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A European aerosol phenomenology - 7 : high-time resolution chemical characteristics of submicron particulate matter across Europe
M. Bressi, F. Cavalli, Jean-Philippe Putaud, R. Fröhlich, J. -E. Petit, W. Aas, M. Äijälä, A. Alastuey, J. D. Allan, M. Aurela, Iasonas Stavroulas, Marta Via, 2021, izvirni znanstveni članek

Opis: Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62°N and 10° W – 26°E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36–64%) of NR-PM1 followed by sulfate (12–44%) and nitrate (6–35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in mid-latitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (μg/m³) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 μg/m³ at half of the sites.
Ključne besede: aerosol, chemical composition, mass spectrometry, phenomenology
Objavljeno v RUNG: 10.05.2024; Ogledov: 261; Prenosov: 2
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Molekularna karakterizacija lebdećih čestica slobodne troposfere sa Opservatorija Pico planine
Katja Džepina, Claudio Mazzoleni, Paulo Fialho, Swarup China, B. Zhang, R. Chris Owen, D. Helmig, J. Hueber, Sumit Kumar, J. A. Perlinger, 2017, objavljeni povzetek znanstvenega prispevka na konferenci

Opis: Long-range transported free tropospheric aerosol was sampled at the PMO (38°28’15’’N, 28°24’14’’W; 2225 m amsl) on Pico Island of the Azores in the North Atlantic. Filter-collected aerosol during summer 2012 was analysed for organic and elemental carbon, and inorganic ions. The average aerosol ambient concentration was 0.9 µg m-3. Organic aerosol contributed the majority of mass (57%), followed by sulphate (21%) and nitrate (17%). Filter-collected aerosol was positively correlated with on-line aerosol measurements of black carbon, light scattering and number concentration. Water-soluble organic compounds (WSOC) from 9/24 and 9/25 samples collected during a pollution event were analysed with ultrahigh-resolution FT-ICR MS. FLEXPART analysis showed the air masses were very aged (>12 days). ~4000 molecular formulas were assigned to each of the mass spectra between m/z 100-1000. The majority of the assigned molecular formulas have unsaturated structures with CHO and CHNO elemental compositions. WSOC have an average O/C of ~0.45, relatively low compared to O/C of other aged aerosol, which might be the result of evaporation and fragmentation during long-range transport. The increase in aerosol loading during 9/24 was linked to biomass burning emissions from North America by FLEXPART and MODIS fire counts. This was confirmed with WSOC biomass burning markers and with the morphology and mixing state of particles as determined by SEM. The presence of markers characteristic of aqueous-phase reactions of biomass burning phenolic species suggests that the aerosol collected at Pico had undergone cloud processing. The air masses on 9/25 were more aged (~15 days) and influenced by marine emissions, as indicated by organosulphates and species characteristic for marine aerosol (e.g. fatty acids). The change in air masses for the two samples was corroborated by the changes in ozone, ethane, propane, morphology of particles, as well as by FLEXPART. In this presentation we will presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at the PMO.
Ključne besede: Atmospheric aerosol, Free troposphere, Mass spectrometry, Pico mountain observatory
Objavljeno v RUNG: 26.05.2021; Ogledov: 2903; Prenosov: 0
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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.
Ključne besede: polycyclic aromatic-hydrocarbons, positive matrix factorization, mass-spectrometry, volatility measurements
Objavljeno v RUNG: 11.04.2021; Ogledov: 2236; Prenosov: 0
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Uranium bearing dissolved organic matter in the porewaters of uranium contaminated lake sediments
Breda Novotnik, Wei Chen, R. Douglas Evans, 2018, izvirni znanstveni članek

Opis: Uranium (U) mobility in the environment strongly depends on its oxidation state and the presence of complexing agents such as inorganic carbon, phosphates, and dissolved organic matter (DOM). Despite the importance of DOM in U mobility, the exact mechanism is still poorly understood. Therefore, the aim of our investigation was to characterise sediment porewater DOM in two lakes in Ontario, Canada (Bow and Bentley Lakes) that were historically contaminated with U and propose possible composition of UO2-bearing DOM. Depth profiles of U concentrations in porewaters and total sediment digests reveal U levels of up to 1.3 mg L−1 in porewater and up to 0.8 mg−1 g in sediment. Depth profiles of U did not correlate with Fe, Mn, SO4 2−, or Eh profiles. Therefore, porewater DOM was analysed and taken into consideration as the primary source of U mobility. Porewater DOM in each sediment section (1 cm sections, 20 cm core length) was analysed by high-resolution electrospray ionisation mass spectrometry. PCA analyses of porewater DOM mass spectra showed grouping and clear separation of DOM in sediment sections with elevated U concentrations in comparison to sections with background U concentrations. Several criteria were set to characterise UO2-bearing DOM and more than 70 different molecules were found. The vast majority of these UO2-DOM compounds fell in the category of carboxyl-containing aliphatic molecules (H/C between 0.85 and 1.2 and O/C≤0.4) and had a mean value of m/z about 720.
Ključne besede: Uranium Lake sediments Porewater Disolved organic matter High resolution mass spectrometry
Objavljeno v RUNG: 09.10.2019; Ogledov: 3403; Prenosov: 0
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Capturing and Storing Exhaled Breath for Offline Analysis
Iain R. White, Stephen J. Fowler, 2019, samostojni znanstveni sestavek ali poglavje v monografski publikaciji

Opis: In this chapter we will summarize and discuss methods for the capture and storage of exhaled breath, prior to offline (and indirect online) analysis. We will detail and compare methods currently in use, including their applications, key strengths, and limitations. In synthesizing the best features of each technique, we will propose an ideal standardized breath sampling solution, and give a personal vision on the next steps to be taken in this exciting area of breath research.
Ključne besede: Breath analysis, Breath sampling, Offline analysis, Thermal desorption, Gas chromatography-mass spectrometry
Objavljeno v RUNG: 22.07.2019; Ogledov: 3561; Prenosov: 0
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Hypoxia influences the cellular cross-talk of human dermal fibroblasts. A proteomic approach.
Boraldi Federica, Annovi Giulia, Carraro Fabio, Naldini Antonella, Tiozzo Roberta, Sommer Pascal, Quaglino Daniela, 2007, izvirni znanstveni članek

Opis: The ability of cells to respond to changes in oxygen availability is critical for many physiological and pathological processes (i.e. development, aging, wound healing, hypertension, cancer). Changes in the protein profile of normal human dermal fibroblasts were investigated in vitro after 96 h in 5% CO2 and 21% O2 (pO2=140 mm Hg) or 2% O2 (pO2=14 mm Hg), these parameters representing a mild chronic hypoxic exposure which fibroblasts may undergo in vivo. The proliferation rate and the protein content were not significantly modified by hypoxia, whereas proteome analysis demonstrated changes in the expression of 56 proteins. Protein identification was performed by mass spectrometry. Data demonstrate that human fibroblasts respond to mild hypoxia increasing the expression of hypoxia inducible factor (HIF1a) and of the 150-kDa oxygen-regulated protein. Other differentially expressed proteins appeared to be related to stress response, transcriptional control, metabolism, cytoskeleton, matrix remodelling and angiogenesis. Furthermore, some of them, like galectin 1, 40S ribosomal protein SA, N-myc-downstream regulated gene-1 protein, that have been described in the literature as possible cancer markers, significantly changed their expression also in normal hypoxic fibroblasts. Interestingly, a bovine fetuin was also identified that appeared significantly less internalised by hypoxic fibroblasts. In conclusion, results indicate that human dermal fibroblasts respond to an in vitro mild chronic hypoxic exposure by modifying a number of multifunctional proteins. Furthermore, data highlight the importance of stromal cells in modulating the intercellular cross-talk occurring in physiological and in pathologic conditions.
Ključne besede: Human fibroblast, Primary cell culture, Hypoxia, Connective tissue, Proteome, 2D gel electrophoresis, Mass-spectrometry
Objavljeno v RUNG: 22.07.2019; Ogledov: 3597; Prenosov: 0
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Real-time multi-marker measurement of organic compounds in human breath: Towards fingerprinting breath
Iain R. White, Kerry A Willis, Christopher Whyte, Rebecca Cordell, Robert S Blake, Andrew J Wardlaw, 2013, izvirni znanstveni članek

Opis: The prospects for exploiting proton transfer reaction-time of flight-mass spectrometry (PTR-ToF-MS) in medical diagnostics are illustrated through a series of case studies. Measurements of acetone levels in the breath of 68 healthy people are presented along with a longitudinal study of a single person over a period of 1 month. The median acetone concentration across the population was 484 ppbV with a geometric standard deviation (GSD) of 1.6, whilst the average GSD during the single subject longtitudinal study was 1.5. An additional case study is presented which highlights the potential of PTR-ToF-MS in pharmacokinetic studies, based upon the analysis of online breath samples of a person following the consumption of ethanol. PTR-ToF-MS comes into its own when information across a wide mass range is required, particularly when such information must be gathered in a short time during a breathing cycle. To illustrate this property, multicomponent breath analysis in a small study of cystic fibrosis patients is detailed, which provides tentative evidence that online PTR-ToF-MS analysis of tidal breath can distinguish between active infection and non-infected patients.
Ključne besede: Volatile Organic Compounds, breath, proton transfer reaction mass spectrometry, Cystic Fibrosis
Objavljeno v RUNG: 22.07.2019; Ogledov: 3509; Prenosov: 0
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Observations of the release of non-methane hydrocarbons from fractured shale
Roberto Sommariva, Robert S Blake, Robert J Cuss, Rebecca L Cordell, Jon F Harrington, Iain R. White, Paul S Monks, 2014, izvirni znanstveni članek

Opis: The organic content of shale has become of commercial interest as a source of hydrocarbons, owing to the development of hydraulic fracturing ("fracking"). While the main focus is on the extraction of methane, shale also contains significant amounts of non-methane hydrocarbons (NMHCs). We describe the first real-time observations of the release of NMHCs from a fractured shale. Samples from the Bowland-Hodder formation (England) were analyzed under different conditions using mass spectrometry, with the objective of understanding the dynamic process of gas release upon fracturing of the shale. A wide range of NMHCs (alkanes, cycloalkanes, aromatics, and bicyclic hydrocarbons) are released at parts per million or parts per billion level with temperature- and humidity-dependent release rates, which can be rationalized in terms of the physicochemical characteristics of different hydrocarbon classes. Our results indicate that higher energy inputs (i.e., temperatures) significantly increase the amount of NMHCs released from shale, while humidity tends to suppress it; additionally, a large fraction of the gas is released within the first hour after the shale has been fractured. These findings suggest that other hydrocarbons of commercial interest may be extracted from shale and open the possibility to optimize the "fracking" process, improving gas yields and reducing environmental impacts.
Ključne besede: Environmental impact, Hydraulic fracturing, Mass spectrometry
Objavljeno v RUNG: 18.07.2019; Ogledov: 3121; Prenosov: 0
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Increased sensitivity in proton transfer reaction mass spectrometry by incorporation of a radio frequency ion funnel
Shane Barber, Robert S Blake, Iain R. White, Paul S Monks, Fraser Reich, Stephen Mullock, Andrew M Ellis, 2012, izvirni znanstveni članek

Opis: A drift tube capable of simultaneously functioning as an ion funnel is demonstrated in proton transfer reaction mass spectrometry (PTR-MS) for the first time. The ion funnel enables a much higher proportion of ions to exit the drift tube and enter the mass spectrometer than would otherwise be the case. An increase in the detection sensitivity for volatile organic compounds of between 1 and 2 orders of magnitude is delivered, as demonstrated using several compounds. Other aspects of analytical performance explored in this study include the effective E/N (ratio of electric field to number density of the gas) and dynamic range over which the drift tube is operated. The dual-purpose drift tube/ion funnel can be coupled to various types of mass spectrometers to increase the detection sensitivity and may therefore offer considerable benefits in PTR-MS work.
Ključne besede: Analytical performance, Detection sensitivity, Drift tube, Dynamic range, Ion funnels, Proton-transfer reaction mass spectrometry, Volatile organic compounds
Objavljeno v RUNG: 18.07.2019; Ogledov: 3104; Prenosov: 0
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