1. |
- Elfving, P, et al.
(author)
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In situ IR study on the initial sulphition and carbonation of Ca(OH)(2) and CaO by SO2 polluted air
- 1996
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In: Atmospheric Environment. - 1873-2844 .- 1352-2310. ; 30:23, s. 4085-4089
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Journal article (peer-reviewed)abstract
- Absorptions of SO2 and CO2 to fresh and aged forms of CaO and Ca(OH)2 are investigated at dry and humid conditions. Sulphite formation on Ca(OH)2 is found to be fairly independent of the relative humidity, while surface water is found to be a necessary condition for the corresponding carbonation reaction. Results supportive of Ca(OH)2 sulphition to be strongly preferred before carbonation at humid conditions are produced. Marked improvements in SO2 adsorption are seen for the fresh substrates. The observations are put in perspective of an on-going effort to understand the roles of SO2 in the deterioration of calcareous stone monuments, and are relevant to the chemistry of building materials.
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2. |
- Berglund, Johan, et al.
(author)
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Manganese-Catalyzed Autoxidation of Dissolved Sulfur Dioxide in the Atmospheric Aqueous Phase
- 1995
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In: Atmospheric Environment. - 1352-2310. ; 29:12, s. 1379-1391
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Journal article (peer-reviewed)abstract
- Autoxidation of SO2(aq) in the presence of manganese(II) is one of the important pathways for sulfuric acid formation in atmospheric clouds and fogs. Recent experimental results indicating that the catalyzed reaction takes place via a complex free-radical mechanism are discussed. Previous literature is reviewed in the light of this mechanism. Under atmospheric conditions of low total concentrations of manganese(II) ( < 2 × 10−5 M) and sulfur(IV) ( ≤ 10−5 M) and 2.5 < pH < 5, the rate law for conversion of SO2(aq) to SO3(aq) is reduced to d[S(IV)]/dt = k[Mn(II)][S(IV)], where [S(IV)] denotes the total concentration. A value of the overall rate constant k of 1.4 × 103 M−1s−1 is recommended for use in atmospheric model calculations.
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3. |
- Brandt, Christian, et al.
(author)
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Role of Chromium and Vanadium in the Atmospheric Oxidation of Sulfur(IV)
- 1998
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In: Atmospheric Environment. - 1352-2310. ; 32:4, s. 797-800
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Journal article (peer-reviewed)abstract
- Oxidation of HSO3- in aqueous solution has been studied in the presence of vanadium(V), chromium(III) and chromium(VI). Based on spectrophotometric kinetics data and product analysis it is concluded that the autoxidation rate of sulfur(IV) in slightly acidic solution is unaffected by the presence of vanadium(V) and chromium(III). Chromate(VI), on the other hand, oxidizes sulfur(IV) in a direct redox process in acidic solution. The overall rate of this reaction decreases with increasing pH and it becomes relatively slow in the atmospherically relevant pH range 4-6. Moreover, chromium(III) dominates strongly over chromium(VI) in the atmospheric aqueous phase. Hence, it is concluded that cations of vanadium vanadium and chromium have no significant influence on the atmospheric aqueous-phase oxidation of sulfur(IV) under most ambient atmospheric conditions. Only in very acidic droplets, direct redox between chromium(VI) and sulfite might be of some importance.
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4. |
- Cederfelt, S. I., et al.
(author)
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Field validation of the droplet aerosol analyser
- 1997
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In: Atmospheric Environment. - 1352-2310. ; 31:16, s. 2657-2670
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Journal article (peer-reviewed)abstract
- A new instrument for the study of cloud droplets and its relation to aerosol particles, the droplet aerosol analyser (DAA), was for the first time used in a field campaign. The DAA has the unique feature of measuring the ambient size of cloud droplets or cloud interstitial aerosol particles together with the size of its dry residue. This is obtained with a two-parameter data acquisition technique which results in a three-dimensional data set (ambient size, dry residue size, number concentration). The principle and design of the DAA is briefly described. The DAA was intercompared with differential mobility particle sizers, particulate volume monitors and a forward scattering spectrometer probe with respect to interstitial and cloud droplet dry residue size distribution as well as particle-size-dependent scavenging due to cloud droplet nucleation and for cloud droplet number concentration and size distribution and cloud liquid water concentration. Overall, the DAA showed good agreement with respect to all these six aerosol/cloud properties.
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5. |
- Choularton, T. W., et al.
(author)
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The Great Dun Fell Cloud Experiment 1993 : An overview
- 1997
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In: Atmospheric Environment. - 1352-2310. ; 31:16, s. 2393-2405
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Journal article (peer-reviewed)abstract
- The 1993 Ground-based Cloud Experiment on Great Dun Fell used a wide range of measurements of trace gases, aerosol particles and cloud droplets at five sites to study their sources and sinks especially those in cloud. These measurements have been interpreted using a variety of models. The conclusions add to our knowledge of air pollution, acidification of the atmosphere and the ground, eutrophication and climate change. The experiment is designed to use the hill cap cloud as a flow-through reactor, and was conducted in varying levels of pollution typical of much of the rural temperate continental northern hemisphere in spring-time.
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6. |
- Ferrara, R, et al.
(author)
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Atmospheric mercury concentrations and fluxes in the Almaden District (Spain)
- 1998
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In: Atmospheric Environment. - 1352-2310. ; 32:22, s. 3897-3904
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Journal article (peer-reviewed)abstract
- Atmospheric mercury levels around the world's largest mining and refining complex (Almaden, Spain) were determined during two field campaigns (September 1993 and February 1994) using both point monitors and lidar techniques. High mercury concentrations (0.1-5 mu g m(-3)) were measured over the village of Almaden in the prevailing wind direction. In the month of September the total mercury flux into the atmosphere was estimated to range from 600 to 1200 g h(-1). An attempt was made to measure the contribution from individual mercury sources. (C) 1998 Elsevier Science Ltd. All rights reserved.
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7. |
- Gieray, R., et al.
(author)
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Phase partitioning of aerosol constituents in cloud based on single-particle and bulk analysis
- 1997
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In: Atmospheric Environment. - 1352-2310. ; 31:16, s. 2491-2502
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Journal article (peer-reviewed)abstract
- Single-particle analysis, performed by laser microprobe mass spectrometry and bulk analytical techniques were used to study aerosol-cloud interactions within the third field campaign of the EUROTRAC subproject 'ground-based cloud experiments' at the Great Dun Fell, Cumbria, U.K. in spring 1993. The shape of the ridge made it possible for ground-based instrumentation to sample similar parcels of air before, during and after their transit through the cloud. A single jet five-stage minicascade impactor was used for sampling particles of the interstitial aerosol. A second impactor worked in tandem with a counter-flow virtual impactor and collected residues of cloud droplets. Considering marine conditions largest droplets nucleated on sea-salt particles, whereas smaller droplets were formed on sulphate and methane sulphonate containing particles. This clearly indicates chemical inhomogeneities in the droplet phase. Particles, which were disfavoured by droplet formation, often contained the highest amounts of water-insoluble carbonaceous matter. For the submicron size range we found that the carbonaceous matter was always internally mixed with sulphate. The fraction of carbonaceous matter increased with decreasing size. A detectable fraction of particles remained in the cloud interstitial air, although they were in size as well as in composition suitable to form cloud droplets. The findings confirm that nucleation is the most important process affecting phase partitioning in cloud, but that spatial and temporal variations of water vapour supersaturation have also an influence on the observed phase partitioning. Proton induced X-ray emission analysis and light absorption measurements of filter samples showed that the average scavenged fraction was 0.77 for sulphur and 0.57 for soot in clouds formed by continental influenced air and 0.62 and 0.44, respectively, for marine influenced clouds.
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8. |
- Martinsson, B. G., et al.
(author)
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Experimental determination of the connection between cloud droplet size and its dry residue size
- 1997
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In: Atmospheric Environment. - 1352-2310. ; 31:16, s. 2477-2490
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Journal article (peer-reviewed)abstract
- The droplet activation process and droplet growth was studied during early stages of the formation of orographically-induced clouds. The experimental results were compared with the results obtained with a closed parcel, adiabatic cloud model. Good agreement was in most cases found between model and measurements with respect to cloud droplet number concentration, cloud droplet solute concentration and particle sizes scavenged due to cloud droplet nucleation. The experimental results were mainly obtained with a new instrument, the droplet aerosol analyser (DAA), which allows the determination of ambient sizes of cloud droplets and interstitial aerosol particles directly connected with the size of its dry residue in a two-parameter data acquisition. The resulting three-dimensional data set (ambient size, dry size, number concentration) was utilised to determine several cloud/aerosol properties, whereof some unique.
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9. |
- Svenningsson, Birgitta, et al.
(author)
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Cloud droplet nucleation scavenging in relation to the size and hygroscopic behaviour of aerosol particles
- 1997
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In: Atmospheric Environment. - 1352-2310. ; 31:16, s. 2463-2475
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Journal article (peer-reviewed)abstract
- The size distributions and hygroscopic growth spectra of aerosol particles were measured during the GCE cloud experiment at Great Dun Fell in the Pennine Hills in northern England. Hygroscopic growth is defined as the particle diameter at 90% RH divided by the particle diameter at 10% RH. The fraction of the aerosol particles scavenged by cloud droplets as a function of particle size was also measured. The general aerosol type was a mixture of marine and aged anthropogenic aerosols. The Aitken and accumulation mode numbers (average ± 1 S.D.) were 1543 ± 1078 and 1023 ± 682 cm-3, respectively. The mean diameters were in the range 30-100 nm and 100-330 nm. The hygroscopic growth spectra were bimodal about half the time. The less-hygroscopic particles had average growth factors of 1.06, 1.06; 1.03, 1.03, and 1.03 for particle diameters of 50, 75, 110, 165, and 265 nm, respectively. For the more-hygroscopic particles of the same sizes, the average hygroscopic growth was 1.34, 1.37, 1.43, 1.47, and 1.53. The effects of ageing on the aerosol particle size distribution and on hygroscopic behaviour are discussed. The scavenged fraction of aerosol particles was a strong function of particle diameter. The diameter with 50% scavenging was in the range 90-220 nm. No tail of smaller particles activated to cloud drops was observed. A small tail of larger particles that remained in the interstitial aerosol can be explained by there being a small fraction of less-hygroscopic particles. A weak correlation between the integral dry particle diameter and the diameter with 50% scavenging was seen.
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10. |
- Swietlicki, Erik, et al.
(author)
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Source identification during the Great Dun Fell Cloud Experiment 1993
- 1997
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In: Atmospheric Environment. - 1352-2310. ; 31:16, s. 2441-2451
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Journal article (peer-reviewed)abstract
- A characterisation of the sources influencing the site for the final field campaign of the EUROTRAC subproject GCE (Ground-based Cloud Experiment) at Great Dun Fell, Cumbria, Great Britain in April-May 1993 is presented. The sources were characterised mainly by means of aerosol filter and cascade impactor data, single particle analysis, gas data, data on aromatic organic compounds, cloud water ionic composition, measurements of aerosol size distributions and hygroscopic properties and various meteorological information. Receptor models applied on the aerosol filter and impactor data sets separately revealed two major source types being a marine sea spray source and a long-range transported anthropogenic pollution source. The results of the receptor models were largely consistent with the other observations used in the source identification. Periods of considerable anthropogenic pollution as well as almost pure marine air masses were clearly identified during the course of the experiment.
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