Hochschule für Technik und Umwelt FHNW

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Autor:in: search.filters.author.Dommen, JosefThema: search.filters.subject.550 - Geowissenschaften

Bereich: Suchergebnisse

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  • Vorschaubild
    Publikation
    Fine and ultrafine particles in the Zürich (Switzerland) area measured with a mobile laboratory: an assessment of the seasonal and regional variation throughout a year
    (Copernicus, 24.09.2003) Bukowiecki, Nicolas; Dommen, Josef; Prévôt, André S.H.; Weingartner, Ernest; Baltensperger, Urs
    On occasion of the project YOGAM (year of gas phase and aerosol measurements), the spatial and temporal variation of selected aerosol and gas phase parameters was assessed for the Zürich (Switzerland) area with a new mobile pollutant measurement laboratory. This assessment based on on-road measurements along a specified route on selected days during different seasons in 2001/2002, covering urban, suburban and rural regions. Special focus was put on the investigation and characterization of particles in the fine (particle diameter D<2.5 mm) and ultrafine (D<100 nm) size ranges. Analysis of Variance (ANOVA) showed that the variance of all considered fine and ultrafine aerosol parameters (i.e. particle background and total number concentration for particles larger than 3 nm, number concentrations in the size ranges 7-30 nm and 80-140 nm, as well as the active surface area concentration) was significantly larger for day-to-day than for spatial variation. However, Principal Component Analysis (PCA) found a similar regional pollution pattern within every single measuring day. Lowest particle background levels (D>3 nm) were found in rural areas at higher elevation (15 000 cmˉ³), while corresponding mean background values for urban and freeway-influenced areas were typically 35 000 cmˉ³ and >80 000 cmˉ³, respectively. Meteorology, i.e. prevailing weather conditions not only governed the day-to-day concentration variations in the selected area, but also influenced the formation of primary (directly traffic-related) and in few cases secondary (biogenic or anthropogenic) ultrafine particles. Overall, low temperatures regularly enhanced primary ultrafine particle formation in urban areas. There was a possible indication for relatively low number concentrations of secondary ultrafine particles during a few warm and sunny spring days. Mobile measurements as they were performed in this study have been shown to be suitable for pollutant assessments to obtain good information on spatial and day-to-day variability. For experimental studies concerning spatial resolution on a relatively short time scale (<1 day), a mobile measurement design may even be more appropriate than a network of stationary measuring sites.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Kein Vorschaubild vorhanden
    Publikation
    A mobile pollutant measurement laboratory - measuring gas phase and aerosol ambient concentrations with high spatial and temporal resolution
    (Elsevier, 12/2002) Bukowiecki, Nicolas; Dommen, Josef; Prévôt, André S.H.; Richter, Rene; Weingartner, Ernest; Baltensperger, Urs
    A mobile pollutant measurement laboratory was designed and built at the Paul Scherrer Institute (Switzerland) for the measurement of on-road ambient concentrations of a large set of trace gases and aerosol parameters with high time resolution (<15 s for most instruments), along with geographical and meteorological information. This approach allowed for pollutant level measurements both near traffic (e.g. in urban areas or on freeways/main roads) and at rural locations far away from traffic, within short periods of time and at different times of day and year. Such measurements were performed on a regular base during the project year of gas phase and aerosol measurements (YOGAM). This paper presents data measured in the Zürich (Switzerland) area on a late autumn day (6 November) in 2001. The local urban particle background easily reached 50 000 cmˉ³, with additional peak particle number concentrations of up to 400 000 cmˉ³. The regional background of the total particle number concentration was not found to significantly correlate with the distance to traffic and anthropogenic emissions of carbon monoxide and nitrogen oxides. On the other hand, this correlation was significant for the number concentration of particles in the size range 50–150 nm, indicating that the particle number concentration in this size range is a better traffic indicator than the total number concentration. Particle number size distribution measurements showed that daytime urban ambient air is dominated by high number concentrations of ultrafine particles (nanoparticles) with diameters < 50 nm, which are immediately formed by traffic exhaust and thus belong to the primary emissions. However, significant variation of the nanoparticle mode was also observed in number size distributions measured in rural areas both at daytime and nighttime, suggesting that nanoparticles are not exclusively formed by primary traffic emissions. While urban daytime total number concentrations were increased by a factor of 10 compared to the nighttime background, corresponding factors for total surface area and total volume concentrations were 2 and 1.5, respectively.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Kein Vorschaubild vorhanden
    Publikation
    Evidence for the role of organics in aerosol particle formation under atmospheric conditions
    (National Academy of Sciences, 19.01.2010) Metzger, Axel; Verheggen, Bart; Dommen, Josef; Duplissy, Jonathan; Prévôt, André S.H.; Weingartner, Ernest; Riipinen, Ilona; Kulmala, Markku; Spracklen, Dominick V.; Carslaw, Kenneth S.; Baltensperger, Urs
    New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H2SO4 and organic condensable species. Nucleation occurs at H2SO4 concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H2SO4 and an organic molecule. This suggests that only one H2SO4 molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Kein Vorschaubild vorhanden
    Publikation
    Aerosol nucleation and growth in a mixture of sulfuric acid/alpha-pinene oxidation products at the CERN CLOUD chamber
    (AIP Publishing, 2013) Tröstl, Jasmin; Bianchi, Federico; Kürten, Andreas; Rondo, Linda; Simon, Mario; Sarnela, Nina; Jokinen, Tuija; Heinritzi, Martin; Dommen, Josef; Kirkby, Jasper; Weingartner, Ernest; Baltensperger, Urs; DeMott, Paul J.; O'Dowd, Colin D.
    The role of α-pinene in aerosol nucleation and growth was investigated using the CERN CLOUD chamber, a nano scanning mobility particle sizer (nanoSMPS) and several condensation particle counters (CPCs) with different diameter cut-offs. Different oxidation conditions for α-pinene - OH⋅ vs. ozone oxidation - were considered to investigate their contributions to particle nucleation and growth. Results from the latest CERN experiment from fall 2012 (CLOUD 7) are presented.
    04B - Beitrag Konferenzschrift
  • Kein Vorschaubild vorhanden
    Publikation
    Laboratory observation of oligomers in the aerosol from isoprene/NOₓ photooxidation
    (Wiley, 2006) Dommen, Josef; Metzger, Axel; Duplissy, Jonathan; Kalberer, Markus; Alfarra, M. Rami; Gascho, Astrid; Weingartner, Ernest; Prévôt, André S.H.; Verheggen, Bart; Baltensperger, Urs
    Compounds assigned to be oxidation products of isoprene (2-methyl-1,3-butadiene) have recently been observed in ambient aerosols, suggesting that isoprene might play an important role in secondary organic aerosol (SOA) formation due to its large global source strength. SOA yields from photooxidation of isoprene and NOₓ in a chamber agree fairly well with previous data. Matrix assisted laser desorption/ionization mass spectrometry showed the formation of high molecular weight compounds over the course of 15-hour experiments. Concurrently, the volatility of the SOA decreased markedly as observed by a tandem differential mobility analyzer. The volume fraction remaining of SOA at 150°C increased steadily from 5 to 25% during the same experiments. These observations are attributed to oligomerization reactions occurring in the aerosol phase. Under dry conditions a lower volatility was observed.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Kein Vorschaubild vorhanden
    Publikation
    Cloud forming potential of secondary organic aerosol under near atmospheric conditions
    (Wiley, 2008) Duplissy, Jonathan; Gysel, Martin; Alfarra, M. Rami; Dommen, Josef; Metzger, Axel; Prévôt, André S.H.; Weingartner, Ernest; Laaksonen, Ari; Raatikainen, Tomi; Good, Nicholas; Turner, S. Fiona; McFiggans, Gordon; Baltensperger, Urs
    Cloud droplets form by nucleation on atmospheric aerosol particles. Populations of such particles invariably contain organic material, a major source of which is thought to be condensation of photo‐oxidation products of biogenic volatile organic compounds (VOCs). We demonstrate that smog chamber studies of the formation of such biogenic secondary organic aerosol (SOA) formed during photo‐oxidation must be conducted at near atmospheric concentrations to yield atmospherically representative particle composition, hygroscopicity and cloud‐forming potential. Under these conditions, the hygroscopicity measured at 95% relative humidity can be used reliably to predict the CCN activity of the SOA particles by assuming droplet surface tension of pure water. We also show that the supersaturation required to activate a given size of particle decreases with age.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild
    Publikation
    Impact of aftertreatment devices on primary emissions and secondary organic aerosol formation potential from in-use diesel vehicles: results from smog chamber experiments
    (Copernicus, 06.12.2010) Chirico, Roberto; DeCarlo, Peter F.; Heringa, Maarten F.; Tritscher, Torsten; Richter, René; Prévôt, André S. H.; Dommen, Josef; Weingartner, Ernest; Wehrle, Günther; Gysel, Martin; Laborde, Marie; Baltensperger, Urs
    Diesel particulate matter (DPM) is a significant source of aerosol in urban areas and has been linked to adverse health effects. Although newer European directives have introduced increasingly stringent standards for primary PM emissions, gaseous organics emitted from diesel cars can still lead to large amounts of secondary organic aerosol (SOA) in the atmosphere. Here we present results from smog chamber investigations characterizing the primary organic aerosol (POA) and the corresponding SOA formation at atmospherically relevant concentrations for three in-use diesel vehicles with different exhaust aftertreatment systems. One vehicle lacked exhaust aftertreatment devices, one vehicle was equipped with a diesel oxidation catalyst (DOC) and the third vehicle used both a DOC and diesel particulate filter (DPF). The experiments presented here were obtained from the vehicles at conditions representative of idle mode, and for one car in addition at a speed of 60 km/h. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was used to measure the organic aerosol (OA) concentration and to obtain information on the chemical composition. For the conditions explored in this paper, primary aerosols from vehicles without a particulate filter consisted mainly of black carbon (BC) with a low fraction of organic matter (OM, OM/BC < 0.5), while the subsequent aging by photooxidation resulted in a consistent production of SOA only for the vehicles without a DOC and with a deactivated DOC. After 5 h of aging ~80% of the total organic aerosol was on average secondary and the estimated "emission factor" for SOA was 0.23–0.56 g/kg fuel burned. In presence of both a DOC and a DPF, only 0.01 g SOA per kg fuel burned was produced within 5 h after lights on. The mass spectra indicate that POA was mostly a non-oxidized OA with an oxygen to carbon atomic ratio (O/C) ranging from 0.10 to 0.19. Five hours of oxidation led to a more oxidized OA with an O/C range of 0.21 to 0.37.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Kein Vorschaubild vorhanden
    Publikation
    Secondary organic aerosols from anthropogenic and biogenic precursors
    (Royal Society of Chemistry, 2005) Baltensperger, Urs; Kalberer, Markus; Dommen, Josef; Paulsen, Dwane; Alfarra, M. Rami; Coe, Hugh; Fisseha, Rebeka; Gascho, Astrid; Gysel, Martin; Nyeki, Stephan; Sax, Mirjam; Steinbacher, Martin; Prévôt, André S.H.; Sjögren, Staffan; Weingartner, Ernest; Zenobi, Renato
    Secondary organic aerosol (SOA) formation from the photooxidation of an anthropogenic (1,3,5-trimethylbenzene) and a biogenic (α-pinene) precursor was investigated at the new PSI smog chamber. The chemistry of the gas phase was followed by proton transfer reaction mass spectrometry, while the aerosol chemistry was investigated with aerosol mass spectrometry, ion chromatography, laser desorption ionization mass spectrometry, and infrared spectroscopy, along with volatility and hygroscopicity studies. Evidence for oligomer formation for SOA from both precursors was given by an increasing abundance of compounds with a high molecular weight (up to 1000 Da) and by an increasing thermal stability with increasing aging time. The results were compared to data obtained from ambient aerosol samples, revealing a number of similar features.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Kein Vorschaubild vorhanden
    Publikation
    Identification of polymers as major components of atmospheric organic aerosols
    (Springer, 2004) Kalberer, Markus; Paulsen, Dwane; Sax, Mirjam; Steinbacher, Martin; Dommen, Josef; Prévôt, André S.H.; Fisseha, Rebeka; Weingartner, Ernest; Frankevich, Vladimir; Zenobi, Renato; Baltensperger, Urs
    Results from photooxidation of aromatic compounds in a reaction chamber show that a substantial fraction of the organic aerosol mass is composed of polymers. This polymerization results from reactions of carbonyls and their hydrates. After aging for more than 20 hours, about 50% of the particle mass consists of polymers with a molecular mass up to 1000 daltons. This results in a lower volatility of this secondary organic aerosol and a higher aerosol yield than a model using vapor pressures of individual organic species would predict.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild
    Publikation
    Investigations of primary and secondary particulate matter of different wood combustion appliances with a high-resolution time-of-flight aerosol mass spectrometer
    (Copernicus, 23.06.2011) Heringa, Maarten F.; DeCarlo, Peter F.; Chirico, Roberto; Tritscher, Torsten; Dommen, Josef; Weingartner, Ernest; Richter, René; Wehrle, Günther; Prévôt, André S.H.; Baltensperger, Urs
    A series of photo-oxidation smog chamber experiments were performed to investigate the primary emissions and secondary aerosol formation from two different log wood burners and a residential pellet burner under different burning conditions: starting and flaming phase. Emissions were sampled from the chimney and injected into the smog chamber leading to primary organic aerosol (POA) concentrations comparable to ambient levels. The composition of the aerosol was measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and black carbon (BC) instrumentation. The primary emissions were then exposed to xenon light to initiate photo-chemistry and subsequent secondary organic aerosol (SOA) production. After correcting for wall losses, the average increase in organic matter (OM) concentrations by SOA formation for the starting and flaming phase experiments with the two log wood burners was found to be a factor of 4.1±1.4 after five hours of aging. No SOA formation was observed for the stable burning phase of the pellet burner. The startup emissions of the pellet burner showed an increase in OM concentration by a factor of 3.3. Including the measured SOA formation potential, average emission factors of BC+POA+SOA, calculated from CO2 emission, were found to be in the range of 0.04 to 3.9 g/kg wood for the stable burning pellet burner and an old log wood burner during startup respectively. SOA contributed significantly to the ion C2H4O2+ at mass to charge ratio m/z 60, a commonly used marker for primary emissions of wood burning. This contribution at m/z 60 can overcompensate for the degradation of levoglucosan leading to an overestimation of the contribution of wood burning or biomass burning to the total OM. The primary organic emissions from the three different burners showed a wide range in O:C atomic ratio (0.19−0.60) for the starting and flaming conditions, which also increased during aging. Primary wood burning emissions have a rather low relative contribution at m/z 43 (f 43) to the total organic mass spectrum. The non-oxidized fragment C3H7+ has a considerable contribution at m/z 43 for the fresh OA with an increasing contribution of the oxygenated ion C2H3O+ during aging. After five hours of aging, the OA has a rather low C2H3O+ signal for a given CO2+ fraction, possibly indicating a higher ratio of acid to non-acid oxygenated compounds in wood burning OA compared to other oxygenated organic aerosol (OOA).
    01A - Beitrag in wissenschaftlicher Zeitschrift