| 1. |
- Fick, Jerker, et al.
(författare)
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A study of the gas-phase ozonolysis of terpenes: the impact of radicals formed during the reaction
- 2002
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Ingår i: Atmospheric Environment. - 1352-2310 .- 1873-2844. ; 36:20, s. 3299-3308
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Tidskriftsartikel (refereegranskat)abstract
- The gas-phase ozonolysis of α-pinene, Δ3-carene and limonene was investigated at ppb levels and the impact of the ozone, relative air humidity (RH), and time was studied using experimental design. The amounts of terpene reacted varied in the different settings and were as high as 8.1% for α-pinene, 10.9% forΔ3-carene and 23.4% for limonene. The designs were able to describe almost all the variation in the experimental data and were also successful in predicting omitted values. The results described the effects of time and ozone and also showed that RH did not have a statistically significant effect on the ozonolysis. The results also showed that all three terpenes were affected by an additional oxidation of OH radicals and/or other reactive species. The results from the designs states that this additional oxidation was responsible for 40% of the total amount of α-pinene reacted, 33% of the total amount of Δ3-carene reacted and 41% of the total amount of limonene reacted at the settings 20 ppb terpene, 75 ppb ozone, 20% RH and a reaction time of 213 s. Additional experiments with 2-butanol as OH radical scavenger showed that the reaction with OH radicals was responsible for 37% of the total α-pinene reacted and 39% of the total Δ3-carene reacted at the same settings. The scavenger experiments also showed that there were no significant amounts of OH radicals formed during the ozonolysis of limonene. The results from the designs were also compared to a mathematical model in order to evaluate further the data.
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| 2. |
- Janhäll, Sara, et al.
(författare)
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Vertical distribution of air pollutants at the Gustavii Cathedral in Göteborg, Sweden
- 2003
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Ingår i: Atmospheric Environment. - : Elsevier. - 1352-2310 .- 1873-2844. ; 37:2, s. 209-217
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric trace gases and particles were measured at two heights at the Gustavii Cathedral in Göteborg, Sweden, during 7 weeks in September and October 1999. The Gustavii Cathedral is situated in the city centre of Göteborg, which is near the harbour area and encircled by heavy traffic some hundred metres away. The main body of the church is as high as the surrounding buildings, while the tower extends well above. The sampling points were placed on the west wall of the tower at 10 and 32 meter height, i.e. well below and above the roof top level of surrounding buildings, respectively.Sulphur dioxide and nitric acid were sampled using the denuder technique and analysed by Ion Chromatography, IC. Total suspended particulates (TSP) were sampled using filter cups and subsequently analysed by energy dispersive X-ray fluorescence spectroscopy (EDXRF). In addition to the diurnal sampling of species, nitrogen oxides were measured using chemiluminescence detectors. Additional data from the Environmental Office in Göteborg was used in the analysis.Differences between the concentrations measured at the upper and lower levels were calculated and their variation and dependence on meteorological factors were evaluated. On the average larger concentrations were found at the lower level for soil derived elements and TSP, while nitric acid and nitric oxide showed larger concentrations at the upper level. Sulphur dioxide and nitrogen dioxide, as well as many of the elements in the TSP, showed equal concentrations at the two levels. However, depending on wind direction the measured differences of nitrogen oxides could be both positive and negative.
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| 3. |
- Libiseller, Claudia, 1975-, et al.
(författare)
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Model selection for local and regional meteorological normalisation of background concentrations of tropospheric ozone
- 2003
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Ingår i: Atmospheric Environment. - 1352-2310 .- 1873-2844. ; 37:28, s. 3923-3931
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Tidskriftsartikel (refereegranskat)abstract
- Meteorological normalisation of time series of air quality data aims to extract anthropogenic signals by removing natural fluctuations in the collected data. We showed that the currently used procedures to select normalisation models can cause over-fitting to observed data and undesirable smoothing of anthropogenic signals. A simulation study revealed that the risk of such effects is particularly large when: (i) the observed data are serially correlated, (ii) the normalisation model is selected by leave-one-out cross-validation, and (iii) complex models, such as artificial neural networks, are fitted to data. When the size of the test sets used in the cross-validation was increased, and only moderately complex linear models were fitted to data, the over-fitting was less pronounced. An empirical study of the predictive ability of different normalisation models for tropospheric ozone in Finland confirmed the importance of using appropriate model selection strategies. Moderately complex regional models involving contemporaneous meteorological data from a network of stations were found to be superior to single-site models as well as more complex regional models involving both contemporaneous and time-lagged meteorological data from a network of stations.
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| 4. |
- Molnár, Peter, 1967, et al.
(författare)
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Roadside measurements of fine and ultrafine particles at a major road north of Gothenburg
- 2002
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Ingår i: Atmospheric Environment. - 1352-2310 .- 1873-2844. ; 36:25, s. 4115-4123
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Tidskriftsartikel (refereegranskat)abstract
- Particle measurements were conducted at a road site 15 km north of the city of Gothenburg for 3 weeks in June 2000. The size distribution between 10 and 368 nm was measured continuously by using a differential mobility particle sizer (DMPS) system. PM2.5 was sampled on a daily basis with subsequent elemental analysis using EDXRF-spectroscopy. The road is a straight four-lane road with a speed limit of 90 kph. The road passing the site is flat with no elevations where the vehicles run on a steady workload and with constant speed. The traffic intensity is about 20,000 cars per workday and 13,000 vehicles per day during weekends. The diesel fuel used in Sweden is low in sulphur content (< 10 ppm) and therefore the diesel vehicles passing the site contribute less to particle emissions in comparison with other studies. A correlation between PM2.5 and accumulation mode particles (100-368 nm) was observed. However, no significant correlation was found between number concentrations of ultrafine particles (10-100 nm) and PM2.5 or the accumulation mode number concentration. The particle distribution between 10 and 368 nm showed great dependency on wind speed and wind direction, where the wind speed was the dominant factor for ultrafine (10-100nm) particle concentrations. The difference in traffic intensity between workday and weekend together with wind data made it possible to single out the traffic contribution to particle emissions and measure the size distribution. The results presented in combination with previous studies show that both PM2.5 and the mass of accumulation mode particles are bad estimates for ultrafine particles. (C) 2002 Elsevier Science Ltd. All rights reserved.
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| 5. |
- Pommer, Linda, et al.
(författare)
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Development of a NO2 scrubber for accurate sampling of ambient levels of terpenes
- 2002
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Ingår i: Atmospheric Environment. - 1352-2310 .- 1873-2844. ; 36:9, s. 1443-1452
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Tidskriftsartikel (refereegranskat)abstract
- The result of pumping air containing 56 ppb NO2 through a terpene-spiked adsorbent (90–130 ng, 90–100 ml min−1), Tenax TA, for 20 min (1.8–2.0 l) was that 8% of α-pinene, 7% of β-pinene, 21% of Δ3-carene and 5% of limonene were oxidised. In similar experiments with air containing 56 ppb O3, 3% of α-pinene, 4% of β-pinene, 10% of Δ3-carene and 38% of limonene were oxidised. Sampling a mixture of a terpene and NO2 using Tenax TA can give unwanted overestimation of the amount of reaction products from the terpene–NO2 reaction or underestimation of the original terpene levels. A scrubber was needed to reduce the problems caused by interfering reactions on the adsorbent of NO2 and to reduce discrimination of reactive compounds due to their relatively fast decay on the adsorbent. Several chemicals have been tested for their ability of removing NO2 and our objective was to develop a well functioning, reusable, easy to handle, easy manufactured NO2 scrubber. The result of the experiments was a scrubber consisting of two glass fibre filters coated with Na2SO3 assembled in a dust collector. The recovery of the terpenes through the scrubber varied between 75% and 97% at 15–75% relative humidity, and the scrubber is a one-use scrubber due to memory effects. The Na2SO3 scrubber could be stored in room air for at least one month without loosing the capacity of removing NO2.
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| 6. |
- Wingfors, Håkan, et al.
(författare)
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Characterisation and determination of profiles of polycyclic aromatic hydrocarbons in a traffic tunnel in Gothenburg, Sweden
- 2001
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Ingår i: Atmospheric Environment. - 1352-2310 .- 1873-2844. ; 35:36, s. 6361-6369
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Tidskriftsartikel (refereegranskat)abstract
- The concentrations of semi-volatile polycyclic aromatic hydrocarbons (PAHs), hydrocarbons (HCs), particulate matter (PM 1, 2.5 and 10 μm) and total suspended particles (TSPs) were measured in a traffic tunnel in Gothenburg, Sweden. Emission factors (EFs) were also calculated. These variables are assumed to provide good estimates of average vehicle emissions, since all types of vehicle, using all types of fuel, pass through this tunnel. It was shown that the majority of particle-associated PAHs were found on particles with an aerodynamic diameter of <1 μm. The concentrations of PAHs were one order higher in magnitude in air samples from the tunnel than in air samples at two urban locations. However, the PAH profiles of air samples from the tunnel and the urban sites were similar. This was demonstrated using principal component analysis (PCA). Finally, and notably, there was no significant change in the total emissions when the proportion of heavy-duty vehicles (HDVs) increased from 8% to 24%. Previously, diesel vehicles had been found to release larger quantities of PAHs and related substances. Advances in fuel quality, and HDV motor and exhaust system design during the last decade may have contributed to this promising result. However, it was shown, using partial least squares regression to latent structures (PLS), that some of the parameters measured displayed correlations with the proportions of HDVs and light-duty vehicles (LDVs). Concentrations of total HCs, TSPs, dibenzothiopene, phenantrene, anthracene and monomethyl-derivatives of phenantrene and anthracene were all correlated to the proportion of HDVs. The concentrations of naphthalene, some mono- and dimethylnaphthalenes and most large PAHs (with 5–7 fused rings) were correlated to the proportion of LDVs.
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| 7. |
- Gidhagen, Lars, et al.
(författare)
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Simulation of NOx and ultrafine particles in a street canyon in Stockholm, Sweden
- 2004
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 38:14
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Tidskriftsartikel (refereegranskat)abstract
- A computational fluid dynamic (CFD) model has been used to assess the concentrations of NOx and particle number in a street canyon in Stockholm with a high traffic volume. Comparisons of a simulated 11-week long time series of NOx with measurements (both sides of the street, urban background excluded) show good agreement, especially if emissions are distributed to be three times higher along the side of the street where the traffic is uphill, as compared to the downhill side. The simulation of number concentrations of inert particles indicates a similar asymmetry in emissions. A month-long measurement of particle size distribution (7–450 nm) at street level indicates that the ratio of nucleation size mode particle (7–20 nm) to total particle number (7–450 nm) is decreasing for increased particle surface area. Given the strong dominance of the locally generated particles over the urban background, this is interpreted as a local change in the size distribution. The results of a monodisperse aerosol dynamic model, coupled to the CFD model that simulates also the turbulence generated by vehicle movements, show that coagulation and deposition may reduce total particle inside the canyon with approximately 30% during low wind speeds. Most of the removal occurs shortly after emission, before the particles reach the leeward curb-side. Losses between the leeward curb-side and other locations in the street, e.g. roof levels, is estimated to be smaller, less than 10%. Coagulation is the dominating removal process under low wind speed conditions and deposition for higher wind speeds, the summed removal being smaller for high wind velocities. Deposition is enhanced over the road surface due to the velocities generated by vehicle movements. Although coagulation and deposition removal is most effective on the smallest ultrafine particles, this effect is not sufficient to explain the observed change in size distribution. It is suggested that also the formation of particles in the exhaust plumes is influenced by a larger particle surface area in the ambient air.
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| 8. |
- Gårdfeldt, Katarina, 1959, et al.
(författare)
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Evasion of Mercury from coastal and open waters of the Atlantic ocean and the Mediterranean sea
- 2003
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Ingår i: Atmospheric Environment. - 1352-2310 .- 1873-2844. ; 37:Suppl 1
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Tidskriftsartikel (refereegranskat)abstract
- Dissolved gaseous mercury (DGM) was measured in coastal Atlantic seawater and in the Mediterranean Sea. The Atlantic measurements were performed during September 1999 at the Mace Head Atmospheric Research Station, situated on the Irish west coast. The measurements in the Mediterranean Sea were made along a 6000 km cruise path from 14 July to 9 August 2000 in the framework of the Med-Oceanor project. Total gaseous mercury (TGM) concentrations in air were continuously measured with a 5 min time resolution using an automated mercury analyser (Tekran 2537A) during both expeditions. Paired TGM and DGM samples from all campaigns showed that the surface water was supersaturated with elemental mercury. The mercury evasion was estimated using a gas exchange model (J. Geophys. Res. 97 (1992) 7373), which uses salinity, wind speed and water temperature as independent parameters. The predicted average mercury evasion from the coastal Atlantic water was 2.7 ng m−2 h−1 implying that the concentration of TGM in the Atlantic air is enhanced by mercury evasion from the sea. Measurements in different regions of the Mediterranean Sea showed spatial variations in DGM concentrations. The highest DGM concentration (90 pg l−1) was observed at a location in the Strait of Sicily (37°16N 11°52E). The mercury evasion in the eastern sector of the Mediterranean Sea (area: 32–36°N, 17–28°E) was generally higher (7.9 ng m−2 h−1) than that observed in the Tyrrhenian Sea (4.2 ng m−2 h−1) or in the western sector (2.5 ng m−2 h−1) (areas: 38–42°N, 8–13°E and 38–41°N, 7–8°E, respectively). Estimations of mercury evasion were also made at Mediterranean coastal sites using a dynamic chamber technique. In addition, a newly developed method making continuous in situ DGM measurements possible was tested.
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| 9. |
- Gårdfeldt, Katarina, 1959, et al.
(författare)
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Oxidation of atomic mercury by hydroxyl radicals and photoinduced decomposition of methylmercury species in the aqueous phase
- 2001
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Ingår i: Atmospheric Environment. - 1352-2310 .- 1873-2844. ; 35:17, s. 3039-3047
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Tidskriftsartikel (refereegranskat)abstract
- The rate constant for Hg0+.OH, kHg0+.OH=(2.4±0.3)×109 M−1 s−1, in the aqueous phase was determined using a relative rate technique with methyl mercury as reference compound. The .OH initiated mercury reaction proceeds via the molecular Hg(I) radical which is oxidised to Hg(II) by dissolved O2. The reaction can be of importance under certain atmospheric circumstances, such as when the aqueous phase capacity of forming OH radicals is significant and the gas phase concentration of ozone drops. The same end product, i.e. Hg(II) was observed from the photodegradation of methylmercury hydroxide. In this case, molecular Hg(I) radicals are again likely to be formed after photodegradation of the Hg–C bond with subsequent oxidation. A lifetime of 230 h of methylmercury at outdoor conditions was estimated due to this reaction. The action of .OH on methylmercury species also involves breaking of organometallic bonds and formation of Hg(II). Speciation of these reaction products from methylmercury is important for the estimation of biogeochemical cycling of mercury.
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| 10. |
- Hazenkamp-Von Arx, M.E., et al.
(författare)
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PM2.5 and NO2 assessment in 21 European study centres of ECRHS II : annual means and seasonal differences
- 2004
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Ingår i: Atmospheric Environment. - : Elsevier. - 1352-2310 .- 1873-2844. ; 38:13, s. 1943-1953
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Tidskriftsartikel (refereegranskat)abstract
- The follow-up of cohorts of adults from more than 20 European centres of the former ECRHS I (1989-1992) investigates long-term effects of exposure to ambient air pollution on respiratory health, in particular asthma and change of pulmonary function. Since PM2.5 is not routinely monitored in Europe, we measured PM2.5 concentrations in 21 participating centres to estimate 'background' exposure in these cities. Winter (November-February), summer (May-August) and annual mean (all months) values of PM2.5 were determined from measuring periods between June 2000 and November 2001. Sampling was conducted for 7 days per month for a year. Annual and winter mean concentrations of PM2.5 vary substantially being lowest in Iceland and highest in centres in Northern Italy. Annual mean concentrations ranged from 3.7 to 44.9 mug m(-3), winter mean concentrations from 4.8 to 69.2 mug m(-3), and summer mean concentrations from 3.3 to 23.1 mugm(-3). Seasonal variability occurred but did not follow the same pattern across all centres. Therefore, ranking of centres varied from summer to winter. Simultaneously, NO2 concentrations were measured using passive sampling tubes. Annual mean NO2 concentrations range from 4.9 to 72.1 mug m(-3) with similar seasonal variations across centres and constant ranking of centres between seasons. The correlation between annual NO2 and PM2.5 concentrations is fair (Spearman correlation coefficient r(s) = 0.75), but when considered as monthly means the correlation is far less consistent and varies substantially between centres. The range of PM2.5 mass concentrations obtained in ECRHS II is larger than in other current cohort studies on long-term effects of air pollution. This substantial variation in PM2.5 exposure will improve statistical power in future multilevel health analyses and to some degree may compensate for the lack of information on within-city variability. Seasonal means may be used to indicate potential differences in the toxicity across the year. Across ECRHS cities annual NO2 might serve as a surrogate for PM2.5, especially for past exposure assessment, when PM2.5 is not available.
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