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Carcinogenic organic content of particulate matter at urban locations with different pollution sources
Gordana Pehnec, Ivana Jakovljević, Ranka Godec, Sabina Žero, Jasna Huremović, Katja Džepina, Zdravka Sever Štrukil, 2020, izvirni znanstveni članek

Opis: Polycyclic aromatic hydrocarbons (PAHs) are compounds known for their adverse effects on human health. Many of them are proven carcinogens, especially those with 5 and 6 aromatic rings, which under normal tropospheric conditions are found in the particle-phase. Benzo(a)pyrene (BaP) is often measured as their general representative. Sarajevo, the capital of Bosnia and Herzegovina, is among the European cities with the poorest air quality. However, in Sarajevo PAHs are neither routinely measured within the air quality monitoring network nor have been a subject of extended, continuous field studies during the most polluted cold periods of the year. The capital of Croatia, Zagreb, is located approximately 300 km air distance north-west from Sarajevo. PAH mass concentrations in Zagreb have been measured continuously since 1994 within air quality monitoring networks. During winter 2017/2018, the SAFICA project (Sarajevo Canton Winter Field Campaign 2018) was carried out in order to characterize the chemical composition of organic and inorganic aerosol in the Sarajevo Canton. This paper presents the results of PAH measurements in the cities of Sarajevo and Zagreb at one urban location per city. Daily (24 h), continuous samples of PM10 (particulate matter with aerodynamic diameters ≤10 μm) were collected during heating season, from December 27, 2017 to February 27, 2018. Mass concentrations of eleven particle-phase PAHs in Sarajevo and Zagreb from filter samples collected during the same period were compared. The average BaP ambient mass concentrations in Sarajevo and Zagreb were 6.93 ng m−3 and 3.11 ng m−3, respectively. The contribution of BaP to the total PAH mass concentration was similar at both locations (11%). However, much higher contributions of particle-phase fluoranthene and pyrene were found in Sarajevo. Contributions of individual PAH, diagnostic ratios and factor analysis indicate that combustion of gasoline and diesel from vehicle traffic are a potential source of PAHs at both locations, as well as combustion of other liquid fossil fuels (petroleum and fuel oil). Wood burning was occasionally indicated as a PAH emission source in Zagreb, while in Sarajevo the contribution of PAHs from wood and coal combustion was more evident. Calculated value for total carcinogenic potency (TCP) of PAHs, which was estimated using toxic equivalence factors from the literature, in PM10 samples collected in Sarajevo was more than twice higher than in Zagreb (10.6 ng m−3 and 4.7 ng m−3, respectively). BaP had the highest contribution to the TCP at both locations (69 and 67%).
Najdeno v: osebi
Ključne besede: carcinogenic potency, diagnostic ratio, factor analysis, PM10, polycyclic aromatic hydrocarbons
Objavljeno: 09.04.2021; Ogledov: 72; Prenosov: 0
.pdf Polno besedilo (661,08 KB)

Evaluation of recently-proposed secondary organic aerosol models for a case study in Mexico City
Katja Džepina, R. M. Volkamer, Sasha Madronich, P. Tulet, I. M. Ulbrich, Q. Zhang, C. D. Cappa, P. J. Ziemann, Jose L. Jimenez, 2009, izvirni znanstveni članek

Opis: Recent field studies have found large discrepancies in the measured vs. modeled SOA mass loadings in both urban and regional polluted atmospheres. The reasons for these large differences are unclear. Here we revisit a case study of SOA formation in Mexico City described by Volkamer et al. (2006), during a photochemically active period when the impact of regional biomass burning is minor or negligible, and show that the observed increase in OA/Delta CO is consistent with results from several groups during MILAGRO 2006. Then we use the case study to evaluate three new SOA models: 1) the update of aromatic SOA yields from recent chamber experiments (Ng et al., 2007); 2) the formation of SOA from glyoxal (Volkamer et al., 2007a); and 3) the formation of SOA from primary semivolatile and intermediate volatility species (P-S/IVOC) (Robinson et al., 2007). We also evaluate the effect of reduced partitioning of SOA into POA (Song et al., 2007). Traditional SOA precursors (mainly aromatics) by themselves still fail to produce enough SOA to match the observations by a factor of similar to similar to 7. The new low-NOx aromatic pathways with very high SOA yields make a very small contribution in this high-NOx urban environment as the RO2 center dot+NO reaction dominates the fate of the RO2 center dot radicals. Glyoxal contributes several mu g m(-3) to SOA formation, with similar timing as the measurements. P-S/IVOC are estimated from equilibrium with emitted POA, and introduce a large amount of gas-phase oxidizable carbon that was not in models before. With the formulation in Robinson et al. (2007) these species have a high SOA yield, and this mechanism can close the gap in SOA mass between measurements and models in our case study. However the volatility of SOA produced in the model is too high and the O/C ratio is somewhat lower than observations. Glyoxal SOA helps to bring the O/C ratio of predicted and observed SOA into better agreement. The sensitivities of the model to some key uncertain parameters are evaluated.
Najdeno v: osebi
Ključne besede: polycyclic aromatic-hydrocarbons, positive matrix factorization, mass-spectrometry, volatility measurements
Objavljeno: 11.04.2021; Ogledov: 69; Prenosov: 0
.pdf Polno besedilo (1,18 MB)

Sources and transformations of particle-bound polycyclic aromatic hydrocarbons in Mexico City
L. C. Marr, Katja Džepina, Jose L. Jimenez, F. Reisen, H. L. Bethel, Janet Arey, J. S. Gaffney, N. A. Marley, Luisa T. Molina, Mario J. Molina, 2006, izvirni znanstveni članek

Opis: Understanding sources, concentrations, and transformations of polycyclic aromatic hydrocarbons (PAHs) in the atmosphere is important because of their potent mutagenicity and carcinogenicity. The measurement of particle-bound PAHs by three different methods during the Mexico City Metropolitan Area field campaign in April 2003 presents a unique opportunity for characterization of these compounds and intercomparison of the methods. The three methods are ( 1) collection and analysis of bulk samples for time-integrated gas- and particle-phase speciation by gas chromatography/ mass spectrometry; ( 2) aerosol photoionization for fast detection of PAHs on particles' surfaces; and ( 3) aerosol mass spectrometry for fast analysis of size and chemical composition. This research represents the first time aerosol mass spectrometry has been used to measure ambient PAH concentrations and the first time that fast, real-time methods have been used to quantify PAHs alongside traditional filter-based measurements in an extended field campaign. Speciated PAH measurements suggest that motor vehicles and garbage and wood burning are important sources in Mexico City. The diurnal concentration patterns captured by aerosol photoionization and aerosol mass spectrometry are generally consistent. Ambient concentrations of particle-phase PAHs typically peak at similar to 110 ng m(-3) during the morning rush hour and rapidly decay due to changes in source activity patterns and dilution as the boundary layer rises, although surface-bound PAH concentrations decay faster. The more rapid decrease in surface versus bulk PAH concentrations during the late morning suggests that freshly emitted combustion-related particles are quickly coated by secondary aerosol material in Mexico City's atmosphere and may also be transformed by heterogeneous reactions.
Najdeno v: osebi
Ključne besede: aerosol mass-spectrometer, aerodynamic diameter measurements, oxygenated organic aerosols, relative rate constants
Objavljeno: 12.04.2021; Ogledov: 90; Prenosov: 0
.pdf Polno besedilo (1,06 MB)

Molecular and physical characteristics of aerosol at a remote free troposphere site
Simeon K. Schum, Bo Zhang, Katja Džepina, Paulo Fialho, Claudio Mazzoleni, Lynn R. Mazzoleni, 2018, izvirni znanstveni članek

Opis: Aerosol properties are transformed by atmospheric processes during long-range transport and play a key role in the Earth’s radiative balance. To understand the molecular and physical characteristics of free tropospheric aerosol, we studied samples collected at the Pico Mountain Observatory in the North Atlantic. The observatory is located in the marine free troposphere at 2225m above sea level, on Pico Island in the Azores archipelago. The site is ideal for the study of long-range-transported free tropospheric aerosol with minimal local influence. Three aerosol samples with elevated organic carbon concentrations were selected for detailed analysis. FLEXPART retroplumes indicated that two of the samples were influenced by North American wildfire emissions transported in the free troposphere and one by North American outflow mainly transported within the marine boundary layer. Ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry was used to determine the detailed molecular composition of the samples. Thousands of molecular formulas were assigned to each of the individual samples. On average  60% of the molecular formulas contained only carbon, hydrogen, and oxygen atoms (CHO),  30% contained nitrogen (CHNO), and  10% contained sulfur (CHOS). The molecular formula compositions of the two wildfire-influenced aerosol samples transported mainly in the free troposphere had relatively low average O=C ratios (0:480:13 and 0:450:11) despite the 7–10 days of transport time according to FLEXPART. In contrast, the molecular composition of the North American outflow transported mainly in the boundary layer had a higher average O=C ratio (0:570:17) with 3 days of transport time. To better understand the difference between free tropospheric transport and boundary layer transport, the meteorological conditions along the FLEXPART simulated transport pathways were extracted from the Global Forecast System analysis for the model grids. We used the extracted meteorological conditions and the observed molecular chemistry to predict the relative-humidity-dependent glass transition temperatures (Tg) of the aerosol components. Comparisons of the Tg to the ambient temperature indicated that a majority of the organic aerosol components transported in the free troposphere were more viscous and therefore less susceptible to oxidation than the organic aerosol components transported in the boundary layer. Although the number of observations is limited, the results suggest that biomass burning organic aerosol injected into the free troposphere is more persistent than organic aerosol in the boundary layer having broader implications for aerosol aging.
Najdeno v: osebi
Ključne besede: secondary organic aerosols, brown carbon, particle dispersion model, ultrahigh-resolution FT-ICR MS, Pico Mountain Observatory
Objavljeno: 10.04.2021; Ogledov: 69; Prenosov: 0
.pdf Polno besedilo (5,35 MB)

Analysis of PM[sub](10), Pb, Cd, and Ni atmospheric concentrations during domestic heating season in Sarajevo, Bosnia and Herzegovina, from 2010 to 2019
Merjema Cepić, Amila Čeliković, Irma Musić, Midheta Bašić, Nudžeima Huseinbašić, Katja Džepina, Jasna Huremović, Sabina Žero, Erna Bubalo, Minela Dacić, 2020, izvirni znanstveni članek

Opis: This paper examines atmospheric concentrations of particulate matter with an aerodynamic diameter smaller than 10 μm (PM10) and related particle-phase toxic heavy metals Cd, Ni, and Pb during domestic heating seasons from 2010 to 2019 in Sarajevo, Bosnia and Herzegovina. In total, 242 daily PM10 samples were collected using medium and high volume air samplers. The mean daily PM10 mass concentration for all measurements is 75.16 μg/m3 (with the range of 28.77–149.00 μg/m3). Variation of ambient PM10 was observed throughout the study in different years. Hourly values for PM10 measurements during two heating seasons are also presented. Metal concentrations in PM10 were analyzed by electrothermal atomic absorption spectrometry (ETAAS). Quantities of atmospheric mass concentrations of studied trace metals were observed in the following order: Pb > Ni > Cd. The mean concentrations of metals varied with Pb showing the highest concentration (ranging from 1.38 to 234.00 ng/m3), Ni ranging from 0.87 to 42.43 ng/m3, and Cd showing the lowest concentration ranging from 0.26 to 10.09 ng/m3. The concentration of Pb and Cd in PM10 was strongly correlated, suggesting a common source or dependence of these metals in PM10 in Sarajevo. Bioaccessibility of metals in the synthetic gastric juice was also estimated. The quantities of average bioaccessible metal fractions in PM10 samples showed the following trend: Cd > Pb > Ni. The health risk assessment shows that the population of Sarajevo is at increased lifetime risk of experiencing cancer because of exposure to these Cd concentrations in PM10. In addition, parallel PM10 sampling on two samplers showed that obtained results are highly comparable.
Najdeno v: osebi
Ključne besede: air, PM10, heavy metals, Sarajevo
Objavljeno: 09.04.2021; Ogledov: 68; Prenosov: 0
.pdf Polno besedilo (1,30 MB)

Ice cloud formation potential by free tropospheric particles from long-range transport over the Northern Atlantic Ocean
Claudio Mazzoleni, Katja Džepina, Kendra Wright, R. Chris Owen, Paulo Fialho, Lynn R. Mazzoleni, Swarup China, Peter A. Alpert, Bo Zhang, Simeon K. Schum, 2017, izvirni znanstveni članek

Opis: Long-range transported free tropospheric particles can play a significant role on heterogeneous ice nucleation. Using optical and electron microscopy we examine the physicochemical characteristics of ice nucleating particles (INPs). Particles were collected on substrates from the free troposphere at the remote Pico Mountain Observatory in the Azores Islands, after long-range transport and aging over the Atlantic Ocean. We investigate four specific events to study the ice formation potential by the collected particles with different ages and transport patterns. We use single-particle analysis, as well as bulk analysis to characterize particle populations. Both analyses show substantial differences in particle composition between samples from the four events; in addition, single-particle microscopy analysis indicates that most particles are coated by organic material. The identified INPs contained mixtures of dust, aged sea salt and soot, and organic material acquired either at the source or during transport. The temperature and relative humidity (RH) at which ice formed, varied only by 5% between samples, despite differences in particle composition, sources, and transport patterns. We hypothesize that this small variation in the onset RH may be due to the coating material on the particles. This study underscores and motivates the need to further investigate how long-range transported and atmospherically aged free tropospheric particles impact ice cloud formation.
Najdeno v: osebi
Ključne besede: atmospheric aerosols, ice nucleating particles, long-range transport, optical microscopy, electron microscopy, Pico Mountain Observatory
Objavljeno: 11.04.2021; Ogledov: 69; Prenosov: 2
URL Polno besedilo (0,00 KB)
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Morphology and mixing state of aged soot particles at a remote marine free troposphere site
Sumit Kumar, Katja Džepina, Michael P. Dziobak, Paulo Fialho, Judith A. Perlinger, Swarup China, Barbara Scarnato, Robert C. Owen, Bo Zhang, MarianT. Ampadu, 2015, izvirni znanstveni članek

Opis: The radiative properties of soot particles depend on their morphology and mixing state, but their evolution during transport is still elusive. Here we report observations from an electron microscopy analysis of individual particles transported in the free troposphere over long distances to the remote Pico Mountain Observatory in the Azores in the North Atlantic. Approximately 70% of the soot particles were highly compact and of those 26% were thinly coated. Discrete dipole approximation simulations indicate that this compaction results in an increase in soot single scattering albedo by a factor of <= 2.17. The top of the atmosphere direct radiative forcing is typically smaller for highly compact than mass-equivalent lacy soot. The forcing estimated using Mie theory is within 12% of the forcing estimated using the discrete dipole approximation for a high surface albedo, implying that Mie calculations may provide a reasonable approximation for compact soot above remote marine clouds.
Najdeno v: osebi
Ključne besede: atmospheric aerosol, soot, long-range transport, free troposphere, single scattering albedo
Objavljeno: 11.04.2021; Ogledov: 82; Prenosov: 0
.pdf Polno besedilo (899,35 KB)

Long-term ozone data analysis
Vjera Butković, Tomislav Cvitaš, Katja Džepina, Nenad Kezele, Leo Klasinc, 2002, izvirni znanstveni članek

Opis: Various approaches to the analysis of 10-year continuous ozone monitoring from the EUROTRAC-TOR network station Puntijarka near Zagreb are reported. The site has a rural character (45.90degrees N; 15.97degrees E, 980 m a.s.l.) and is representative of the lower troposphere of a wider region. Mean hourly ozone volume fractions measured from 1990-1999, autocorrelation plots for all data and for data for summer periods (May-Sep.), box and whiskers representations of diurnal variations during winter (Nov.-March) and summer periods, mean monthly values and 12-month moving averages, and the Fourier transform of the complete set of 94,248 hourly mean ozone volume fractions are discussed. The data show no increase, or possibly a slight decrease, of the ozone volume fraction toward the end of the decade.
Najdeno v: osebi
Ključne besede: long term ozone data, fourier analysis, ozone trend analysis, Puntijarka field station
Objavljeno: 12.04.2021; Ogledov: 86; Prenosov: 0
.pdf Polno besedilo (123,82 KB)

Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory
J. Hueber, Sumit Kumar, J. A. Perlinger, Katja Džepina, Claudio Mazzoleni, Paulo Fialho, Swarup China, Bo Zhang, R. Chris Owen, D. Helmig, 2015, izvirni znanstveni članek

Opis: Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ∼ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 µg m−3 . On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51 %), followed by sulfate (23 ± 28 %), nitrate (13 ± 10 %), chloride (2 ± 3 %), and elemental carbon (2 ± 2 %). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O /C ratio of ∼ 0.45, which is relatively low compared to O /C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.
Najdeno v: osebi
Ključne besede: organic aerosol, ultrahigh-resolution FT-ICR MS, electron microscopy, remote marine atmosphere, Pico Mountain Observatory
Objavljeno: 11.04.2021; Ogledov: 47; Prenosov: 0
.pdf Polno besedilo (4,36 MB)

Atmospheric peroxyacetyl nitrate (PAN)
H. B. Singh, A. Roiger, Katja Džepina, D. B. Millet, Jiandong Mao, F. Paulot, R. M. Yantosca, M. P. Sulprizio, E. V. Fischer, D. J. Jacob, 2014, izvirni znanstveni članek

Opis: Peroxyacetyl nitrate (PAN) formed in the atmospheric oxidation of non-methane volatile organic compounds (NMVOCs) is the principal tropospheric reservoir for nitrogen oxide radicals (NOx = NO + NO2). PAN enables the transport and release of NOx to the remote troposphere with major implications for the global distributions of ozone and OH, the main tropospheric oxidants. Simulation of PAN is a challenge for global models because of the dependence of PAN on vertical transport as well as complex and uncertain NMVOC sources and chemistry. Here we use an improved representation of NMVOCs in a global 3-D chemical transport model (GEOS-Chem) and show that it can simulate PAN observations from aircraft campaigns worldwide. The immediate carbonyl precursors for PAN formation include acetaldehyde (44 % of the global source), methylglyoxal (30 %), acetone (7 %), and a suite of other isoprene and terpene oxidation products (19 %). A diversity of NMVOC emissions is responsible for PAN formation globally including isoprene (37 %) and alkanes (14 %). Anthropogenic sources are dominant in the extratropical Northern Hemisphere outside the growing season. Open fires appear to play little role except at high northern latitudes in spring, although results are very sensitive to plume chemistry and plume rise. Lightning NOx is the dominant contributor to the observed PAN maximum in the free troposphere over the South Atlantic.
Najdeno v: osebi
Ključne besede: peroxyacetyl nitrate, non-methane volatile organic compounds, global 3-D chemical transport model, GEOS-chem
Objavljeno: 11.04.2021; Ogledov: 53; Prenosov: 0
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