was generally the dominant diacid species in both fine and coarse fractions, followed by malonic (C₃) and succinic (C₄) acids. Concentrations of total diacids in the fine aerosol fraction (0.2–64 ng m⁻³) were 5–60 times higher than those in the coarse fraction (0.01–3 ng m⁻³). After polar sunrise in early-March, the total concentration of fine aerosol diacids increased by a factor of 3–5 while the coarse mode did not change significantly. From dark winter to sunlit spring, temporal changes in correlations and ratios of these water-soluble organics to vanadium and sulfate measured simultaneously suggest that atmospheric diacids and related organic compounds are largely controlled by long-range atmospheric transport of polluted air during winter, but they are significantly affected by photochemical production. The latter can occur in sunlight either during transport to the Arctic or during photochemical events associated with surface ozone depletion and bromine chemistry near Alert in spring. Conversion of gaseous precursors to particulate matter via photochemical oxidation was intensified at polar sunrise, resulting in a peak in the ratio of total diacids to V. During ozone depletion events, complex patterns are indicated in photochemical production and loss depending on the diacid compound. Unsaturated (maleic and phthalic) diacids were inversely correlated with particulate Br whereas saturated diacids (C₂–C₄) positively correlated with particulate Br. These results suggest that Br chemistry associated with ozone depletion leads to degradation of unsaturated diacids and to the production of smaller saturated diacids.     

Factors determining the fluctuation of fluoride concentrations in PM10 aerosols in the urbanized coastal area of the Baltic Sea (Gdynia, Poland)

Fluoride concentrations were determined in PM10 samples collected in the urbanized coastal area of the Baltic Sea (Gdynia) in the period between 1 August 2008 and 8 January 2010. F^? concentrations remained within the range of 0.4–36.6 ng?·?m^?3. The economic transformations which have taken place in Poland increasing ecological awareness have had an excellent effect on the levels of fluoride pollution in the air of the studied region. In our measurements, fluoride concentrations increased in wintertime, when air temperature dropped, at low wind speeds (<1 m?·?s^?1) and with low dispersion of pollutants originating from local sources (traffic, industry, domestic heating). At times when wind speed grew to >10 m?·?s^?1, fluorides were related to marine aerosols or else brought from distant sources. Apart from wind speed and air temperature, other significant meteorological parameters which determined the variability of F^? turned out to be air humidity and precipitation volume. Aerosols were washed out effectively, even with small precipitation (h?=?4 mm), and if a dry period lasted for several days, their concentrations grew rapidly to over 30.0 ng?·?m^?3.     

Factors controlling benzo(a)pyrene concentration in aerosols in the urbanized coastal zone. A case study: Gdynia, Poland (Southern Baltic Sea)

Annual study on the benzo(a)pyrene (BaP) concentration in aerosols in the coastal zone of the Gulf of Gdansk (southern Baltic) has been performed at Gdynia station. Combustion processes, especially domestic heating of both local and regional origin, were identified as the main sources of benzo(a)pyrene in this area. Concentrations observed during the heating season (mean 2.18 ng?m^?3) were significantly higher than these recorded in the non-heating season (mean 0.05 ng?m^?3). High benzo(a)pyrene concentrations were associated with low temperature and high humidity. Whereas high levels of precipitation usually decreased the BaP concentration in aerosols. The concentration of this factor in the studied area depended also on the wind direction and air masses trajectories. During heating season, continental air masses (coming from S, SE, SW) seemed to increase benzo(a)pyrene concentration, while maritime air masses (from N, NE, NW) caused its decrease. The differences in the BaP concentration resulting from potentially different emission levels of this compound during working and non-working days were not clearly pronounced.     

Physicochemical variations in atmospheric aerosols recorded at sea onboard the Atlantic–Mediterranean 2008 Scholar Ship cruise (Part I): Particle mass concentrations,size ratios,and main chemical components

We report on ambient atmospheric aerosols present at sea during the Atlantic–Mediterranean voyage of Oceanic II (The Scholar Ship) in spring 2008. A record was obtained of hourly PM₁₀, PM_2.5, and PM₁ particle size fraction concentrations and 24-h filter samples for chemical analysis which allowed for comparison between levels of crustal particles, sea spray, total carbon, and secondary inorganic aerosols. On-board monitoring was continuous from the equatorial Atlantic to the Straits of Gibraltar, across the Mediterranean to Istanbul, and back via Lisbon to the English Channel. Initially clean air in the open Atlantic registered PM₁₀ levels <10 μg m^?3 but became progressively polluted by increasingly coarse PM as the ship approached land. Away from major port cities, the main sources of atmospheric contamination identified were dust intrusions from North Africa (NAF), smoke plumes from biomass burning in sub-Saharan Africa and Russia, industrial sulphate clouds and other regional pollution sources transported from Europe, sea spray during rough seas, and plumes emanating from islands. Under dry NAF intrusions PM₁₀ daily mean levels averaged 40–60 μg m^?3 (30–40 μg m^?3 PM_2.5; c. 20 μg m^?3 PM₁), peaking briefly to >120 μg m^?3 (hourly mean) when the ship passed through curtains of higher dust concentrations amassed at the frontal edge of the dust cloud. PM₁/PM₁₀ ratios ranged from very low during desert dust intrusions (0.3–0.4) to very high during anthropogenic pollution plume events (0.8–1).     

Quantitative chemical composition and characteristics of aerosols over western India: One-year record of temporal variability

One-year quantitative chemical data set consisting of water-soluble constituents (NH₄⁺, Na⁺, K⁺, Mg²⁺, Ca²⁺, Cl^?, NO₃^?, SO₄^2? and HCO₃^?), crustal and trace elements (Al, Fe, Ca, Mg, K, Mn, Zn, Pb) and carbonaceous species (OC, EC) in ambient aerosols, collected over an urban site located in a high-dust semi-arid region of western India, reveals excellent linear relationship (r² = 0.92; slope = 0.96 ± 0.05) between gravimetrically assessed TSP (total suspended particulates) and chemically analyzed aerosol mass. The TSP abundance ranging from 60 to 250 μg m^?3, over a period of 12 months (January–December), is dominated by mineral dust (～70%); whereas contribution from sea-salts, anthropogenic and carbonaceous species exhibits significant temporal variability depending upon the wind regimes. The mineral dust is enriched in Ca, Mg and Fe with respect to upper continental crust (UCC); whereas Zn and Pb exhibit a characteristic anthropogenic source and high enrichment factors. The carbonaceous species show significant seasonality; with dominance of OC (range: 4.6–28 μg m^?3; average: 12.8 μg m^?3; SD: 6.8) and minor contribution from EC (range: 0.3–4.4 μg m^?3; average: 2.4 μg m^?3; SD: 1.4). The observed concentrations are significantly lower than those reported for the metro cities in South Asia but the OC/EC ratios (range: 4.3–35; average: 8.3; SD: 5.7) are significantly higher than the characteristic ratio (～2–4) reported for the urban atmosphere. Such quantitative chemical characterization of aerosols is essential in assessing their role in atmospheric chemistry and climate change. This study could also be useful in understanding the physical and optical aerosol properties documented from the same site and thus, in validating regional climate models.     

Organic and inorganic components of aerosols over the central Himalayas: winter and summer variations in stable carbon and nitrogen isotopic composition

The aerosol samples were collected from a high elevation mountain site, Nainital, in India (1958 m asl) during September 2006 to June 2007 and were analyzed for water-soluble inorganic species, total carbon, nitrogen, and their isotopic composition (δ¹³C and δ¹⁵N, respectively). The chemical and isotopic composition of aerosols revealed significant anthropogenic influence over this remote free-troposphere site. The amount of total carbon and nitrogen and their isotopic composition suggest a considerable contribution of biomass burning to the aerosols during winter. On the other hand, fossil fuel combustion sources are found to be dominant during summer. The carbon aerosol in winter is characterized by greater isotope ratios (av. ?24.0?‰), mostly originated from biomass burning of C₄ plants. On the contrary, the aerosols in summer showed smaller δ¹³C values (?26.0?‰), indicating that they are originated from vascular plants (mostly of C₃ plants). The secondary ions (i.e., SO₄ ^2?, NH₄ ⁺, and NO₃ ^?) were abundant due to the atmospheric reactions during long-range transport in both seasons. The water-soluble organic and inorganic compositions revealed that they are aged in winter but comparatively fresh in summer. This study validates that the pollutants generated from far distant sources could reach high altitudes over the Himalayan region under favorable meteorological conditions.     

Source identification of inorganic airborne particle fraction (PM10) at ultratrace levels by means of INAA short irradiation

Many studies have focused their attention on the determination of elements of toxicological and environmental interest in atmospheric particulate matter using analytical techniques requiring chemical treatments. The instrumental nuclear activation analysis technique allows achieving high sensitivity, good precision, and excellent limit of detection without pretreatment, also considering the problems related to the radioisotope characteristics (e.g., half-life time, interfering reactions, spectral interferences). In this paper, elements such as Al, As, Br, Cl, Cu, I, La, Mg, Mn, Na, Sb, Si, Ti, and V are studied in atmospheric PM₁₀ sampled in downtown Rome: The relative radionuclides after activation of the sample are characterized by very short (ranging from 2.24 to 37.2 min) and short (ranging from 2.58 h to 2.70 days) half-lives. Furthermore, As, Br, La, Mn, and Sb were also determined for evaluating the aerosol characteristics. The results, elaborated considering the matrix effects and the interfering reaction contribution to the radioisotope formation (e.g., ²⁸Al generated by both (n,γ) reaction from ²⁷Al and (n,p) reaction from ²⁸Si), show interesting values of As (0.3–6.1 ng m^?3), Cu (22–313 ng m^?3), Mn (17–125 ng m^?3), V (7–63 ng m^?3), higher than those determined in an area not influenced by autovehicular traffic, and significant levels of I (1–11 ng m^?3) and Ti (25–659 ng m^?3) in Rome PM₁₀. The other elements show a pattern similar to the very few data present in the literature. It should be underlined the good correlation (r ²) of Al vs. Mg (0.915) and Al vs. La (0.726), indicating a same sources for these species as well as Br–Sb showing a little lower correlation (0.623). This last hypothesis is confirmed by the study of the enrichment factors: Sb and Br may be attributed to anthropogenic sources; Cu, Cl, and I show a mixed origin (natural and anthropogenic), whereas Al, Si, Ti, Mn, Na, Mg, and As are of crustal origin. For having more information, a statistical approach based on the principal component analysis and the canonical discriminant analysis has been performed: All the samples (except one) are grouped in a cluster, and elements such as As, Br, Cu, I, La, Mn, Sb, Ti, and V are highly correlated, whereas Na and Cl and Mg and Al assemble in two different clusters. Finally, a comparison with other similar studies is reported showing interesting values for Al, As, Mg, Mn, and Ti.     

Concentration and composition variations of metals in the outdoor PM10 of elementary schools during river dust episodes

Aeolian river dust can seriously affect the air quality in central Taiwan. The main purpose of this study was to assess the concentration variations of PM₁₀ and metals at different elementary schools during river dust episodes. River dust samples were taken from eight sites in the main bare soil areas of the Choshui River. PM₁₀ aerosols from four elementary schools in Yulin County were collected by means of high-volume samplers. Fifteen elements (Fe, Al, Ca, Mg, Mn, Zn, Ti, Ni, V, Cr, As, Pb, Cu, Co, and Cd) in the river dust and PM₁₀ were analyzed in this study. The coefficients of divergence (CDs) were obtained by comparing the metal compositions in PM₁₀ aerosols at the four schools on the sampling days with the mean metal contents in the river soil samples as reference. The CD values showed that metal compositions in the aerosols at high-exposure sites during river dust episodes were similar to those compositions in the river dust. The concentrations of PM₁₀ at the high-exposure schools during river dust episodes were much higher than those during non-river-dust episodes. This study also indicated that at the high-exposure sites, both the PM₁₀ and metal concentrations were higher than at the low-exposure and control sites, not only during the river dust episodes, but also after the river dust episodes. The concentrations of toxic metals (Ni, Cr, As, and Cd) at the high-exposure sites were about 11.3 times higher during the river dust episodes (189 ng/m³) than during non-river-dust episodes (16.7 ng/m³) and about 8.9 times higher during the same periods at the control site (21.3 ng/m³).     

Characterization of major pollution events (dust, haze, and two festival events) at Agra, India

Total suspended particulate (TSP) samples were collected during dust, haze, and two festival events (Holi and Diwali) from February 2009 to June 2010. Pollutant gases (NO₂, SO₂, and O₃) along with the meteorological parameters were also measured during the four pollution events at Agra. The concentration of pollutant gases decreases during dust events (DEs), but the levels of the gases increase during other pollution events indicating the impact of anthropogenic emissions. The mass concentrations were about two times higher during pollution events than normal days (NDs). High TSP concentrations during Holi and Diwali events may be attributed to anthropogenic activities while increased combustion sources in addition to stagnant meteorological conditions contributed to high TSP mass during haze events. On the other hand, long-range transport of atmospheric particles plays a major role during DEs. In the dust samples, Ca²⁺, Cl^?, NO₃ ^?, and SO₄ ^2? were the most abundant ions and Ca²⁺ alone accounted for 22 % of the total ionic mass, while during haze event, the concentrations of secondary aerosols species, viz., NO₃ ^?, SO₄ ^2?, and NH₄ ⁺, were 3.6, 3.3, and 5.1 times higher than the normal days. During Diwali, SO₄ ^2? concentration (17.8 μg?m^?3) was highest followed by NO₃ ^?, K⁺, and Cl^? while the Holi samples were strongly enriched with Cl^? and K⁺ which together made up 32.7 % of the total water-soluble ions. The ion balances indicate that the haze samples were acidic. On the other hand, Holi, Diwali, and DE samples were enriched with cations. The carbonaceous aerosol shows strong variation with the highest concentration during Holi followed by haze, Diwali, DEs, and NDs. However, the secondary organic carbon concentration follows the order haze > DEs > Diwali > Holi > NDs. The scanning electron microscope/EDX results indicate that KCl and carbon-rich particles were more dominant during Holi and haze events while DE samples were enriched with particles of crustal origin.     

Ionic composition of wet precipitation over the southern slope of central Himalayas,Nepal

Severe atmospheric pollution transported to Himalayas from South Asia may affect fragile ecosystem and can be harmful for human health in the region. In order to understand the atmospheric chemistry in the southern slope of central Himalayas, where the data is limited, precipitation has been sampled at four sites: Kathmandu (1,314 m), Dhunche (2,065 m), Dimsa (3,078 m), and Gosainkunda (4,417 m) in Nepal for over a 1-year period characterized by an urban, rural, and remote sites, respectively. HCO₃ ^? is the dominant anion, while the NH₄ ⁺ is the dominant cation in precipitation at the four sites. Generally, most of ions (e.g., SO₄ ^2?, NO₃ ^?, NH₄ ⁺, HCO₃ ^?, and Ca²⁺) have higher concentrations in urban site compared to the rural sites. Neutralization factor calculation showed that precipitation in the region is highly neutralized by NH₄ ⁺ and Ca²⁺. Empirical orthogonal function and correlation analysis indicated that the precipitation chemistry was mostly influenced by crustal, anthropogenic, and marine sources in Nepal. Among different sites, urban area was mostly influenced by anthropogenic inputs and crustal dusts, whereas remote sites were mostly from marine and crustal sources. Seasonal variations show higher ionic concentrations during non-monsoon seasons mainly due to limited precipitation amount. On the other hand, lower ionic concentrations were observed during monsoon season when higher amount of precipitation washes out aerosols. Thus, precipitation chemistry from this work can provide a useful database to evaluate atmospheric environment and its impacts on ecosystem in the southern slope of central Himalayas, Nepal.     

Spatial and temporal variations of nitrous oxide flux between coastal marsh and the atmosphere in the Yellow River estuary of China

To investigate the spatial and seasonal variations of nitrous oxide (N₂O) fluxes and understand the key controlling factors, we explored N₂O fluxes and environmental variables in high marsh (HM), middle marsh (MM), low marsh (LM), and mudflat (MF) in the Yellow River estuary throughout a year. Fluxes of N₂O differed significantly between sampling periods as well as between sampling positions. During all times of day and the seasons measured, N₂O fluxes ranged from ?0.0051 to 0.0805 mg N₂O m^?2 h^?1, and high N₂O emissions occurred during spring (0.0278 mg N₂O m^?2 h^?1) and winter (0.0139 mg N₂O m^?2 h^?1) while low fluxes were observed during summer (0.0065 mg N₂O m^?2 h^?1) and autumn (0.0060 mg N₂O m^?2 h^?1). The annual average N₂O flux from the intertidal zone was 0.0117 mg N₂O m^?2 h^?1, and the cumulative N₂O emission throughout a year was 113.03 mg N₂O m^?2, indicating that coastal marsh acted as N₂O source. Over all seasons, N₂O fluxes from the four marshes were significantly different (p?<?0.05), in the order of HM (0.0256?±?0.0040 mg N₂O m^?2 h^?1)?>?MF (0.0107?±?0.0027 mg N₂O m^?2 h^?1)?>?LM (0.0073?±?0.0020 mg N₂O m^?2 h^?1)?>?MM (0.0026?±?0.0011 mg N₂O m^?2 h^?1). Temporal variations of N₂O emissions were related to the vegetations (Suaeda salsa, Phragmites australis, and Tamarix chinensis) and the limited C and mineral N in soils during summer and autumn and the frequent freeze/thaw cycles in soils during spring and winter, while spatial variations were mainly affected by tidal fluctuation and plant composition at spatial scale. This study indicated the importance of seasonal N₂O contributions (particularly during non-growing season) to the estimation of local N₂O inventory, and highlighted both the large spatial variation of N₂O fluxes across the coastal marsh (CV?=?158.31 %) and the potential effect of exogenous nitrogen loading to the Yellow River estuary on N₂O emission should be considered before the annual or local N₂O inventory was evaluated accurately.     

Sources of submicron aerosol during fog-dominated wintertime at Kanpur

The main objective of this atmospheric study was to determine the major sources of PM₁ (particles having aerodynamic diameter <1.0 μm) within and near the city of Kanpur, in the Indo-Gangetic Plain. Day and night, 10 h long each, filter-based aerosol samples were collected for 4 months (November 2009 to February 2010) throughout the winter season. These samples were subjected to gravimetric and quantitative chemical analyses for determining water-soluble ions (NH₄ ⁺, F^?, Cl^?, NO₃ ^?, and SO₄ ^2?) using an ion chromatograph and trace elements using an inductively coupled plasma–optical emission spectrometer. The mean PM₁ mass concentrations were recorded as 114?±?71 μg/m³ (day) and 143?±?86 μg/m³ (night), respectively. A significantly higher diurnal contribution of ions (NH₄ ⁺, F^?, Cl^?, NO₃ ^?, and SO₄ ^2?) in PM₁ mass was observed during the fog-affected days and nights throughout the winter season, for which the average values were recorded as 38.09?±?13.39 % (day) and 34.98?±?12.59 % (night), respectively, of the total PM₁ mass. This chemical dataset was then used in a source-receptor model, UNMIX, and the model results are described in detail. UNMIX provided a maximum number of five source factors, including crustal material, composite vehicle, secondary aerosol, coal combustion, and iron/steel production and metallurgical industries, as the dominant air pollution sources for this study.     

Elevated nitrogen isotope ratios of tropical Indian aerosols from Chennai: Implication for the origins of aerosol nitrogen in South and Southeast Asia

To better understand the origins of aerosol nitrogen, we measured concentrations of total nitrogen (TN) and its isotope ratios (δ¹⁵N) in tropical Indian aerosols (PM₁₀) collected from Chennai (13.04°N; 80.17°E) on day- and night-time basis in winter and summer 2007. We found high δ¹⁵N values (+15.7 to +31.2‰) of aerosol N (0.3–3.8 μg m^?3), in which NH₄⁺ is the major species (78%) with lesser contribution from NO₃^? (6%). Based on the comparison of δ¹⁵N in Chennai aerosols with those reported for atmospheric aerosols from mid-latitudes and for the particles emitted from point sources (including a laboratory study), as well as the δ¹⁵N ratios of cow-dung samples (this study), we found that the atmospheric aerosol N in Chennai has two major sources; animal excreta and bio-fuel/biomass burning from South and Southeast Asia. We demonstrate that a gas-to-particle conversion of NH₃ to NH₄HSO₄ and (NH₄)₂SO₄ and the subsequent exchange reaction between NH₃ and NH₄⁺ are responsible for the isotopic enrichment of ¹⁵N in aerosol nitrogen.     

Chemical characteristics and source apportionment of PM<Subscript>2.5</Subscript> using PCA/APCS,UNMIX, and PMF at an urban site of Delhi,India

The present study investigated the comprehensive chemical composition [organic carbon (OC), elemental carbon (EC), water-soluble inorganic ionic components (WSICs), and major & trace elements] of particulate matter (PM_2.5) and scrutinized their emission sources for urban region of Delhi. The 135 PM_2.5 samples were collected from January 2013 to December 2014 and analyzed for chemical constituents for source apportionment study. The average concentration of PM_2.5 was recorded as 121.9 ± 93.2 μg m^?3 (range 25.1–429.8 μg m^?3), whereas the total concentration of trace elements (Na, Ca, Mg, Al, S, Cl, K, Cr, Si, Ti, As, Br, Pb, Fe, Zn, and Mn) was accounted for ～17% of PM_2.5. Strong seasonal variation was observed in PM_2.5 mass concentration and its chemical composition with maxima during winter and minima during monsoon seasons. The chemical composition of the PM_2.5 was reconstructed using IMPROVE equation, which was observed to be in good agreement with the gravimetric mass. Source apportionment of PM_2.5 was carried out using the following three different receptor models: principal component analysis with absolute principal component scores (PCA/APCS), which identified five major sources; UNMIX which identified four major sources; and positive matrix factorization (PMF), which explored seven major sources. The applied models were able to identify the major sources contributing to the PM_2.5 and re-confirmed that secondary aerosols (SAs), soil/road dust (SD), vehicular emissions (VEs), biomass burning (BB), fossil fuel combustion (FFC), and industrial emission (IE) were dominant contributors to PM_2.5 in Delhi. The influences of local and regional sources were also explored using 5-day backward air mass trajectory analysis, cluster analysis, and potential source contribution function (PSCF). Cluster and PSCF results indicated that local as well as long-transported PM_2.5 from the north-west India and Pakistan were mostly pertinent.     

Ammonia emissions from different pig production scales and their temporal variations in the North China Plain

ABSTRACT

Pig production systems in China are shifting from small to industrial scale. Significant variation in housing ammonia (NH₃) emissions can exist due to differences in diet, housing design, and management practices. However, there is a knowledge gap regarding the impacts of farm-scale in China, which may be critical in identifying hotspots and mitigation targets. Here, continuous in-situ NH₃ concentration measurements were made at pig farms of different scales for sows and fattening pigs over periods of 3–6 days during two different seasons (summer vs. winter). For the sow farms, NH₃ emission rates were greater at the small farm (summer: 0.52 g pig^?1 hr^?1; winter: 0.21 g pig^?1 hr^?1) than at the large farm (summer: 0.34 g pig^?1 hr^?1; winter: 0.12 g pig^?1 hr^?1). For the fattening pig farms, NH₃ emission rates were greater at the large farm (summer: 0.22 g pig^?1 hr^?1; winter: 0.16 g pig^?1 hr^?1) than at the small farm (summer: 0.19 g pig^?1 hr^?1; winter: 0.07 g pig^?1 hr^?1). Regardless of farm scale, the NH₃ emission rates measured in summer were greater than those in winter; the NH₃ emission rates were greater in the daytime than at the nighttime; a positive relationship (R² = 0.06–0.68) was established between temperature and NH₃ emission rate, whereas a negative relationship (R² = 0.10–0.47) was found between relative humidity and NH₃ emission rate. The effect of farm-scale on indoor NH₃ concentration could mostly be explained by the differences in ventilation rates between farms. The diurnal variation in NH₃ concentration could be partly explained by ventilation rate (R² = 0.48–0.78) in the small traditional farms and by emission rate (R² = 0.26–0.85) in the large industrial farms, except for the large fattening pig farm in summer. Overall, mitigation of NH₃ emissions from sow farms should be a top priority in the North China Plain.

Implications: The present study firstly examined the farm-scale effect of ammonia emissions in the North China Plain. Of all farms, the sow farm was identified as the greatest source of ammonia emission. Regardless of farm scale, ammonia emission rates were observed to be higher in summer. Ammonia concentrations were mostly higher in the large industrial farms partly due to lower ventilation rates than in the small traditional farms.