Effect of temperature on the methyl chloride production rate in a marine phytoplankton, <Emphasis Type="Italic">Phaeodactylum tricornutum</Emphasis>

Methyl halides such as methyl chloride (CH₃Cl) are known to be important carriers of halogen from the ocean to the atmosphere, and the halogens they release into the stratosphere by photolysis catalyze ozone depletion. Marine phytoplankton have been reported as a source of CH₃Cl, but the effects of environmental temperature on the CH₃Cl production by phytoplankton have not been investigated. In this study, we investigated the effects of temperature on the production of CH₃Cl in the culture of a marine diatom, Phaeodactylum tricornutum CCMP 630, incubated at 10, 15, 20, 25, and 30 °C. CH₃Cl concentrations in cultured samples were determined using purge and trap gas chromatograph–mass spectrometry. Phytoplankton growth was monitored by measuring the chlorophyll a concentrations. CH₃Cl production was observed for several weeks at four different temperatures ranging from 10 to 25 °C. The CH₃Cl production from P. tricornutum was increased with increasing temperature from 10 to 25 °C, and the maximum production rate for CH₃Cl was 0.21~0.26 μmol (g chlorophyll a)^?1 d^?1 at 25 °C, which was several times higher than that at 10 °C (~0.03 μmol (g chlorophyll a)^?1 d^?1). The Arrhenius equation was successfully used to characterize the effects of temperature on the production rates of CH₃Cl in the culture of P. tricornutum. Our results suggest that water temperature directly affects CH₃Cl production derived from P. tricornutum and that water temperature would be a significant factor for estimating the emissions of CH₃Cl from marine environments.     

Estimate of Hydrofluorocarbon Emissions for 2012–16 in the Yangtze River Delta,China

Hydrofluorocarbons(HFCs) have been widely used in China as substitutes for ozone-depleting substances,the production and use of which are being phased out under the Montreal Protocol.China is a major consumer of HFCs around the world,with its HFC emissions in CO_2-equivalent contributing to about 18% of the global emissions for the period2012-16.Three methods are widely used to estimate the emissions of HFCs-namely,the bottom-up method,top-down method and tracer ratio method.In this study,the tracer ratio method was adopted to estimate HFC emissions in the Yangtze River Delta(YRD),using CO as a tracer.The YRD region might make a significant contribution to Chinese totals owing to its rapid economic growth.Weekly flask measurements for ten HFCs(HFC-23,HFC-32,HFC-125,HFC-134 a,HFC-143 a,HFC-152 a,HFC-227 ea,HFC-236 fa,HFC-245 fa and HFC-365 mfc) were conducted at Lin'an Regional Background Station in the YRD over the period 2012-16,and the HFC emissions were 2.4±1.4 Gg yr~(-1) for HFC-23,2.8±1.2 Gg yr~(-1) for HFC-32,2.2±1.2 Gg yr~(-1) for HFC-125,4.8±4.8 Gg yr~(-1) for HFC-134 a,0.9±0.6 Gg yr~(-1) for HFC-152 a,0.3±0.3 Gg yr~(-1) for HFC-227 ea and 0.3±0.2 Gg yr~(-1) for HFC-245 fa.The YRD total HFC emissions reached 53 Gg CO_2-e yr~(-1),contributing 34% of the national total.The per capita HFC CO_2-equivalent emissions rate was 240 kg yr-1,while the values of per unit area emissions and per million GDP emissions reached 150 Mg km~(-2)yr~(-1) and 3500 kg yr~(-1)(million CNY GDP)-1,which were much higher than national or global levels.     

Impact of intensive fish farming on methane emission in a tropical hydropower reservoir

Fisheries and aquaculture are important sources of food for hundreds of millions of people around the world. World fish production is projected to increase by 15% in the next 10 years, reaching around 200 million tonnes per year. The main driver of this increase will be based on fish farming management in developing countries. In Brazil, fish farming is increasing due to the climate conditions and large supply of water resources, with the production system based on Nile tilapia (Oreochromis niloticus) farming in reservoirs. Inland waters like reservoirs are a natural source of methane (CH₄) to the atmosphere. However, knowledge of the impact from intensive fish production in net cages on CH₄ fluxes is not well known. This paper presents in situ measurements of CH₄ fluxes and dissolved CH₄ (DM) in the Furnas Hydroelectric Reservoir in order to evaluate the impact of fish farming on methane emissions. Measurements were taken in a control area without fish production and three areas with fish farming. The overall mean of diffusive methane flux (DMF) (5.9?±?4.5 mg CH₄ m^?2 day^?1) was significantly lower when compared to the overall mean of bubble methane flux (BMF) (552.9?±?1003.9 mg CH₄ m^?2 day^?1). The DMF and DM were significantly higher in the two areas with fish farming, whereas the BMF was not significantly different. The DMF and DM were correlated to depth and chlorophyll-a. However, the low production of BMF did not allow the comparison with the limnological parameters measured. This case study shows that CH₄ emissions are influenced more by reservoir characteristics than fish production. Further investigation is necessary to assess the impact of fish farming on the greenhouse gas emissions.     

A nocturnal atmospheric loss of CH<Subscript>2</Subscript>I<Subscript>2</Subscript> in the remote marine boundary layer

Ocean emissions of inorganic and organic iodine compounds drive the biogeochemical cycle of iodine and produce reactive ozone-destroying iodine radicals that influence the oxidizing capacity of the atmosphere. Di-iodomethane (CH₂I₂) and chloro-iodomethane (CH₂ICl) are the two most important organic iodine precursors in the marine boundary layer. Ship-borne measurements made during the TORERO (Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOC) field campaign in the east tropical Pacific Ocean in January/February 2012 revealed strong diurnal cycles of CH₂I₂ and CH₂ICl in air and of CH₂I₂ in seawater. Both compounds are known to undergo rapid photolysis during the day, but models assume no night-time atmospheric losses. Surprisingly, the diurnal cycle of CH₂I₂ was lower in amplitude than that of CH₂ICl, despite its faster photolysis rate. We speculate that night-time loss of CH₂I₂ occurs due to reaction with NO₃ radicals. Indirect results from a laboratory study under ambient atmospheric boundary layer conditions indicate a k _CH2I2+NO3 of ≤4 × 10^?13 cm³ molecule^?1 s^?1; a previous kinetic study carried out at ≤100 Torr found k _CH2I2+NO3 of 4 × 10^?13 cm³ molecule^?1 s^?1. Using the 1-dimensional atmospheric THAMO model driven by sea-air fluxes calculated from the seawater and air measurements (averaging 1.8 +/? 0.8 nmol m^?2 d^?1 for CH₂I₂ and 3.7 +/? 0.8 nmol m^?2 d^?1 for CH₂ICl), we show that the model overestimates night-time CH₂I₂ by >60 % but reaches good agreement with the measurements when the CH₂I₂ + NO₃ reaction is included at 2–4 × 10^?13 cm³ molecule^?1 s^?1. We conclude that the reaction has a significant effect on CH₂I₂ and helps reconcile observed and modeled concentrations. We recommend further direct measurements of this reaction under atmospheric conditions, including of product branching ratios.     

Assessment of PM<Subscript>2.5</Subscript> chemical compositions in Delhi: primary vs secondary emissions and contribution to light extinction coefficient and visibility degradation

Haze-fog conditions over northern India are associated with visibility degradation and severe attenuation of solar radiation by airborne particles with various chemical compositions. PM_2.5 samples have been collected in Delhi, India from December 2011 to November 2012 and analyzed for carbonaceous and inorganic species. PM₁₀ measurements were made simultaneously such that PM_10–2.5 could be estimated by difference. This study analyzes the temporal variation of PM_2.5 and carbonaceous particles (CP), focusing on identification of the primary and secondary aerosol emissions, estimations of light extinction coefficient (b_ext) and the contributions by the major PM_2.5 chemical components. The annual mean concentrations of PM_2.5, organic carbon (OC), elemental carbon (EC) and PM_10–2.5 were found to be 153.6 ± 59.8, 33.5 ± 15.9, 6.9 ± 3.9 and 91.1 ± 99.9 μg m^?3, respectively. Total CP, secondary organic aerosols and major anions (e.g., SO₄ ^2? and NO₃ ^?) maximize during the post-monsoon and winter due to fossil fuel combustion and biomass burning. PM_10–2.5 is more abundant during the pre-monsoon and post-monsoon. The OC/EC varies from 2.45 to 9.26 (mean of 5.18 ± 1.47), indicating the influence of multiple combustion sources. The b_ext exhibits highest values (910 ± 280 and 1221 ± 371 Mm^?1) in post-monsoon and winter and lowest in monsoon (363 ± 110 and 457 ± 133 Mm^?1) as estimated via the original and revised IMPROVE algorithms, respectively. Organic matter (OM =1.6 × OC) accounts for ~39 % and ~48 % of the b_ext, followed by (NH₄)₂SO₄ (~21 % and ~24 %) and EC (~13 % and ~10 %), according to the original and revised algorithms, respectively. The b_ext estimates via the two IMPROVE versions are highly correlated (R² = 0.95, root mean square error = 38 % and mean bias error = 28 %) and are strongly related to visibility impairment (r = ?0.72), mostly associated with anthropogenic rather than natural PM contributions. Therefore, reduction of CP and precursor gas emissions represents an urgent opportunity for air quality improvement across Delhi.     

Characteristics, loss and gain of atmospheric carbonyl compounds in winters of 2008–2010 in Pearl River Delta region, China

Formaldehyde (HCHO), acetaldehyde (CH₃CHO) and acetone (CH₃COCH₃) were measured at Wanqingsha (WQS) in south China during November-December 2008–2010. Carbonyl compound pollution characteristics under the influence of the financial crisis (FC) were studied. Atmospheric carbonyl compound concentrations in the 2008 and 2009 sampling periods were affected by the 2008 FC. The industrial downturn plus the high closing down number of the small enterprises with limited emission treatment during the FC played an important role in the reduction of the industry-related CH₃CHO and CH₃COCH₃. In 2010, the recovery of industrial activities occurred, but affected by traffic restriction enforcement in Guangzhou over the Asian Games period, HCHO concentration (daytime 7.59?±?2.59 μg m^?3) was lower than expectation. Carbonyl compounds in WQS site were highly influenced by regional pollution transport from different upwind urban cities and industrial districts in the north-northwest to northeast wind sector in winter. Also, the interaction of the winter monsoon with the warm ocean along the coastline as well as day and night boundary layer mixing height variation affected carbonyl compound concentrations in WQS. The daytime mean dry deposition losses of HCHO and CH₃CHO were first time model-estimated for 2009 and 2010. For loss of HCHO in the early afternoon, photolysis was the dominant sink, followed by dry deposition and removal by OH radical (?OH), while for CH₃CHO, dry deposition was dominant. For the gain of HCHO and CH₃CHO, the production rates during early afternoon in 2009 and 2010 were estimated by an indirect approach.     

Estimation of Nocturnal Area Fluxes of Carbon Cycle Gases in Saint Petersburg Suburbs

Carbon dioxide, methane, and carbon monoxide are the carbon cycle gases, the data on their emissions are needed when monitoring air pollution and developing methods for reducing anthropogenic emissions to the atmosphere and for climate forecasting. The estimates of nocturnal area fluxes for CO₂, CH₄, and CO presented for a suburb of Saint Petersburg (Peterhof) are obtained using the box model and continuous observations of concentration of these gases. The mean values of CH₄, CO₂, and CO fluxes estimated for Peterhof for 2014–2015 are 44 ± 27, 6100 ± 4000, and 90 ± 100 t/(km² year), respectively. The intensity of the CO area flux has pronounced seasonal variations characterized by the maximum of ~(160 ± 120) t/(km² year) in November—February and by the minimum of ~(30 ± 20) t/(km² year) in June-July. The analysis of the ratio of CO/CO₂ fluxes identified the main types of anthropogenic sources typical of Peterhof: motor transport, natural gas combustion, and the use of wood stoves for the heating of private low-rise buildings (in the cold season).     

Biogenic hydrogen sulphide emissions and non-sea sulfate aerosols over the Indian Sundarban mangrove forest

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.     

AGAGE Observations of Methyl Bromide and Methyl Chloride at Mace Head, Ireland, and Cape Grim, Tasmania, 1998–2001

In situ AGAGE GC-MS measurements of methyl bromide (CH₃Br) and methyl chloride (CH₃Cl) at Mace Head, Ireland and Cape Grim, Tasmania (1998–2001) reveal a complex pattern of sources. At Mace Head both gases have well-defined seasonal cycles with similar average annual decreases of 3.0% yr⁻¹ (CH₃Br) and 2.6% yr⁻¹ (CH₃Cl), and mean northern hemisphere baseline mole fractions of 10.37 ± 0.05 ppt and 535.7 ± 2.2 ppt, respectively. We have used a Lagrangian dispersion model and local meteorological data to segregate the Mace Head observations into different source regions, and interpret the results in terms of the known sources and sinks of these two key halocarbons. At Cape Grim CH₃Br and CH₃Cl also show annual decreases in their baseline mixing ratios of 2.5% yr⁻¹ and 1.5% yr⁻¹, respectively. Mean baseline mole fractions were 7.94 ± 0.03 ppt (CH₃Br) and 541.3 ± 1.1 ppt (CH₃Cl). Although CH₃Cl has astrong seasonal cycle there is no well-defined seasonal cycle in the Cape Grim CH₃Br record. The fact that both gases are steadily decreasing in the atmosphere at both locations implies that a change has occurred which is affecting a common, major source of both gases (possibly biomass burning) and/or their major sink process (destruction by hydroxyl radical).     

Carbonaceous and inorganic species in PM<Subscript>10</Subscript> during wintertime over Giridih,Jharkhand (India)

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.     

Photochemical activation of chlorine by iron-oxide aerosol

The photochemical activation of chlorine by dissolved iron in artificial sea-salt aerosol droplets and by highly dispersed iron oxide (Fe₂O₃) aerosol particles (mainly hematite, specific surface ~150 m² g^?1) exposed to gaseous HCl, was investigated in humidified air in a Teflon simulation chamber. Employing the radical-clock technique, we quantified the production of gaseous atomic chlorine (Cl) from the irradiated aerosol. When the salt aerosol contained Fe₂O₃ at pH 6, no significant Cl production was observed, even if the dissolution of iron was forced by “weathering” (repeatedly freezing and thawing for five times). Adjusting the pH in the stock suspension to 2.6, 2.2, and 1.9 and equilibrating for one week resulted in a quantifiable amount of dissolved iron (0.03, 0.2, and 0.6 mmol L^?1, respectively) and in gaseous Cl production rates of ~1.6, 6, and 8?×?10²¹ atoms cm^?2 h^?1, respectively. In a further series of experiments, the pure Fe₂O₃ aerosol was exposed to various levels of gaseous hydrogen chloride (HCl). The resulting Cl production rates ranged from 8?×?10²⁰ Cl atoms cm^?2 h^?1 (at ~4 ppb HCl) to 5?×?10²² Cl atoms cm^?2 h^?1 (at ~350 ppb HCl) and confirmed the uptake and conversion of HCl to atomic Cl (at HCl to Cl conversion yields of 2–5 %, depending on the relative humidity). The Fe₂O₃ experiments indicate that iron-induced Cl formation may be important for highly soluble combustion-aerosol particles in marine environments in the presence of gaseous HCl.     

Water-soluble inorganic ions of size-differentiated atmospheric particles from a suburban site of Mexico City

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.     

Atmospheric ionic species in PM2.5 and PM1 aerosols in the ambient air of eastern central India

This study elucidates the characteristics of ambient PM_2.5 (fine) and PM₁ (submicron) samples collected between July 2009 and June 2010 in Raipur, India, in terms of water soluble ions, i.e. Na⁺, NH ₄ ⁺ , K⁺, Mg²⁺, Ca²⁺, Cl^?, NO ₃ ^? and SO ₄ ^2? . The total number of PM_2.5 and PM₁ samples collected with eight stage cascade impactor was 120. Annual mean concentrations of PM_2.5 and PM₁ were 150.9?±?78.6 μg/m³ and 72.5?±?39.0 μg/m³, respectively. The higher particulate matter (PM) mass concentrations during the winter season are essentially due to the increase of biomass burning and temperature inversion. Out of above 8 ions, the most abundant ions were SO ₄ ^2? , NO ₃ ^? and NH ₄ ⁺ for both PM_2.5 and PM₁ aerosols; their average concentrations were 7.86?±?5.86 μg/m³, 3.12?±?2.63 μg/m³ and 1.94?±?1.28 μg/m³ for PM_2.5, and 5.61?±?3.79 μg/m³, 1.81?±?1.21 μg/m³ and 1.26?±?0.88 μg/m³ for PM₁, respectively. The major secondary species SO ₄ ^2? , NO ₃ ^? and NH ₄ ⁺ accounted for 5.81%, 1.88% and 1.40% of the total mass of PM_2.5 and 11.10%, 2.68%, and 2.48% of the total mass of PM₁, respectively. The source identification was conducted for the ionic species in PM_2.5 and PM₁ aerosols. The results are discussed by the way of correlations and principal component analysis. Spearman correlation indicated that Cl^? and K⁺ in PM_2.5 and PM₁ can be originated from similar type of sources. Principal component analysis reveals that there are two major sources (anthropogenic and natural such as soil derived particles) for PM_2.5 and PM₁ fractions.     

Trace ambient levels of particulate mercury and its sources at a rural site near Delhi

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.     

Regional Sources of Methyl Chloride, Chloroform and Dichloromethane Identified from AGAGE Observations at Cape Grim, Tasmania, 1998–2000

There are large uncertainties in identifying and quantifying the natural and anthropogenic sources of chloromethanes – methyl chloride (CH₃Cl), chloroform (CHCl₃) and dichloromethane (CH₂Cl₂), which are responsible for about 15% of the total chlorine in the stratosphere. We report two years of in situ observations of these species from the AGAGE (Advanced Global Atmospheric Gas Experiment) program at Cape Grim, Tasmania (41° S, 145° E). The average background levels of CH₃Cl, CHCl₃ and CH₂Cl₂ during 1998–2000 were 551± 8, 6.3± 0.2 and 8.9± 0.2 ppt (dry air mole fractions expressed in parts per 10¹²) respectively, with a two-year average amplitude of the seasonal cycles in background air of 25, 1.1 and 1.5 ppt respectively. The CH₃Cl and CHCl₃ records at Cape Grim show clear episodes of elevated mixing ratios up to 1300 ppt and 55 ppt respectively, which are highly correlated, suggesting common source(s). Trajectory analyses show that the sources of CH₃Cl and CHCl₃ that are responsible for these elevated observations are located in coastal-terrestrial and/or coastal-seawater regions in Tasmania and the south-eastern Australian mainland. Elevated levels of CH₂Cl₂ (up to 70 ppt above background) are associated mainly with emissions from the Melbourne/Port Phillip region, a large urban/industrial complex (population 3.5 million) 300 km north of Cape Grim.Now at the Centre for Atmospheric ChemistryNow at School of Environmental Sciences     

Seasonal and annual trends of carbonaceous species of PM<Subscript>10</Subscript> over a megacity Delhi,India during 2010–2017

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.     

A semi-continuous measurement of gaseous ammonia and particulate ammonium concentrations in PM<Subscript>2.5</Subscript> in the ambient atmosphere

Ammonia has a short residence time in the atmosphere and rapidly neutralizes acid gases that occur near its source, requiring a rapid measurement system for ammonia and particulate ammonium concentrations to better understand their sources, temporal variation of ammonia emissions, and the formation of secondary ammonium aerosols. A semi-continuous measurement system, consisting of a diffusion scrubber, a particle growth chamber, an air-liquid separator, and a fluorescent detector, was developed to determine both gaseous ammonia (NH₃) and particulate ammonium (NH ₄ ⁺ ) in PM_2.5 in the ambient atmosphere of Gwangju, South Korea, during the months of March, April, July, and September of 2007. During the sampling periods, the average concentrations of ammonia and ammonium were found to be 2.33?±?1.29 μg/m³ and 1.89?±?0.99 μg/m³, respectively. Although the average gaseous ammonia concentration was highest in March, the particulate ammonium concentration was higher during the warmer season, reaching 2.08?±?1.07 μg/m³ and 2.32?±?0.94 μg/m³ in April and July, respectively, while only 1.68?±?0.61 μg/m³ in March and 1.24?±?0.99 μg/m³ in September. It is proposed that the higher availability of acid species during the warmer months produced a significant amount of particulate ammonium sulfate. Diurnal fluctuation of ammonia and ammonium during the warmer months showed that their peak time occurred at approximately 10:00 am. Both ammonia and ammonium concentrations were better correlated during the warmer months than during the cooler months. Further, the data suggest that the ammonia and ammonium were measured under well dispersed conditions, and multiple sources contributed to the ammonia at the sampling site.     

Trace gases and PM2.5-bound metal abundance over a tropical urban environment,South India

Pre and Post-Monsoon levels of ambient SO₂, NO₂, PM_2.5 and the trace metals Fe, Cu, etc. were measured at industrial and residential regions of the Kochi urban area in South India for a period of two years. The mean PM_2.5, SO₂ and NO₂ concentrations across all sites were 38.98?±?1.38 µg/m³, 2.78?±?0.85 µg/m³ and 11.90?±?4.68 µg/m³ respectively, which is lower than many other Indian cities. There was little difference in any on the measured species between the seasons. A few sites exceeded the NAAQS (define acronym and state standard) and most of the sites exceeded WHO (define acronym and state standard) standard for PM_2.5. The average trace metal concentrations (ng/m³) were found to be Fe (32.58)?>?Zn (31.93)?>?Ni (10.13)?>?Cr (5.48)?>?Pb (5.37)?>?Cu (3.24). The maximum concentration of trace metals except Pb were reported in industrial areas. The enrichment factor, of metals relative to crustal material, indicated anthropogenic dominance over natural sources for the trace metal concentration in Kochi’s atmosphere. This work demonstrates the importance of air quality monitoring in this area.

     

A global model study of natural bromine sources and the effects on tropospheric chemistry using MOZART4

Halogens in the atmosphere chemically destroy ozone. In the troposphere, bromine has higher ozone destruction efficiency than chlorine and is the halogen species with the widest geographical spread of natural sources. We investigate the relative strength of various sources of reactive tropospheric bromine and the influence of bromine on tropospheric chemistry using a 6-year simulation with the global chemistry transport model MOZART4. We consider the following sources: short-lived bromocarbons (CHBr₃, CH₂BrCl, CHBr₂Cl, CHBrCl₂, and CH₂Br₂) and CH₃Br, bromine from airborne sea salt particles, and frost flowers and sea salt on or in the snowpack in polar regions. The total bromine emissions in our simulations add up to 31.7 Gmol(Br)/yr: 63 % from polar sources, 24.6 % from short-lived bromocarbons and 12.4 % from airborne sea salt particles. We conclude from our analysis that our global bromine emission is likely to be on the lower end of the range, because of too low emissions from airborne sea salt. Bromine chemistry has an effect on the oxidation capacity of the troposphere, not only due to its direct influence on ozone concentrations, but also by reactions with other key chemical species like HO _x and NO _x . Globally, the impact of bromine chemistry on tropospheric O₃ is comparable to the impact of gas-phase sulfur chemistry, since the inclusion of bromine chemistry in MOZART4 leads to a decrease of the O₃ burden in the troposphere by 6 Tg, while we get an increase by 5 Tg if gas-phase sulfur chemistry is switched off in the standard model. With decreased ozone burden, the simulated oxidizing capacity of the atmosphere decreases thus affecting species associated with the oxidation capacity of the atmosphere (CH₃OOH, H₂O₂).     

The impacts of urbanization on air quality over the Pearl River Delta in winter: roles of urban land use and emission distribution

In this study, ideal but realistic numerical experiments are performed to explore the relative effects of changes in land use and emission distribution on air quality in the Pearl River Delta (PRD) region in winter. The experiments are accomplished using the Lagrangian particle transport and dispersion model FLEXPART coupled with the Weather Research and Forecasting model under different scenarios. Experiment results show that the maximum changes in daily mean air pollution concentration (as represented by SO₂ concentration) caused by land use change alone reaches up to 2?×?10^?6 g m^?3, whereas changes in concentrations due to the anthropogenic emission distribution are characterized by a maximum value of 6?×?10^?6 g m^?3. Such results reflect that, although the impacts of land use change on air quality are non-negligible, the emission distribution exerts a more significant influence on air quality than land use change. This provides clear implications for policy makers to control urban air pollution over the PRD region, especially for the urban planning in spatial arrangements for reasonable emissions.