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Spatiotemporal distribution of carbonyl compounds in China
2015
Ho, K.F. | Ho, Steven Sai Hang | Huang, R.-J. | Dai, W.T. | Cao, J.J. | Tian, Linwei | Deng, W.J.
A sampling campaign was carried out at nine Chinese cities in 2010/2011. Fifteen monocarbonyls (C# = 1–9) were quantified. Temperature is the rate-determining factor of the summertime carbonyl levels. The carbonyl emissions in winter are mainly driven by the primary anthropogenic sources like automobile. A molar ratio of propionaldehyde to nonaldehyde is a barometer of the impact of atmospheric vegetation emission which suggesting that strong vegetation emissions exist in summer and high propionaldehyde abundance is caused by fossil fuel combustion in winter. Potential health risk assessment of formaldehyde and acetaldehyde was conducted and the highest cumulative risks were observed at Chengdu in summer and Wuhan in winter. Because of the strong photochemical reaction and large amount of anthropogenic emissions, high concentrations of carbonyl compounds were observed in Chengdu. The use of ethanol-blended gasoline in Wuhan is the key reason of acetaldehyde emission and action should be taken to avoid potential health risks.
Show more [+] Less [-]Concentrations of polycyclic aromatic hydrocarbons in resuspendable fraction of settled bus dust and its implications for human exposure
2015
Gao, Peng | Liu, Sa | Feng, Yujie | Lin, Nan | Lu, Binyu | Zhang, Zhaohan | Cui, Fuyi | Xing, Baoshan | Hammond, S Katharine
This preliminary study measured Polycyclic Aromatic Hydrocarbons (PAHs) concentrations in the resuspendable fraction of settled dust on 39 bus lines, to evaluate the impact of engine type (gasoline and compressed natural gas) on exposure for commuters and drivers. Benzo(b)fluoranthene(BbF) was the predominant PAH in resuspendable fraction of settled bus dust. The concentration of total PAHs was 92.90 ± 116.00 μg/g (range: 0.57–410) in gasoline buses and 3.97 ± 1.81 (range: 2.01–9.47) in compressed natural gas (CNG) buses. Based on Benzo[a]pyrene (BaP) equivalent concentrations for the sum of 16 PAHs, the average daily dose (ADD) via dust ingestion and dermal contact was calculated. The ADD of PAHs was higher for commuters and drivers in gasoline-powered buses than in buses using CNG buses. For both short and long duration journeys, young commuters were exposed to higher levels of PAHs via dust ingestion and dermal contact than adult commuters.
Show more [+] Less [-]Hydrophobic poly(alkoxysilane) organogels as sorbent material for oil spill cleanup
2015
Ozan Aydin, Gulsah | Bulbul Sonmez, Hayal
In this study, reusable poly(alkoxysilane) organogels with high absorption capacities were synthesized by the condensation of a cyclo aliphatic glycol (UNOXOL™) and altering the chain length of the alkyltriethoxysilanes. The structural and thermal properties of cross-linked poly(alkoxysilane) polymers were determined by FTIR, solid-state 13C and 29Si CPMAS NMR and TGA. The oil absorbency of poly(alkoxysilane)s was determined through oil absorption tests, absorption and desorption kinetics. Results showed that the highest oil absorbency capacities were found to be 295% for hexane, 389% for euro diesel, 428% for crude oil, 652% for gasoline, 792% for benzene, 792% for toluene, 868% for tetrahydrofuran, and 1060% for dichloromethane for the poly(alkoxysilane) gels based on UNOXOL™ and dodecyltriethoxysilane. Owing to their hydrophobic structure, the poly(alkoxysilane) organogels can selectively absorb crude oil from water. The reusability of the absorbents was quantitatively investigated, demonstrating that absorbents can be used effectively at least nine times.
Show more [+] Less [-]on–road measurement of gaseous emissions and fuel consumption for two hybrid electric vehicles in Macao
2015
Wu, Xiaomeng | Zhang, Shaojun | Wu, Ye | Li, Zhenhua | Ke, Wenwei | Fu, Lixin | Hao, Jiming
Hybrid electric vehicles (HEVs) are promoted in China to ease increasing pressures of urban air pollution and oil security. In this paper, we measured two Toyota Prius HEVs by using a portable emission measurement system (PEMS) to evaluate their real–world performance with regard to gaseous emission factors and fuel consumption. Our results indicated that their average exhaust emission factors of CO, THC, NOX and CO2 were 0.25±0.08 gkm–1, 0.015±0.002 gkm–1, 0.009±0.005 gkm–1 and 136±21 gkm–1 (i.e., 5.81±0.90 L 100km–1 for fuel consumption) respectively, while driving the averaged on–road traffic pattern. Compared to conventional gasoline and diesel vehicles, the tested HEVs demonstrated significant advantages in simultaneously mitigating major air pollutants (e.g., NOX), greenhouse gas emissions (CO2) and fuel consumption. For example, average CO2 emission factors are reduced by approximately 35% and 15% relative to conventional gasoline and diesel cars in Macao. Unlike conventional gasoline and diesel cars, relative CO2 emission factors of HEVs were much less sensitive to speed change, while their relative NOX emission factors were reduced as average speed became lower. This indicates significant environmental and energy benefits from HEVs under congested driving conditions. Our assessment suggests that HEVs are a competitive technology option for the taxi fleet in Macao with strong advantages in saving fuel cost for taxi drivers and mitigating NOX emissions.
Show more [+] Less [-]Electrospun PS/PAN fibers with improved mechanical property for removal of oil from water
2015
Li, Peng | Qiao, Ying | Zhao, Lili | Yao, Dahu | Sun, Haixiang | Hou, Yingfei | Li, Shuo | Li, Qi
A mechanically robust and high-capacity oil sorbent is prepared by electrospinning a blend of polystyrene (PS) and polyacrylonitrile (PAN). The morphology, oil sorption capacity and mechanical property of the fibers formed in different compositions are investigated in detail. It is shown that the oil sorption capacity is a result of both the chemical composition and the specific surface area which related to diameter size. The addition of PAN as a component in fibrous sorbents can significantly improve the mechanical properties of PS fibers. Moreover, the oil sorption capacity increases with decreasing fiber diameter. The results also show that the maximum sorption capacities of the PS/PAN sorbent for pump oil, peanut oil, diesel, and gasoline were 194.85, 131.70, 66.75, and 43.38gg−1, respectively. Additionally, the sorbent exhibits quick oil sorption speed as well as high buoyancy, which make it a promising candidate for use as an oil spill cleanup sorbent.
Show more [+] Less [-]Characterization of VOC sources in an urban area based on PTR-MS measurements and receptor modelling
2015
Stojić, A. | Stojić, S Stanišić | Šoštarić, A. | Ilić, L. | Mijić, Z. | Rajšić, S.
In this study, the concentrations of volatile organic compounds were measured by the use of proton transfer reaction mass spectrometry, together with NO ₓ , NO, NO₂, SO₂, CO and PM₁₀ and meteorological parameters in an urban area of Belgrade during winter 2014. The multivariate receptor model US EPA Unmix was applied to the obtained dataset resolving six source profiles, which can be attributed to traffic-related emissions, gasoline evaporation/oil refineries, petrochemical industry/biogenic emissions, aged plumes, solid-fuel burning and local laboratories. Besides the vehicle exhaust, accounting for 27.6 % of the total mixing ratios, industrial emissions, which are present in three out of six resolved profiles, exert a significant impact on air quality in the urban area. The major contribution of regional and long-range transport was determined for source profiles associated with petrochemical industry/biogenic emissions (40 %) and gasoline evaporation/oil refineries (29 %) using trajectory sector analysis. The concentration-weighted trajectory model was applied with the aim of resolving the spatial distribution of potential distant sources, and the results indicated that emission sources from neighbouring countries, as well as from Slovakia, Greece, Poland and Scandinavian countries, significantly contribute to the observed concentrations.
Show more [+] Less [-]Identifying sources of Pb pollution in urban soils by means of MC-ICP-MS and TOF-SIMS
2015
Rodríguez-Seijo, Andrés | Arenas-Lago, Daniel | Andrade, María Luisa | Vega, Flora A.
Lead pollution was evaluated in 17 urban soils from parks and gardens in the city of Vigo (NW Spain). The Pb isotope ratios (²⁰⁷Pb/²⁰⁶Pb,²⁰⁸Pb/²⁰⁴Pb,²⁰⁶Pb/²⁰⁴Pb and²⁰⁸Pb/²⁰⁶Pb) were determined after being measured by MC-ICP-MS. The association of the isotopes (²⁰⁴Pb,²⁰⁶Pb,²⁰⁷Pb and²⁰⁸Pb) with the different components of the soil was studied using TOF-SIMS. The isotopic ranges obtained for the samples were between 1.116 and 1.203 (²⁰⁶Pb/²⁰⁷Pb), 2.044–2.143 (²⁰⁸Pb/²⁰⁶Pb), 37.206–38.608 (²⁰⁸Pb/²⁰⁴Pb), 15.5482–15.6569 (²⁰⁷Pb/²⁰⁴Pb) and 17.357–18.826 (²⁰⁶Pb/²⁰⁴Pb). The application of the three-end-member model indicates that the Pb derived from petrol is the main source of Pb in the soils (43.51 % on average), followed by natural or geogenic Pb (39.12 %) and industrial emissions (17.37 %). The emissions derived from coal combustion do not appear to influence the content of Pb in the soil. TOF-SIMS images show that the Pb mainly interacts with organic matter. This technique contributes to the understanding of the association of anthropogenic Pb with the components of the soil, as well as the particle size of these associations, thus allowing the possible sources of Pb to be identified.
Show more [+] Less [-]Elements and polycyclic aromatic hydrocarbons in exhaust particles emitted by light-duty vehicles
2015
Alves, Célia A. | Barbosa, Cátia | Rocha, Sonia | Calvo, Ana | Nunes, Teresa | Cerqueira, Mário | Pio, Casimiro | Karanasiou, Angeliki | Querol, X. (Xavier)
The main purpose of this work was to evaluate the chemical composition of particulate matter (PM) emitted by eight different light-duty vehicles. Exhaust samples from petrol and diesel cars (Euro 3 to Euro 5) were collected in a chassis dynamometer facility. To simulate the real-world driving conditions, three ARTEMIS cycles were followed: road, to simulate a fluid traffic flow and urban with hot and cold starts, to simulate driving conditions in cities. Samples were analysed for the water-soluble ions, for the elemental composition and for polycyclic aromatic hydrocarbons (PAHs), respectively, by ion chromatography, inductively coupled plasma atomic emission spectroscopy (ICP-AES), inductively coupled plasma mass spectrometry (ICP-MS) and gas chromatography-mass spectrometry (GC-MS). Nitrate and phosphate were the major water-soluble ions in the exhaust particles emitted from diesel and petrol vehicles, respectively. The amount of material emitted is affected by the vehicle age. For vehicles ≥Euro 4, most elements were below the detection limits. Sodium, with emission factors in the ranges 23.5–62.4 and 78.2–227μg km⁻¹, for petrol and diesel Euro 3 vehicles, respectively, was the major element. The emission factors of metallic elements indicated that diesel vehicles release three to five times more than petrol automobiles. Element emissions under urban cycles are higher than those found for on-road driving, being three or four times higher, for petrol vehicles, and two or three times, for diesel vehicles. The difference between cycles is mainly due to the high emissions for the urban cycle with hot start-up. As registered for elements, most of the PAH emissions for vehicles ≥Euro 4 were also below the detection limits. Regardless of the vehicle models or driving cycles, the two- to four-ring PAHs were always dominant. Naphthalene, with emission factors up to 925 μg km⁻¹, was always the most abundant PAH. The relative cancer risk associated with naphthalene was estimated to be up to several orders of magnitude higher than any of the chemical species found in the PM phase. The highest PAH emission factors were registered for diesel-powered vehicles. The condition of the vehicle can exert a decisive influence on both element and PAH emissions.
Show more [+] Less [-]Atmospheric reactions of methylcyclohexanes with Cl atoms and OH radicals: determination of rate coefficients and degradation products
2015
Ballesteros, Bernabé | Ceacero-Vega, Antonio A. | Jiménez, Elena | Albaladejo, José
As the result of biogenic and anthropogenic activities, large quantities of chemical compounds are emitted into the troposphere. Alkanes, in general, and cycloalkanes are an important chemical class of hydrocarbons found in diesel, jet and gasoline, vehicle exhaust emissions, and ambient air in urban areas. In general, the primary atmospheric fate of organic compounds in the gas phase is the reaction with hydroxyl radicals (OH). The oxidation by Cl atoms has gained importance in the study of atmospheric reactions because they may exert some influence in the boundary layer, particularly in marine and coastal environments, and in the Arctic troposphere. The aim of this paper is to study of the atmospheric reactivity of methylcylohexanes with Cl atoms and OH radicals under atmospheric conditions (in air at room temperature and pressure). Relative kinetic techniques have been used to determine the rate coefficients for the reaction of Cl atoms and OH radicals with methylcyclohexane, cis-1,4-dimethylcyclohexane, trans-1,4-dimethylcyclohexane, and 1,3,5-trimethylcyclohexane at 298 ± 2 K and 720 ± 5 Torr of air by Fourier transform infrared) spectroscopy and gas chromatography–mass spectrometry (GC-MS) in two atmospheric simulation chambers. The products formed in the reaction under atmospheric conditions were investigated using a 200-L Teflon bag and employing the technique of solid-phase microextraction coupled to a GC-MS. The rate coefficients obtained for the reaction of Cl atoms with the studied compounds are the following ones (in units of 10⁻¹⁰ cm³ molecule⁻¹ s⁻¹): (3.11 ± 0.16), (2.89 ± 0.16), (2.89 ± 0.26), and (2.61 ± 0.42), respectively. For the reactions with OH radicals the determined rate coefficients are (in units of 10⁻¹¹ cm³ molecule⁻¹ s⁻¹): (1.18 ± 0.12), (1.49 ± 0.16), (1.41 ± 0.15), and (1.77 ± 0.23), respectively. The reported error is twice the standard deviation. A detailed mechanism for ring-retaining product channels is proposed to justify the observed reaction products. The global tropospheric lifetimes estimated from the reported OH- and Cl-rate coefficients show that the main removal path for the investigated methylcyclohexanes is the reaction with OH radicals. But in marine environments, after sunrise, Cl reactions become more important in the tropospheric degradation. Thus, the estimated lifetimes range from 16 to 24 h for the reactions of the OH radical (calculated with [OH] = 10⁶ atoms cm⁻³) and around 7–8 h in the reactions with Cl atoms in marine environments (calculated with [Cl] = 1.3 × 10⁵ atoms cm⁻³). The reaction of Cl atoms and OH radicals and methylcylohexanes can proceed by H abstraction from the different positions.
Show more [+] Less [-]Identification of refined petroleum products in contaminated soils using an identification index for GC chromatograms
2015
Kwon, Dongwook | Ko, Myoung-Soo | Yang, Jung-Seok | Kwon, Man Jae | Lee, Seung-Woo | Lee, Seunghak
Hydrocarbons found in the environment are typically characterized by gas chromatography (GC). The shape of the GC chromatogram has been used to identify the source of petroleum contamination. However, the conventional practice of simply comparing the peak patterns of source products to those of environmental samples is dependent on the subjective decisions of individual analysts. We have developed and verified a quantitative analytical method for interpreting GC chromatograms to distinguish refined petroleum products in contaminated soils. We found that chromatograms for gasoline, kerosene, and diesel could be divided into three ranges with boundaries at C₆, C₈, C₁₆, and C₂₆. In addition, the relative peak area (RPAGC) of each range, a dimensionless ratio of the peak area within each range to that of the total range (C₆–C₂₆), had a unique value for each petroleum product. An identification index for GC chromatograms (IDGC), defined as the ratio of RPAGC of C₈–C₁₆ to that of C₁₆–C₂₆, was able to identify diesel and kerosene sources in samples extracted from artificially contaminated soils even after weathering. Thus, the IDGC can be used to effectively distinguish between refined petroleum products in contaminated soils.
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