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Atmospheric Environment (v.44, #18)
Hydrocarbon emission fingerprints from contemporary vehicle/engine technologies with conventional and new fuels by Larisse Montero; Matthew Duane; Urbano Manfredi; Covadonga Astorga; Giorgio Martini; Massimo Carriero; Alois Krasenbrink; B.R. Larsen (pp. 2167-2175).
The present paper presents results from the analysis of 29 individual C2–C9 hydrocarbons (HCs) specified in the European Commission Ozone Directive. The 29 HCs are measured in exhaust from common, contemporary vehicle/engine/fuel technologies for which very little or no data is available in the literature. The obtained HC emission fingerprints are compared with fingerprints deriving from technologies that are being phased out in Europe. Based on the total of 138 emission tests, thirteen type-specific fingerprints are extracted (Mean±SD percentage contributions from individual HCs to the total mass of the 29 HCs), essential for receptor modelling source apportionment. The different types represent exhaust from Euro3 and Euro4 light-duty (LD) diesel and petrol-vehicles, Euro3 heavy-duty (HD) diesel exhaust, and exhaust from 2-stroke preEuro, Euro1 and Euro2 mopeds. The fuels comprise liquefied petroleum gas, petrol/ethanol blends (0–85% ethanol), and mineral diesel in various blends (0–100%) with fatty acid methyl esters, rapeseed methyl esters palm oil methyl esters, soybean oil methyl or sunflower oil methyl esters. Type-specific tracer compounds (markers) are identified for the various vehicle/engine/fuel technologies.An important finding is an insignificant effect on the HC fingerprints of varying the test driving cycle, indicating that combining HC fingerprints from different emission studies for receptor modelling purposes would be a robust approach.The obtained results are discussed in the context of atmospheric ozone formation and health implications from emissions (mgkm−1 for LD and mopeds and mgkWh−1 for HD, all normalised to fuel consumption: mgdm−3fuel) of the harmful HCs, benzene and 1,3-butadiene.Another important finding is a strong linear correlation of the regulated “total” hydrocarbon emissions (tot-HC) with the ozone formation potential of the 29 HCs (ΣPO3=(1.66±0.04)×tot-RH; r2=0.93). Tot-HC is routinely monitored in emission control laboratories, whereas C2–C9 are not. The revealed strong correlations broadens the usability of data from vehicle emission control laboratories and facilitates the comparison of the ozone formation potential of HCs in exhaust from of old and new vehicle/engine/fuel technologies.
Keywords: Petrol; Diesel; Ethanol; Biofuel; LPG; C; 2; –C; 9; VOC
Seasonal variability in gaseous mercury fluxes measured in a high-elevation meadow by A.D. Converse; A.L. Riscassi; T.M. Scanlon (pp. 2176-2185).
Seasonal patterns of atmospheric mercury (Hg) fluxes measured over vegetated terrestrial systems can provide insight into the underlying process controlling emission and deposition of Hg to vegetated surfaces. Gaseous elemental Hg fluxes were measured for week-long periods in each season (spring, summer, fall, and winter) over an uncontaminated high-elevation wetland meadow in Shenandoah National Park, Virginia using micrometeorological methods. Mean net deposition was observed in the spring (−4.8 ng m−2 h−1), emission in the summer (2.5 ng m−2 h−1), near zero flux in the fall (0.3 ng m−2 h−1), and emission in the winter (4.1 ng m−2 h−1). Nighttime deposition (when stomata are closed) and the poor correlation between Hg fluxes and canopy conductance during periods of active vegetation growth suggest that stomatal processes are not the dominant mechanism for ecosystem-level GEM exchange at this site. The strong springtime deposition relative to summer implies that young vegetation is better at scavenging Hg, with the highest deposition occurring at night possibly via a cuticular pathway. These results suggest that spring is a period of GEM deposition while other seasons exhibit net emission, emphasizing the importance of capturing GEM flux seasonality when determining total Hg budgets.
Keywords: GEM; Elemental mercury; Micrometeorological methods; Stomatal exchange; Cuticular pathway
Air ion concentrations in various urban outdoor environments by Xuan Ling; Rohan Jayaratne; Lidia Morawska (pp. 2186-2193).
Atmospheric ions are produced by many natural and anthropogenic sources and their concentrations vary widely between different environments. There is very little information on their concentrations in different types of urban environments, how they compare across these environments and their dominant sources. In this study, we measured airborne concentrations of small ions, particles and net particle charge at 32 different outdoor sites in and around a major city in Australia and identified the main ion sources. Sites were classified into seven groups as follows: park, woodland, city centre, residential, freeway, power lines and power substation. Generally, parks were situated away from ion sources and represented the urban background value of about 270 ions cm−3. Median concentrations at all other groups were significantly higher than in the parks. We show that motor vehicles and power transmission systems are two major ion sources in urban areas. Power lines and substations constituted strong unipolar sources, while motor vehicle exhaust constituted strong bipolar sources. The small ion concentration in urban residential areas was about 960 cm−3. At sites where ion sources were co-located with particle sources, ion concentrations were inhibited due to the ion-particle attachment process. These results improved our understanding on air ion distribution and its interaction with particles in the urban outdoor environment.
Keywords: Small ions; Aerosol; Charged particle; Urban environment
Ship emissions and their externalities for Greece by Ernestos Tzannatos (pp. 2194-2202).
The existing and emerging international and European policy framework for the reduction of ship exhaust emissions dictates the need to produce reliable national, regional and global inventories in order to monitor emission trends and consequently provide the necessary support for future policy making. Furthermore, the inventories of ship exhaust emissions constitute the basis upon which their external costs are estimated in an attempt to highlight the economic burden they impose upon the society and facilitate the cost–benefit analysis of the proposed emission abatement technologies, operational measures and market-based instruments prior to their implementation.The case of Greece is of particular interest mainly because the dense ship traffic within the Greek seas directly imposes the impact of its exhaust emission pollutants (NOx, SO2 and PM) upon the highly populated, physically sensitive and culturally precious Greek coastline, as well as upon the land and seas of Greece in general, whereas the contribution of Greece in the global CO2 inventory at a time of climatic change awareness cannot be ignored. In this context, this paper presents the contribution of Greece in ship exhaust emissions of CO2, NOx, SO2 and PM from domestic and international shipping over the last 25 years (1984–2008), utilizing the fuel-based (fuel sales) emission methodology. Furthermore, the ship exhaust emissions generated within the Greek seas and their externalities are estimated for the year 2008, through utilizing the fuel-based (fuel sales) approach for domestic shipping and the activity-based (ship traffic) approach for international shipping.On this basis, it was found that during the 1984 to 2008 period the fuel-based (fuel sales) ship emission inventory for Greece increased at an average annual rate of 2.85%. In 2008, the CO2, NOx, SO2 and PM emissions reached 12.9 million tons (of which 12.4 million tons of CO2) and their externalities were found to be around 3.1 billion euro. With regard to shipping within the Greek seas, the utilization of the fuel-based (fuel sales) analysis for domestic shipping and the activity-based (ship traffic) analysis for international shipping shows that the ship-generated emissions reached 7.4 million tons (of which 7 million tons of CO2) and their externalities were estimated at 2.95 billion euro. Finally, the internalization of external costs for domestic shipping was found to produce an increase of 12.96 and 2.71 euro per passenger and transported ton, respectively.
Keywords: Ship emissions; Shipping externalities; Air pollution; Greek shipping
Real-time bias-adjusted O3 and PM2.5 air quality index forecasts and their performance evaluations over the continental United States by Daiwen Kang; Rohit Mathur; S. Trivikrama Rao (pp. 2203-2212).
The National Air Quality Forecast Capacity (NAQFC) system, which links NOAA’s North American Mesoscale (NAM) meteorological model with EPA’s Community Multiscale Air Quality (CMAQ) model, provided operational ozone (O3) and experimental fine particular matter (PM2.5) forecasts over the continental United States (CONUS) during 2008. This paper describes the implementation of a real-time Kalman Filter (KF) bias-adjustment technique to improve the accuracy of O3 and PM2.5 forecasts at discrete monitoring locations. The operational surface-level O3 and PM2.5 forecasts from the NAQFC system were post-processed by the KF bias-adjusted technique using near real-time hourly O3 and PM2.5 observations obtained from EPA’s AIRNow measurement network. The KF bias-adjusted forecasts were created daily, providing 24-h hourly bias-adjusted forecasts for O3 and PM2.5 at all AIRNow monitoring sites within the CONUS domain. The bias-adjustment post-processing implemented in this study requires minimal computational cost; requiring less than 10 min of CPU on a single processor Linux machine to generate 24-h hourly bias-adjusted forecasts over the entire CONUS domain.The results show that the real-time KF bias-adjusted forecasts for both O3 and PM2.5 have performed as well as or even better than the previous studies when the same technique was applied to the historical O3 and PM2.5 time series from archived AQF in earlier years. Compared to the raw forecasts, the KF forecasts displayed significant improvement in the daily maximum 8-h O3 and daily mean PM2.5 forecasts in terms of both discrete (i.e., reduced errors, increased correlation coefficients, and index of agreement) and categorical (increased hit rate and decreased false alarm ratio) evaluation metrics at almost all locations during the study period in 2008.
Keywords: Air quality index forecast; Bias-adjustment; O; 3; PM; 2.5; Kalman filter
Application of OMI observations to a space-based indicator of NOx and VOC controls on surface ozone formation by Bryan N. Duncan; Yasuko Yoshida; Jennifer R. Olson; Sanford Sillman; Randall V. Martin; Lok Lamsal; Yongtao Hu; Kenneth E. Pickering; Christian Retscher; Dale J. Allen; James H. Crawford (pp. 2213-2223).
We investigated variations in the relative sensitivity of surface ozone formation in summer to precursor species concentrations of volatile organic compounds (VOCs) and nitrogen oxides (NOx) as inferred from the ratio of the tropospheric columns of formaldehyde to nitrogen dioxide (the “Ratio”) from the Aura Ozone Monitoring Instrument (OMI). Our modeling study suggests that ozone formation decreases with reductions in VOCs at Ratios <1 and NOx at Ratios >2; both NOx and VOC reductions may decrease ozone formation for Ratios between 1 and 2. Using this criteria, the OMI data indicate that ozone formation became: 1. more sensitive to NOx over most of the United States from 2005 to 2007 because of the substantial decrease in NOx emissions, primarily from stationary sources, and the concomitant decrease in the tropospheric column of NO2, and 2. more sensitive to NOx with increasing temperature, in part because emissions of highly reactive, biogenic isoprene increase with temperature, thus increasing the total VOC reactivity. In cities with relatively low isoprene emissions (e.g., Chicago), the data clearly indicate that ozone formation became more sensitive to NOx from 2005 to 2007. In cities with relatively high isoprene emissions (e.g., Atlanta), we found that the increase in the Ratio due to decreasing NOx emissions was not obvious as this signal was convolved with variations in the Ratio associated with the temperature dependence of isoprene emissions and, consequently, the formaldehyde concentration.
Keywords: Surface ozone; Air quality indicator; OMI; HCHO; NO; 2
The application of profluorescent nitroxides to detect reactive oxygen species derived from combustion-generated particulate matter: Cigarette smoke – A case study by B. Miljevic; K.E. Fairfull-Smith; S.E. Bottle; Z.D. Ristovski (pp. 2224-2230).
Reactive oxygen species (ROS) and related free radicals are considered to be key factors underpinning the various adverse health effects associated with exposure to ambient particulate matter. Therefore, measurement of ROS is a crucial factor for assessing the potential toxicity of particles. In this work, a novel profluorescent nitroxide, BPEAnit, was investigated as a probe for detecting particle-derived ROS. BPEAnit has a very low fluorescence emission due to inherent quenching by the nitroxide group, but upon radical trapping or redox activity, a strong fluorescence is observed. BPEAnit was tested for detection of ROS present in mainstream and sidestream cigarette smoke. In the case of mainstream cigarette smoke, there was a linear increase in fluorescence intensity with an increasing number of cigarette puffs, equivalent to an average of 101 nmol ROS per cigarette based on the number of moles of the probe reacted. Sidestream cigarette smoke sampled from an environmental chamber exposed BPEAnit to much lower concentrations of particles, but still resulted in a clearly detectible increase in fluorescence intensity with sampling time. It was calculated that the amount of ROS was equivalent to 50 ± 2 nmol per mg of particulate matter; however, this value decreased with ageing of the particles in the chamber. Overall, BPEAnit was shown to provide a sensitive response related to the oxidative capacity of the particulate matter. These findings present a good basis for employing the new BPEAnit probe for the investigation of particle-related ROS generated from cigarette smoke as well as from other combustion sources.
Keywords: Combustion particles; Cigarette smoke; Reactive oxygen species; Fluorescence; Profluorescent nitroxides
Chemical composition and mass closure of ambient PM10 at urban sites by Eleni Terzi; George Argyropoulos; Aikaterini Bougatioti; Nikolaos Mihalopoulos; Kostas Nikolaou; Constantini Samara (pp. 2231-2239).
The chemical composition of PM10 was studied during summer and winter sampling campaigns conducted at two different urban sites in the city of Thessaloniki, Greece (urban-traffic, UT and urban-industrial, UI). PM10 samples were chemically analysed for minerals (Si, Al, Ca, Mg, Fe, Ti, K), trace elements (Cd, Cr, Cu, Mn, Pb, V, Zn, Te, Co, Ni, Se, Sr, As, and Sb), water-soluble ions (Cl−, NO3−, SO42−, Na+, K+, NH4+, Ca2+, Mg2+) and carbonaceous compounds (OC, EC). Spatial variations of atmospheric concentrations showed significantly higher levels of minerals, some trace metals and TC at the UI site, while at the UT site significantly higher levels of elements like Cd, Ba, Sn, Sb and Te were observed. Crustal elements, excepting Ca at the UI site, did not exhibit significant seasonal variations at any site pointing to constant emissions throughout the year. In order to reconstruct the particle mass, the determined components were classified into six classes as follows: mineral matter (MIN), trace elements (TE), organic matter (OM), elemental carbon (EC), sea salt (SS) and secondary inorganic aerosol (SIA). Good correlations with slopes close to 1 were found between chemically determined and gravimetrically measured PM10 masses for both sites. According to the chemical mass closure obtained, the major components of PM10 at both sites were MIN (soil-derived compounds), followed by OM and SIA. The fraction unaccounted for by chemical analysis comprised on average 8% during winter and 15% during summer at the urban-industrial site, while at the urban-traffic site the percentages were 21.5% in winter and 4.8% in summer.
Keywords: Chemical speciation; Ionic components; Minerals; Organic carbon; Trace elements; Urban aerosols
Carbonyl species characteristics during the evaporation of essential oils by Hsiu-Mei Chiang; Hua-Hsien Chiu; Yen-Ming Lai; Ching-Yen Chen; Hung-Lung Chiang (pp. 2240-2247).
Carbonyls emitted from essential oils can affect the air quality when they are used in indoors, especially under poor ventilation conditions. Lavender, lemon, rose, rosemary, and tea tree oils were selected as typical and popular essential oils to investigate in terms of composition, thermal characteristics and fifteen carbonyl constituents. Based on thermogravimetric (TG) analysis, the activation energy was 7.6–8.3 kcal mol−1, the reaction order was in the range of 0.6–0.7 and the frequency factor was 360–2838 min−1. Formaldehyde, acetaldehyde, acetone, and propionaldehyde were the dominant carbonyl compounds, and their concentrations were 0.034–0.170 ppm. The emission factors of carbonyl compounds were 2.10–3.70 mg g−1, and acetone, propionaldehyde, acetaldehyde, and formaldehyde accounted for a high portion of the emission factor of carbonyl compounds in essential oil exhaust. Some unhealthy carbonyl species such as formaldehyde and valeraldehyde, were measured at low-temperature during the vaporization of essential oils, indicating a potential effect on indoor air quality and human health.
Keywords: Essential oil; Carbonyl compound; Formaldehyde; Emission factor
An investigation of widespread ozone damage to the soybean crop in the upper Midwest determined from ground-based and satellite measurements by Jack Fishman; John K. Creilson; Peter A. Parker; Elizabeth A. Ainsworth; G. Geoffrey Vining; John Szarka; Fitzgerald L. Booker; Xiaojing Xu (pp. 2248-2256).
Elevated concentrations of ground-level ozone (O3) are frequently measured over farmland regions in many parts of the world. While numerous experimental studies show that O3 can significantly decrease crop productivity, independent verifications of yield losses at current ambient O3 concentrations in rural locations are sparse. In this study, soybean crop yield data during a 5-year period over the Midwest of the United States were combined with ground and satellite O3 measurements to provide evidence that yield losses on the order of 10% could be estimated through the use of a multiple linear regression model. Yield loss trends based on both conventional ground-based instrumentation and satellite-derived tropospheric O3 measurements were statistically significant and were consistent with results obtained from open-top chamber experiments and an open-air experimental facility (SoyFACE, Soybean Free Air Concentration Enrichment) in central Illinois. Our analysis suggests that such losses are a relatively new phenomenon due to the increase in background tropospheric O3 levels over recent decades. Extrapolation of these findings supports previous studies that estimate the global economic loss to the farming community of more than $10 billion annually.
Keywords: Air pollution; Crop damage; Ozone; Remote sensing; Soybean; Yield
The estimation of historical CO2 trajectories is indeterminate: Comment on “A new look at atmospheric carbon dioxide” by Craig Loehle (pp. 2257-2259).
A paper by is critiqued. It is shown that their exponential model for characterizing CO2 trajectories for historical data is not estimated properly. An exponential model is properly estimated and is shown to fit over the entire 51 year period of available data. Further, the entire problem of estimating models for the CO2 historical data is shown to be ill-posed because alternate model forms fit the data equally well. To illustrate this point the past 51 years of CO2 data were analyzed using three different time-dependent models that capture the historical pattern of CO2 increase. All three fit with R2>0.98, are visually indistinguishable when overlaid, and match each other during the calibration period with R2>0.999. Projecting the models forward to 2100, the exponential model comes quite close to the Intergovernmental Panel on Climate Change (IPCC) best estimate of 836ppmv. The other two models project values far below the IPCC low estimates. The problem of characterizing historical CO2 levels is thus indeterminate, because multiple models fit the data equally well but forecast very different future trajectories.
Keywords: Greenhouse gases; Business as usual scenario; IPCC; Climate