Hochschule für Technik und Umwelt FHNW
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Publikation Simultaneous dry and ambient measurements of aerosol size distributions at the Jungfraujoch(Stockholm University Press, 01.01.2003) Nessler, R.; Bukowiecki, Nicolas; Henning, Silvia; Weingartner, Ernest; Calpini, Bertrand; Baltensperger, UrsIn a field campaign at the high-alpine site Jungfraujoch (JFJ, 3580 m asl), in-situ aerosol size distributions were measured simultaneously outdoor at ambient conditions (temperature T < -5 °C) and indoor at dry conditions (T ≈ 25 °C and relative humidity RH < 10%) by means of two scanning mobility particle sizers (SMPS). In addition, measurements of hygroscopic growth factors were performed with a hygroscopicity tandem differential mobility analyzer (H-TDMA). The measured growth factors, being a monotonic function of the relative humidity (RH), were fitted with a modified Köhler model. A comparison between dry and ambient size distributions shows two main features: First, the dry total number concentration is often considerably smaller (on average 28%) than the ambient total number concentration, and is most likely due to the evaporation of volatile material at the higher temperature. These particle losses mainly concern small particles (dry diameter D ≲ 100 nm), and therefore have only a minimal affect on the surface and volume concentrations. A slight correlation between ambient RH and the magnitude of particle loss was observed, but it was not possible to establish an empirical model for a quantification. Second, the dry number size distribution is shifted towards smaller particles, reflecting the hygroscopic behavior of the aerosols. To link the ambient and the dry size distributions we modeled this shift using the H-TDMA measurements and a modified Köhler model. The corrected dry surface and volume concentrations are in good agreement with the ambient measurements for the whole RH range, but the correction works best for RH < 80%. The results indicate that size distribution data measured at indoor conditions (i.e. dry and warm) may be successfully corrected to reflect ambient conditions, which are relevant for determining the impact of aerosol on climate.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation 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, UrsA 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 ZeitschriftPublikation Separation of volatile and non-volatile aerosol fractions by thermodesorption. instrumental development and applications(Elsevier, 04/2001) Burtscher, Heinz; Baltensperger, Urs; Bukowiecki, Nicolas; Cohn, P.; Hüglin, Christoph; Mohr, Martin; Matter, Urs; Nyeki, Stephan; Schmatloch, Volker; Streit, Niklaus; Weingartner, ErnestAn instrument to remove volatile material from aerosol particles by thermal desorption is presented. The thermodesorber consists of a heated tube, where volatile material is desorbed from the particles, and a water- or air-cooled tube, consisting of activated charcoal. This last tube removes desorbed material and thus prevents it from re-adsorbing onto particles. Although designed for measuring particulate emissions from combustion processes it can also be applied to atmospheric aerosols. After theoretical and experimental determination of thermodesorber operating characteristics (temperature profile, losses, removal of desorbed material), examples of applications in several fields are given. Examples of atmospheric measurements at several remote and urban sites are presented. In combustion technology, the thermodesorber is applied to remove all volatile materials, allowing separation of volatile species and the non-volatile core (mainly elemental carbon) of combustion particles. Finally, the thermodesorber is used to study adsorption and desorption processes of polycyclic aromatic hydrocarbons on particles.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Real-time characterization of ultrafine and accumulation mode particles in ambient combustion aerosols(Elsevier, 08/2002) Bukowiecki, Nicolas; Kittelson, David B.; Watts, Winthrop F.; Burtscher, Heinz; Weingartner, Ernest; Baltensperger, UrsThe diffusion charging sensor (DC), photoelectric aerosol sensor (PAS) and condensation particle counter (CPC) are real-time particle instruments that have time resolutions < 10s and are suitable for field use. This paper shows how the relative fraction of nuclei mode particles (D ≤ 50nm) in ambient combustion aerosols can be determined, along with the coverage degree of the respective accumulation mode particles with a modal diameter of ~ 100nm. Main tools for interpretation are the diameter of average surface DAve,S (obtained from CPC and DC measurements) and PAS/DC versus DAve,S scatter plots. Compared to the scanning mobility particle sizer (SMPS), which is a standard instrument for aerosol particle size distribution measurements, the presented method has a limited accuracy, but is substantially faster. Additionally, it is experimentally less demanding than SMPS measurements, especially for field applications.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Contribution of railway traffic to local PM10 concentrations in Switzerland(Elsevier, 02/2007) Gehrig, Robert; Hill, Matz; Lienemann, Peter; Zwicky, Christoph N.; Bukowiecki, Nicolas; Weingartner, Ernest; Baltensperger, Urs; Buchmann, BrigitteField measurement campaigns of PM10 and its elemental composition (daily sampling on filters) covering different seasons were performed at two sites near the busiest railway station of Switzerland in Zurich (at a distance of 10 m from the tracks) and at a site near a very busy railway line with more than 700 trains per day. At this latter site parallel samples were taken at 10, 36 and 120 m distances from the tracks with the aim to study the distance dependence of the railway induced PM10 concentrations. To distinguish the relatively small railway emissions from the regional background (typically 20–25 μg m−3), simultaneous samples were also taken at an urban background site in Zurich. The differences in PM10 and elemental concentrations between the railway exposed sites and the background site were allocated to the railway contribution. Small, however, measurable PM10 concentration differences were found at all sites. The elemental composition of these differences revealed iron as the only quantitatively important constituent. As a long-term average it amounted to approximately 1 μg m−3 Fe at a distance of 10 m from the tracks at all three sites. Assuming that iron was at least partly oxidised (e.g. in the form of Fe2O3) the contribution can amount up to 1.5 μg m−3. Emissions of copper, manganese and chromium from trains were also clearly identified. However, compared to iron these, elements were emitted in very low quantities. No significant contribution from rock material (calcium, aluminium, magnesium, sodium) was observed as might have been expected from erosion, abrasion and resuspension from the gravel below the tracks. Particle emissions from diesel exhaust were not considered as trains in Switzerland are operated nearly exclusively by electric locomotives. The railway, induced contribution to ambient PM10 decreased rapidly with increasing distance from the tracks. At a distance of 120 m this contribution dropped to only 25% of the contribution observed at 10 m distance.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Trace metals in ambient air. Hourly size-segregated mass concentrations determined by synchrotron-XRF(American Chemical Society, 28.06.2005) Bukowiecki, Nicolas; Hill, Matthias; Gehrig, Robert; Zwicky, Christoph N.; Lienemann, Peter; Hegedüs, Ferenc; Falkenberg, Gerald; Weingartner, Ernest; Baltensperger, UrsTrace metals are ubiquitous in urban ambient air, with mass concentrations in the range of a few μg/m³ down to less than 100 pg/m³. To measure such low concentrations represents a challenge for chemical and physical analysis. In this study, ambient aerosol was collected in Zürich (Switzerland) in 1-h intervals and three size fractions (aerodynamic diameters 0.1−1 μm, 1−2.5 μm, and 2.5−10 μm), using a three-stage rotating drum impactor (RDI). The samples were analyzed by energy-dispersive Synchrotron radiation X-ray fluorescence spectrometry (SR-XRF) to obtain size-segregated hourly elemental aerosol mass concentrations for Cr, Mn, Fe, Cu, Zn, Br, and Pb, along with S, Cl, and Ca under the selected experimental conditions. The high sensitivity of SR-XRF allowed for detection limits of <50 pg/m³ for most of the above elements, with a net analysis time of only 15 s per sample. The data obtained with this technique illustrate that there is a considerable gain of relevant information when time resolution for measurements is increased from 1 day to 1 h. The individual size fractions of a specific element may show significantly different short-term patterns.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Deposition uniformity and particle size distribution of ambient aerosol collected with a rotating drum impactor(Taylor & Francis, 30.06.2009) Bukowiecki, Nicolas; Richard, Agnes; Furger, Markus; Weingartner, Ernest; Aguirre, Myriam; Huthwelker, Thomas; Lienemann, Peter; Gehrig, Robert; Baltensperger, UrsRotating drum impactors (RDI) are cascade type impactors used for size and time resolved aerosol sampling, mostly followed by spectrometric analysis of the deposited material. They are characterized by one rectangular nozzle per stage and are equipped with an automated stepping mechanism for the impaction wheels. An existing three-stage rotating drum impactor was modified, to obtain new midpoint cutoff diameters at 2.5 μm, 1 μm, and 0.1 μm, respectively. For RDI samples collected under ambient air conditions, information on the size-segregation and the spatial uniformity of the deposited particles are key factors for a reliable spectrometric analysis of the RDI deposits. Two aerodynamic particle sizers (APS) were used for the determination of the RDI size fractionation characteristics, using polydisperse laboratory room air as quasi-stable proxy for urban ambient air. This experimental approach was suitable for the scope of this study, but was subject to numerous boundary conditions that limit a general use. Aerodynamic stage penetration midpoint diameters were estimated to be 2.4 and 1.0 μm for the first two RDI stages. Additionally, the spatial uniformity and geometrical size distribution of the deposited aerosol were investigated using micro-focus synchrotron radiation X-ray fluorescence spectrometry (micro-SR-XRF) and transmission electron microscopy (TEM), respectively. The size distribution of the particles found on the TEM samples agreed well with the results from the APS experiments. The RDI deposits showed sufficient uniformity for subsequent spectrometric analysis, but in the 2.5–10 μm size range the particle area density was very low. All of the applied methods confirmed the theoretical cutoff values of the modified RDI and showed that compared to other cascade impactors, the determined stage penetration sharpness was rather broad for the individual impactor stages.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Iron, manganese and copper emitted by cargo and passenger trains in Zürich (Switzerland). Size-segregated mass concentrations in ambient air(Elsevier, 02/2007) Bukowiecki, Nicolas; Gehrig, Robert; Hill, Matthias; Lienemann, Peter; Zwicky, Christoph N.; Buchmann, Brigitte; Weingartner, Ernest; Baltensperger, UrsParticle emissions caused by railway traffic have hardly been investigated in the past, due to their obviously minor influence on air quality compared to automotive traffic. In this study, emissions related to particle abrasion from wheels and tracks were investigated next to a busy railway line in Zürich (Switzerland), where trains run nearly exclusively with electrical locomotives. Hourly size-segregated aerosol samples (0.1–1, 1–2.5 and 2.5–10 μm) were collected with a rotating drum impactor (RDI) and subsequently analyzed by synchrotron radiation X-ray fluorescence spectrometry (SR-XRF). In this way, hourly elemental mass concentrations were obtained for chromium, manganese, iron and copper, which are the elements most relevant for railway abrasion. Additionally, daily aerosol filters were collected at the same site as well as at a background site for subsequent analysis by gravimetry and wavelength dispersive XRF (WD-XRF). Railway related ambient air concentrations of iron and manganese were calculated for the coarse (2.5–10 μm) and fine (<2.5 μm) particle fraction by means of a Mn/Fe ratio investigation. The comparison to train type and frequency data showed that 75% and 60% of the iron and manganese mass concentrations related to cargo and passenger trains, respectively, were found in the coarse mode. The railway related iron mass concentration normalized by the train frequency ranges between 10 and 100 ng mˉ³ h iron in 10 m distance to the tracks, depending on train type. It is estimated that the personal exposure next to a busy railway line above ground is more than a magnitude lower than inside a subway station.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation A 17 month climatology of the cloud condensation nuclei number concentration at the high alpine site Jungfraujoch(Wiley, 24.05.2011) Jurányi, Zsófia; Gysel, Martin; Weingartner, Ernest; Bukowiecki, Nicolas; Kammermann, Lorenz; Baltensperger, UrsBetween May 2008 and September 2009 the cloud condensation nuclei (CCN) number concentration, NCCN, was measured at the high alpine site Jungfraujoch, which is located in the free troposphere most of the time. Measurements at 10 different supersaturations (0.12%–1.18%) were made using a CCN counter (CCNC). The monthly median NCCN values show a distinct seasonal variability with ∼5–12 times higher values in summer than in winter. The major part of this variation can be explained by the seasonal amplitude of total aerosol number concentration (∼4.5 times higher values in summer), but it is further amplified (factor of ∼1.1–2.6) by a shift of the particle number size distribution toward slightly larger sizes in summer. In contrast to the extensive properties, the monthly median of the critical dry diameter, above which the aerosols activate as CCN, does not show a seasonal cycle (relative standard deviations of the monthly median critical dry diameters at the different supersaturations are 4–9%) or substantial variability (relative standard deviations of individual data points at the different supersaturations are less than 18–37%). The mean CCN-derived hygroscopicity of the aerosol corresponds to a value of the hygroscopicity parameter κ of 0.20 (assuming a surface tension of pure water) with moderate supersaturation dependence. NCCN can be reliably predicted throughout the measurement period with knowledge of the above-mentioned averaged κ value and highly time-resolved (∼5 min) particle number size distribution data. The predicted NCCN was within 0.74 to 1.29 times the measured value during 80% of the time (94,499 data points in total at 10 different supersaturations).01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Analysis of long‐term aerosol size distribution data from Jungfraujoch with emphasis on free tropospheric conditions, cloud influence, and air mass transport(Wiley, 2015) Herrmann, Erik; Weingartner, Ernest; Henne, Stephan; Vuilleumier, Laurent; Bukowiecki, Nicolas; Steinbacher, Martin; Conen, Franz; Collaud Coen, Martine; Hammer, Emanuel; Jurányi, Zsófia; Baltensperger, Urs; Gysel, MartinSix years of aerosol size distribution measurements between 20 and 600 nm diameters and total aerosol concentration above 10 nm from March 2008 to February 2014 at the high‐alpine site Jungfraujoch are presented. The size distribution was found to be typically bimodal with mode diameters and widths relatively stable throughout the year and the observation period. New particle formation was observed on 14.5% of all days without a seasonal preference. Particles typically grew only into the Aitken mode and did not reach cloud condensation nucleus (CCN) sizes on the time scale of several days. Growth of preexisting particles in the Aitken mode, on average, contributed very few CCN. We concluded that the dominant fraction of CCN at Jungfraujoch originated in the boundary layer. A number of approaches were used to distinguish free tropospheric (FT) conditions and episodes with planetary boundary layer (PBL) influence. In the absence of PBL injections, the concentration of particles larger than 90 nm (N90, roughly corresponding to the CCN concentration) reached a value ~40 cm−3 while PBL influence caused N90 concentrations of several hundred or even 1000 cm−3. Comparing three criteria for free tropospheric conditions, we found FT prevalence for 39% of the time with over 60% during winter and below 20% during summer. It is noteworthy that a simple criterion based on standard trace gas measurements appeared to outperform alternative approaches.01A - Beitrag in wissenschaftlicher Zeitschrift