Modelling the formation and atmospheric transport of secondary inorganic aerosols with special attention to regions with high ammonia emissions

Regional simulations of sulfate, nitrate and ammonium aerosols were performed by a nested application of the online-coupled three-dimensional Eulerian model system COSMO-MUSCAT. This was done in a domain covering the northern part of Germany and surrounding regions for the full month of May and a 6-week period in August/September 2006 with the primary focus on secondary inorganic aerosol levels caused by ammonia emissions from domesticated animals and agricultural operations.The results show that in situations with westerly winds ammonium nitrate dominates with concentrations of about 5–10 μg m^?3 whereas the ammonium sulfate concentrations are about 5 μg m^?3. In situations with winds mainly from the East characterized by warmer and dryer air the ammonium sulfate concentrations have their maximum at about 10 μg m^?3 whereas at the same time no ammonium nitrate is present.A reduction of agricultural NH₃ emissions by 50% in a regional scale reduces the ammonium nitrate concentrations to a maximum of 30%, while the ammonium sulfate concentrations are unchanged. The reduction of NH₃ emissions in a more limited area (here in the Federal state of Germany Niedersachsen) does have no noticeable effect neither on ammonium sulfate nor on ammonium nitrate.     

Characterization of gaseous pollutant and particulate matter emission rates from a commercial broiler operation part II: Correlated emission rates

Emission rates of ammonia, acid gases, inorganic aerosols, methane, and size fractionated particulate matter were measured from a commercial broiler facility. This paper discusses the statistically influential parameters on numerous pollutants’ emission from a broiler chicken facility and generates emission correlations to fill data gaps and develop averaged emission factors.Live mass of the birds was commonly a significant variable to each pollutant’s emission. Some variables significantly impacted the pollutants’ emissions, such as litter moisture content, but were measured discretely and cannot be used for filling in data gaps.House parameter correlations were, therefore, developed using parameters measured at the facility, such as indoor temperature, relative humidity, and the live mass of the birds, and relied on the mutual behaviour of discretely measured explanatory parameters and continuously monitored confounding variables. The live mass and the difference in the indoor temperature and the house set-point temperature were the most significant variables in each pollutant’s correlation.The correlations predicted each pollutants emission to within 20% (total mass basis) over most broiler production cycles. Their validation on independent datasets also successfully estimated the flocks’ emissions to within 3%.Emission factors (EFs) were developed for methane, ammonia, and size fractionated particulate matter using measured data and correlated emissions to fill in data gaps. PM₁₀ (particulate matter ≤10 microns) EFs were estimated to be 4.6 and 5.9 g d^?1 [Animal Unit, AU]^?1 for five and six week production cycles, respectively. PM_2.5 (PM ≤ 2.5 microns) EFs were 0.8 and 1.4 g d^?1 AU^?1 for five and six week cycles, respectively. Ammonia and methane emission factors were estimated at 120.8 and 197.0 g d^?1 AU^?1, respectively for a five week production cycle.     

Simulating the fine and coarse inorganic particulate matter concentrations in a polluted megacity

A three dimensional chemical transport model (PMCAMx) is applied to the Mexico City Metropolitan Area (MCMA) in order to simulate the chemical composition and mass of the major PM₁ (fine) and PM_1–10 (coarse) inorganic components and determine the effect of mineral dust on their formation. The aerosol thermodynamic model ISORROPIA-II is used to explicitly simulate the effect of Ca, Mg, and K from dust on semi-volatile partitioning and water uptake. The hybrid approach is applied to simulate the inorganic components, assuming that the smallest particles are in thermodynamic equilibrium, while describing the mass transfer to and from the larger ones. The official MCMA 2004 emissions inventory with improved dust and NaCl emissions is used. The comparison between the model predictions and measurements during a week of April of 2003 at Centro Nacional de Investigacion y Capacitacion Ambiental (CENICA) “Supersite” shows that the model reproduces reasonably well the fine mode composition and its diurnal variation. Sulfate predicted levels are relatively uniform in the area (approximately 3 μg m^?3), while ammonium nitrate peaks in Mexico City (approximately 7 μg m^?3) and its concentration rapidly decreases due to dilution and evaporation away from the urban area. In areas of high dust concentrations, the associated alkalinity is predicted to increase the concentration of nitrate, chloride and ammonium in the coarse mode by up to 2 μg m^?3 (a factor of 10), 0.4 μg m^?3, and 0.6 μg m^?3 (75%), respectively. The predicted ammonium nitrate levels inside Mexico City for this period are sensitive to the physical state (solid versus liquid) of the particles during periods with RH less than 50%.     

Protease production by the keratinolytic Bacillus sp. CL18 through feather bioprocessing

Bacillus sp. CL18 was investigated to propose a bioprocess for protease production using feathers as organic substrate. In feather broth (FB), containing feathers as sole organic substrate (1–100 g l^?1), maximal protease production was observed at 30 g l^?1 (FB30) after 6 days of cultivation, whereas increased feather concentrations negatively affected protease production and feather degradation. Protease production peaks were always observed earlier during cultivations than maximal feather degradation. In FB30, 80% of initial feathers mass were degraded after 7 days. Addition of glucose, sucrose, starch, yeast extract (2 g l^?1), CaCl₂, or MgCl₂ (10 mmol l^?1) to FB30 decreased protease production and feather degradation. FB30 supplementation with NH₄Cl (1 g l^?1) resulted in less apparent negative effects on protease production, whereas peptone (2 g l^?1) increased protease yields earlier during cultivations (3 days). Through a central composite design employed to investigate the effects of peptone and NH₄Cl (0.5–4.5 g l^?1) on protease production and feather degradation, FB30 supplementation with peptone and NH₄Cl (0.5–1.1 g l^?1) increased protease production within a shorter cultivation time (5 days) and hastened complete feather degradation (6 days). Feather bioconversion concurs with sustainable production of value-added products.

     

Ammonia emissions from naturally ventilated dairy cattle buildings and outdoor concrete yards in Portugal

There is a lack of information on ammonia (NH₃) emissions from cattle housing systems in Mediterranean countries, with most published data deriving from NW Europe. An investigation was carried out in NW Portugal to quantify NH₃ emissions for the main types of dairy cattle buildings in Portugal, i.e. naturally ventilated buildings and outdoor concrete yards, and to derive robust emission factors (EFs) for these conditions and compare with EFs used elsewhere in Europe. Measurements were made throughout a 12-month period using the passive flux sampling method in the livestock buildings and the equilibrium concentration technique in outdoor yards.The mean NH₃ emission factor for the whole housing system (buildings + outdoor yards) was 43.7 g NH₃–N LU^?1 day^?1 and for outdoor concrete yards used by dairy cattle was 26.6 g NH₃–N LU^?1 day^?1. Expressing NH₃ emission in terms of the quantity of liquid milk produced gave similar values across the three dairy farms studied (with a mean of 2.3 kg N ton-milk^?1 produced) and may have advantages when comparing different farming systems. In dairy houses with outdoor yards, NH₃ emissions from the yard area contributed to 69–92% of total emissions from this housing system. Emissions were particularly important during spring and summer seasons from outdoor yards with NH₃ emitted in this period accounting for about 72% of annual emissions from outdoor yards. Mean NH₃ emission factors derived for this freestall housing system and outdoor concrete yards used by dairy cattle in Portugal were higher than those measured in northern Europe. In addition, values of animal N excretion estimated in this study were greater than official National standard values. If these emissions are typical for Portuguese dairy systems, then the current National inventory underestimates emissions from this source in NW of Portugal, because of the use of lower standard values of N excretion by dairy cattle.     

Long-range transport episodes of fine particles in southern Finland during 1999–2007

The frequency, strength and sources of long-range transport (LRT) episodes of fine particles (PM_2.5) were studied in southern Finland using air quality monitoring results, backward air mass trajectories, remote sensing of fire hot spots, transport and dispersion modelling of smoke and chemical analysis of particle samples (black carbon, monosaccharide anhydrides, oxalate, succinate, malonate, SO₄^2?, NO₃^?, K⁺ and NH₄⁺). At an urban background site in Helsinki, the daily WHO guideline value (24-h PM_2.5 mean 25 μg m^?3) was exceeded during 1–7 LRT episodes per year in 1999–2007. The 24-h mean maximum concentrations varied between 25 and 49 μg m^?3 during the episodes, which was 3–6 times higher than the local mean concentration (8.7 μg m^?3) in 1999–2007. The highest particle concentrations (max. 1-h mean 163 μg m^?3) and the longest episodes (max. 9 days) were mainly caused by the emissions from open biomass burning, especially during springs and late-summers in 2002 and 2006. During the period 2001–2007, the satellite remote sensing of active fire hot spots and transport and dispersion modelling of smoke indicated that approximately half of the episodes were caused partly by the emissions from wildfires and/or agricultural waste burning in fields in Eastern Europe, especially in Russia, Belarus and Ukraine. Other episodes were mainly caused by the LRT of ordinary anthropogenic pollutants, e.g. from energy production, traffic, industry and wood combustion. During those ‘other episodes’, air masses also arrived from Eastern Europe, including Poland. The highest concentrations of biomass-burning tracers, such as monosaccharide anhydrides (levoglucosan + mannosan + galactosan) and K⁺, were observed during open biomass-burning episodes, but quite high values were also measured during some winter episodes due to wood combustion emissions. Our results indicate that open biomass burning in Eastern Europe causes high fine particle concentration peaks in large areas of Europe almost every year.     

Adaptation of a speciation sampling cartridge for measuring ammonia flux from cattle feedlots using relaxed eddy accumulation

Improved measurements of ammonia losses from cattle feedlots are needed to quantify the national NH₃ emissions inventory and evaluate management techniques for reducing emissions. Speciation cartridges composed of glass honeycomb denuders and filter packs were adapted to measure gaseous NH₃ and aerosol NH₄⁺ fluxes using relaxed eddy accumulation (REA). Laboratory testing showed that a cartridge equipped with four honeycomb denuders had a total capture capacity of 1800 μg of NH₃. In the field, a pair of cartridges was deployed adjacent to a sonic anemometer and an open-path gas analyzer on a mobile tower. High-speed valves were attached to the inlets of the cartridges and controlled by a datalogger so that up- and down-moving eddies were independently sampled based on direction of the vertical wind speed and a user-defined deadband. Air flowed continuously through the cartridges even when not sampling by means of a recirculating air handling system. Eddy covariance measurement of CO₂ and H₂O, as measured by the sonic and open-path gas analyzer, were used to determine the relaxation factor needed to compute REA-based fluxes. The REA system was field tested at the Beef Research Unit at Kansas State University in the summer and fall of 2007. Daytime NH₃ emissions ranged between 68 and 127 μg m^?2 s^?1; fluxes tended to follow a diurnal pattern correlated with latent heat flux. Daily fluxes of NH₃ were between 2.5 and 4.7 g m^?2 d^?1 and on average represented 38% of fed nitrogen. Aerosol NH₄⁺ fluxes were negligible compared with NH₃ emissions. An REA system designed around the high-capacity speciation cartridges can be used to measure NH₃ fluxes from cattle feedlots and other strong sources. The system could be adapted to measure fluxes of other gases and aerosols.     

A four-year size-segregated characterization study of particles PM10, PM2.5 and PM1 depending on air mass origin at Melpitz

PM₁₀ measurements were started in November 1992 at Melpitz site. The mean PM₁₀ concentration in 1993 was 38 μg m^?3 in the summer season (May until October) and about 44 μg m^?3 in the winter season (November until April). The mean PM₁₀ level decreased until 1999 and varies now in ranges from 20–34 μg m^?3 to 17–24 μg m^?3 (minimum and maximum mean values for 1999–2008) in winter and summer seasons, respectively. High volume filter samples of particles PM₁₀, PM_2.5 and PM₁ were characterized for mass, water-soluble ions, organic and elemental carbon from 2004 until 2008. The percentage of PM_2.5 in PM₁₀ varies between summer (71.6%) and winter seasons (81.9%). Mean concentrations of PM₁₀, PM_2.5 and PM₁ in Melpitz were 20, 15, and 13 μg m^?3 in 2004, 22, 18, and 13 μg m^?3 in 2005, 24, 19, and 12 μg m^?3 in 2006 and 22, 17, and 12 μg m^?3 in 2007, respectively. In the four winters the rural background concentration PM₁₀ at Melpitz exceeded the daily 50 μg m^?3 limit for Europe on 8, 8, 7 and 6 days, respectively.Findings for a simple two-sector-classification of the samples (May 2004 until April 2008) using 96-h backward trajectories for the identification of source regions are: Air masses were transported most of time (60%) from the western sector and secondly (17%) from the eastern sector. The lowest daily mean mass concentration PM₁₀ were found during western inflow in summer (17 μg m^?3) containing low amounts of sulphate (2.4 μg m^?3), nitrate (1.7 μg m^?3), ammonium (1.1 μg m^?3) and TC (3.7 μg m^?3). In opposite the highest mean mass concentration PM₁₀ was found during eastern inflow in winter (35 μg m^?3) with high amounts of sulphate (6.1 μg m^?3), nitrate (5.4 μg m^?3), ammonium (3.8 μg m^?3) and TC (9.4 μg m^?3). An estimation of secondary formed OC (SOA) shows 0.8–0.9 μg m^?3 for air masses from West and 2.1–2.2 μg m^?3 from East. The seasonal difference can be neglected.The half-hourly measurements of the particle mass concentration PM₁₀ evaluated as mean daily courses using a TEOM^® show low values (14–21 μg m^?3) in summer and winter for air masses transported from West and the highest concentrations (31–38 μg m^?3) in winter for air masses from East.The results demonstrate the influence of meteorological parameters on long-range transport, secondary particle mass formation and re-emission which modify mass concentration and composition of PM₁₀, PM_2.5 and PM₁. Melpitz site is located in the East of Germany faraway from strong local anthropogenic emissions (rural background). Therefore, this site is suitable for investigation of the influence of long-range transport of air pollution in continental air masses from the East with source regions inside and outside of the European Union.     

Gaseous emissions from outdoor concrete yards used by livestock

Measurements of ammonia (NH₃), nitrous oxide (N₂O) and methane (CH₄) were made from 11 outdoor concrete yards used by livestock. Measurements of NH₃ emission were made using the equilibrium concentration technique while closed chambers were used to measure N₂O and CH₄ emissions. Outdoor yards used by livestock proved to be an important source of NH₃ emission. Greatest emission rates were measured from dairy cow feeding yards, with a mean of 690 mg NH₃-N m⁻² h⁻¹. Smaller emission rates were measured from sheep handling areas, dairy cow collecting yards, beef feeding yards and a pig loading area, with respective mean emission rates of 440, 280, 220 and 140 mg NH₃-N m⁻² h⁻¹. Emission rates of N₂O and CH₄ were much smaller and for CH₄, in particular, emission rates were influenced greatly by the presence or absence of dung on the measurement area.     

Quantifying road dust resuspension in urban environment by Multilinear Engine: A comparison with PMF2

Atmospheric PM pollution from traffic comprises not only direct emissions but also non-exhaust emissions because resuspension of road dust that can produce high human exposure to heavy metals, metalloids, and mineral matter. A key task for establishing mitigation or preventive measures is estimating the contribution of road dust resuspension to the atmospheric PM mixture. Several source apportionment studies, applying receptor modeling at urban background sites, have shown the difficulty in identifying a road dust source separately from other mineral sources or vehicular exhausts. The Multilinear Engine (ME-2) is a computer program that can solve the Positive Matrix Factorization (PMF) problem. ME-2 uses a programming language permitting the solution to be guided toward some possible targets that can be derived from a priori knowledge of sources (chemical profile, ratios, etc.). This feature makes it especially suitable for source apportionment studies where partial knowledge of the sources is available.In the present study ME-2 was applied to data from an urban background site of Barcelona (Spain) to quantify the contribution of road dust resuspension to PM₁₀ and PM_2.5 concentrations. Given that recently the emission profile of local resuspended road dust was obtained (Amato, F., Pandolfi, M., Viana, M., Querol, X., Alastuey, A., Moreno, T., 2009. Spatial and chemical patterns of PM₁₀ in road dust deposited in urban environment. Atmospheric Environment 43 (9), 1650–1659), such a priori information was introduced in the model as auxiliary terms of the object function to be minimized by the implementation of the so-called “pulling equations”.ME-2 permitted to enhance the basic PMF solution (obtained by PMF2) identifying, beside the seven sources of PMF2, the road dust source which accounted for 6.9 μg m^?3 (17%) in PM₁₀, 2.2 μg m^?3 (8%) of PM_2.5 and 0.3 μg m^?3 (2%) of PM₁. This reveals that resuspension was responsible of the 37%, 15% and 3% of total traffic emissions respectively in PM₁₀, PM_2.5 and PM₁. Therefore the overall traffic contribution resulted in 18 μg m^?3 (46%) in PM₁₀, 14 μg m^?3 (51%) in PM_2.5 and 8 μg m^?3 (48%) in PM₁. In PMF2 this mass explained by road dust resuspension was redistributed among the rest of sources, increasing mostly the mineral, secondary nitrate and aged sea salt contributions.     

On-road comparison of a portable emission measurement system with a mobile reference laboratory for a heavy-duty diesel vehicle

On-road comparisons were made between a mobile emissions laboratory (MEL) meeting federal standards and a portable emissions measurement system (PEMS). These comparisons were made over different conditions; including road grade, vibration, altitude, electric fields, and humidity with the PEMS mounted inside and outside of the tractor's cab. Brake-specific emissions were calculated to explore error differences between the MEL and PEMS during the Not-To-Exceed (NTE) engine operating zone. The PEMS brake-specific NOx (bsNOx) NTE emissions were biased high relative to the MEL and, in general, were about 8% of the 2007 in-use NTE NO_x standard of 2.68 g kW^?1 h^?1 (2.0 g hp^?1 h^?1). The bsCO₂ emissions for the PEMS were also consistently biased high relative to the MEL, with an average deviation of +4% ± 2%. NMHC and CO emissions were very low and typically less than 1% of the NTE threshold. This research was part of a comprehensive program to determine the “allowance” when PEMS are used for in-use compliance testing of heavy-duty diesel vehicles (HDDVs).     

Indoor particle size distributions in homes with open fires and improved Patsari cook stoves

Particulate pollution has been clearly linked with adverse health impacts from open fire cookstoves, and indoor air concentrations are frequently used as a proxy for exposures in health studies. Implicit are the assumptions that the size distributions for the open fire and improved stove are not significantly different, and that the relationship between indoor concentrations and personal exposures is the same between stoves. To evaluate the impact of these assumptions size distributions of particulate matter in indoor air were measured with the Sioutas cascade impactor in homes using open fires and improved Patsari stoves in a rural Purepecha community in Michoacan, Mexico. On average indoor concentrations of particles less than 0.25 μm were 72% reduced in homes with improved Patsari stoves, reflecting a reduced contribution of this size fraction to PM_2.5 mass concentrations from 68% to 48%. As a result the mass median diameter of indoor PM_2.5 particulate matter was increased by 29% with the Patsari improved stove compared to the open fire (from 0.42 μm to 0.59 μm, respectively). Personal PM_2.5 exposure concentrations for women in homes using open fires were approximately 61% of indoor concentration levels (156 μg m^?3 and 257 μg m^?3 respectively). In contrast personal exposure concentrations were 77% times indoor air concentration levels for women in homes using improved Patsari stoves (78 μg m^?3and 101 μg m^?3 respectively). Thus, if indoor air concentrations are used in health and epidemiologic studies significant bias may result if the shift in size distribution and the change in relationship between indoor air concentrations and personal exposure concentrations are not accounted for between different stove types.     

Carbon dioxide fluxes over an urban park area

From September 2006 to October 2007 turbulent fluxes of carbon dioxide were measured at an urban tower station (26 m above ground level, z/z_h = 1.73) in Essen, Germany, using the eddy covariance technique. The site was located at the border between a public park area (70 ha) in the south–west of the station and suburban/urban residential as well as light commercial areas in the north and east of the tower. Depending on the land-use two different sectors (park and urban) were identified showing distinct differences in the temporal evolution of the surface-atmosphere exchange of CO₂. While urban fluxes appear to be governed by anthropogenic emissions from domestic heating and traffic (average flux 9.3 μmol m^?2 s^?1), the exchange of CO₂ was steered by biological processes when the park contributed to the flux footprint. The diurnal course during the vegetation period exhibited negative daytime fluxes up to ?10 μmol m^?2 s^?1 on average in summer. Nevertheless, with a mean of 0.8 μmol m^?2 s^?1 park sector fluxes were slightly positive, thus no net carbon uptake by the surface occurred throughout the year.In order to sum the transport of CO₂ a gap-filling procedure was performed by means of artificial neural network generalisation. Using additional meteorological inputs the daily exchange of CO₂ was reproduced using radial basis function networks (RBF). The resulting yearly sum of 6031 g m^?2 a^?1 indicates the entire study site to be a considerable source of CO₂.     

Year-long continuous personal exposure to PM2.5 recorded by a fast responding portable nephelometer

Personal exposure to particulate matter of aerodynamic diameter under 2.5 μm (PM_2.5) was monitored using a DustTrak nephelometer. The battery-operated unit, worn by an adult individual for a period of approximately one year, logged integrated average PM_2.5 concentrations over 5 min intervals. A detailed time-activity diary was used to record the experimental subject’s movement and the microenvironments visited. Altogether 239 days covering all the months (except April) were available for the analysis. In total, 60 463 acceptable 5-min averages were obtained. The dataset was divided into 7 indoor and 4 outdoor microenvironments. Of the total time, 84% was spent indoors, 10.9% outdoors and 5.1% in transport. The indoor 5-min PM_2.5 average was higher (55.7 μg m^?3) than the outdoor value (49.8 μg m^?3). The highest 5-min PM_2.5 average concentration was detected in restaurant microenvironments (1103 μg m^?3), the second highest 5-min average concentration was recorded in indoor spaces heated by stoves burning solid fuels (420 μg m^?3). The lowest 5-min mean aerosol concentrations were detected outdoors in rural/natural environments (25 μg m^?3) and indoors at the monitored person’s home (36 μg m^?3). Outdoor and indoor concentrations of PM_2.5 measured by the nephelometer at home and during movement in the vicinity of the experimental subject’s home were compared with those of the nearest fixed-site monitor of the national air quality monitoring network. The high correlation coefficient (0.78) between the personal and fixed-site monitor aerosol concentrations suggested that fixed-site monitor data can be used as proxies for personal exposure in residential and some other microenvironments. Collocated measurements with a reference method (β-attenuation) showed a non-linear systematic bias of the light-scattering method, limiting the use of direct concentration readings for exact exposure analysis.     

Evidence for short-range transport of atmospheric mercury to a rural,inland site

Atmospheric mercury (Hg) species, including gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particulate-bound mercury (Hg_p), were monitored near three sites, including a cement plant (monitored in 2007 and 2008), an urban site and a rural site (both monitored in 2005 and 2008). Although the cement plant was a significant source of Hg emissions (for 2008, GEM: 2.20 ± 1.39 ng m^?3, RGM: 25.2 ± 52.8 pg m^?3, Hg_p 80.8 ± 283 pg m^?3), average GEM levels and daytime average dry depositional RGM flux were highest at the rural site, when all three sites were monitored sequentially in 2008 (rural site, GEM: 2.37 ± 1.26 ng m^?3, daytime RGM flux: 29 ± 40 ng m^?2 day^?1). Photochemical conversion of GEM was not the primary RGM source, as highest net RGM gains (75.9 pg m^?3, 99.0 pg m^?3, 149 m^?3) occurred within 3.0–5.3 h, while the theoretical time required was 14–23 h. Instead, simultaneous peaks in RGM, Hg_p, ozone (O₃), nitrogen oxides, and sulfur dioxide in the late afternoon suggested short-range transport of RGM from the urban center to the rural site. The rural site was located more inland, where the average water vapor mixing ratio was lower compared to the other two sites (in 2008, rural: 5.6 ± 1.4 g kg^?1, urban: 9.0 ± 1.1 g kg^?1, cement plant: 8.3 ± 2.2 g kg^?1). Together, these findings suggested short-range transport of O₃ from an urban area contributed to higher RGM deposition at the rural site, while drier conditions helped sustain elevated RGM levels. Results suggested less urbanized environments may be equally or perhaps more impacted by industrial atmospheric Hg emissions, compared to the urban areas from where Hg emissions originated.     

Deposition processes of ionic constituents to snow cover

Atmospheric deposition is an important removal process of aerosol particles and gases from the atmosphere. To elucidate the relative contributions of wet and dry processes and in-cloud and below-cloud scavenging based on deposition amounts in winter at Mt. Tateyama, central Japan, we obtained daily samples (December, 2006–March, 2007) of size-segregated aerosol particles and precipitation at Senjyugahara (SJ; 475 m a.s.l.) and vertical samples of spring snow cover at Murododaira (MR, 2450 m a.s.l., 13 km distance from SJ) on the western flank of Mt. Tateyama. The NH₄⁺ and nssSO₄^2? in aerosols were mostly found in the fine fraction (<2 μm), although Na⁺, NO₃^?, and nssCa²⁺ were mainly detected in the coarse fraction (>2 μm). Average ionic concentrations (μg g^?1) in precipitation at SJ were higher about 3.8 for Na⁺ and nssCa²⁺, 3.4 for NO₃^?, 3.7 for NH₄⁺, 2.5 for nssSO₄^2? than those at MR, whereas cumulative precipitation amounts at SJ and MR were, respectively, 84 and 175 cm of water equivalent. Wet and dry deposition amounts during the study period were estimated for sites using size-segregated aerosol data, winter averages of HNO₃, NH₃, and SO₂ concentrations, and dry deposition velocities. Particle-dry deposition comprised about 3% (Na⁺) to 11% (NH₄⁺) of the total deposition at MR. The maximum amounts of gas dry deposition were estimated, respectively, as 4, 13, and 3% of the total deposition at MR for NH₄⁺, NO₃^?, and nssSO₄^2?. The relative contributions of below-cloud scavenging (BCS) between MR and SJ were estimated as considering the wet only deposition amount at MR. Higher contributions of BCS were obtained for Na⁺ (56%) and nssCa²⁺ (45%), whereas BCSs for NH₄⁺, NO₃^?, and nssSO₄^2? were lower than 28%. Ionic constituents existing predominantly in the coarse fraction showed a large contribution of BCS.     

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.     

Experimental and statistical analyses to characterize in-vehicle fine particulate matter behavior inside public transit buses operating on B20-grade biodiesel fuel

This paper presents results from an in-vehicle air quality study of public transit buses in Toledo, Ohio, involving continuous monitoring, and experimental and statistical analyses to understand in-vehicle particulate matter (PM) behavior inside buses operating on B20-grade biodiesel fuel. The study also focused on evaluating the effects of vehicle’s fuel type, operating periods, operation status, passenger counts, traffic conditions, and the seasonal and meteorological variation on particulates with aerodynamic diameter less than 1 micron (PM_1.0). The study found that the average PM_1.0 mass concentrations in B20-grade biodiesel-fueled bus compartments were approximately 15 μg m^?3, while PM_2.5 and PM₁₀ concentration averages were approximately 19 μg m^?3 and 37 μg m^?3, respectively. It was also observed that average hourly concentration trends of PM_1.0 and PM_2.5 followed a “μ-shaped” pattern during transit hours.Experimental analyses revealed that the in-vehicle PM_1.0 mass concentrations were higher inside diesel-fueled buses (10.0–71.0 μg m^?3 with a mean of 31.8 μg m^?3) as compared to biodiesel buses (3.3–33.5 μg m^?3 with a mean of 15.3 μg m^?3) when the windows were kept open. Vehicle idling conditions and open door status were found to facilitate smaller particle concentrations inside the cabin, while closed door facilitated larger particle concentrations suggesting that smaller particles were originating outside the vehicle and larger particles were formed within the cabin, potentially from passenger activity. The study also found that PM_1.0 mass concentrations at the back of bus compartment (5.7–39.1 μg m^?3 with a mean of 28.3 μg m^?3) were higher than the concentrations in the front (5.7–25.9 μg m^?3 with a mean of 21.9 μg m^?3), and the mass concentrations inside the bus compartment were generally 30–70% lower than the just-outside concentrations. Further, bus route, window position, and time of day were found to affect the in-vehicle PM concentrations significantly. Overall, the in-vehicle PM_1.0 concentrations inside the buses operating on B20-grade biodiesel ranged from 0.7 μg m^?3 to 243 μg m^?3, with a median of 11.6 μg m^?3.Statistical models developed to study the effects of vehicle operation and ambient conditions on in-vehicle PM concentrations suggested that while open door status was the most important influencing variable for finer particles and higher passenger activity resulted in higher coarse particles concentrations inside the vehicle compartments, ambient PM concentrations contributed to all PM fractions inside the bus irrespective of particle size.     

Influence of regional development policies and clean technology adoption on future air pollution exposure

Future air pollution emissions in the year 2030 were estimated for the San Joaquin Valley (SJV) in central California using a combined system of land use, mobile, off-road, stationary, area, and biogenic emissions models. Four scenarios were developed that use different assumptions about the density of development and level of investment in transportation infrastructure to accommodate the expected doubling of the SJV population in the next 20 years. Scenario 1 reflects current land-use patterns and infrastructure while scenario 2 encouraged compact urban footprints including redevelopment of existing urban centers and investments in transit. Scenario 3 allowed sprawling development in the SJV with reduced population density in existing urban centers and construction of all planned freeways. Scenario 4 followed currently adopted land use and transportation plans for the SJV. The air quality resulting from these urban development scenarios was evaluated using meteorology from a winter stagnation event that occurred on December 15th, 2000 to January 7th 2001. Predicted base-case PM2.5 mass concentrations within the region exceeded 35 μg m^?3 over the 22-day episode. Compact growth reduced the PM2.5 concentrations by ～1 μg m^?3 relative to the base-case over most of the SJV with the exception of increases (～1 μg m^?3) in urban centers driven by increased concentrations of elemental carbon (EC) and organic carbon (OC). Low-density development increased the PM2.5 concentrations by 1–4 μg m^?3 over most of the region, with decreases (0.5–2 μg m^?3) around urban areas. Population-weighted average PM2.5 concentrations were very similar for all development scenarios ranging between 16 and 17.4 μg m^?3. Exposure to primary PM components such as EC and OC increased 10–15% for high density development scenarios and decreased by 11–19% for low-density scenarios. Patterns for secondary PM components such as nitrate and ammonium ion were almost exactly reversed, with a 10% increase under low-density development and a 5% decrease under high density development. The increased human exposure to primary pollutants such as EC and OC could be predicted using a simplified analysis of population-weighted primary emissions. Regional planning agencies should develop thresholds of population-weighted primary emissions exposure to guide the development of growth plans. This metric will allow them to actively reduce the potential negative impacts of compact growth while preserving the benefits.     

Size partitioning of particulate inorganic nitrogen species between the fine and coarse mode ranges and its implication to their deposition on the surface ocean

In order to discuss the dry deposition fluxes of atmospheric fixed nitrogen species, observations of aerosol chemistry including nitrate (NO₃^?) and ammonium (NH₄⁺) were conducted at two islands, Rishiri Island and Sado Island, over the Sea of Japan. Although the atmospheric concentrations of particulate NH₄⁺–N showed higher values than those of particulate NO₃^?–N at both sites, the dry deposition fluxes of the particulate NO₃^?–N were estimated to be higher than those of the particulate NH₄⁺–N. This was caused by the difference of particle sizes between the particulate NO₃^? and NH₄⁺; NH₄⁺ was almost totally contained in fine particles (d < 2.5 μm) with smaller deposition velocity, whereas NO₃^? was mainly contained in coarse particles (d > 2.5 μm) with greater deposition velocity. Fine mode NO₃^? was strongly associated with fine mode sea-salt and mineral particles, of which higher concentrations shifted the size of particulate NO₃^? toward the fine mode range. This size shift would decrease the dry deposition flux of the fixed nitrogen species on coastal waters and accelerate atmospheric transport of them to the remote oceanic areas.