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Secondary organic aerosol formation from semi- and intermediate-volatility organic compounds and glyoxal
Jose L. Jimenez, Sasha Madronich, Rainer Volkamer, Eleanor M. Waxman, Katja Džepina, Barbara Ervens, Julia Lee-Taylor, Bernard Aumont, 2013, izvirni znanstveni članek

Opis: The role of aqueous multiphase chemistry in the formation of secondary organic aerosol (SOA) remains difficult to quantify. We investigate it here by testing the rapid formation of moderate oxygen-to-carbon (O/C) SOA during a case study in Mexico City. A novel laboratory-based glyoxal-SOA mechanism is applied to the field data, and explains why less gas-phase glyoxal mass is observed than predicted. Furthermore, we compare an explicit gas-phase chemical mechanism for SOA formation from semi- and intermediate-volatility organic compounds (S/IVOCs) with empirical parameterizations of S/IVOC aging. The mechanism representing our current understanding of chemical kinetics of S/IVOC oxidation combined with traditional SOA sources and mixing of background SOA underestimates the observed O/C by a factor of two at noon. Inclusion of glyoxal-SOA with O/C of 1.5 brings O/C predictions within measurement uncertainty, suggesting that field observations can be reconciled on reasonable time scales using laboratory-based empirical relationships for aqueous chemistry.
Najdeno v: osebi
Ključne besede: secondary organic aerosol, glyoxal, aqueous multiphase chemistry, oxygen-to-carbon ratio, single scattering albedo
Objavljeno: 11.04.2021; Ogledov: 182; Prenosov: 0
.pdf Polno besedilo (724,40 KB)

Secondary organic aerosol formation from anthropogenic air pollution
Rainer Volkamer, Jose L. Jimenez, F. M. San Martini, Katja Džepina, Q. Zhang, Dara Salcedo, Luisa T. Molina, D. Worsnop, 2006, izvirni znanstveni članek

Opis: The atmospheric chemistry of volatile organic compounds (VOCs) in urban areas results in the formation of 'photochemical smog', including secondary organic aerosol (SOA). State-of-the-art SOA models parameterize the results of simulation chamber experiments that bracket the conditions found in the polluted urban atmosphere. Here we show that in the real urban atmosphere reactive anthropogenic VOCs (AVOCs) produce much larger amounts of SOA than these models predict, even shortly after sunrise. Contrary to current belief, a significant fraction of the excess SOA is formed from first-generation AVOC oxidation products. Global models deem AVOCs a very minor contributor to SOA compared to biogenic VOCs (BVOCs). If our results are extrapolated to other urban areas, AVOCs could be responsible for additional 3 - 25 Tg yr(-1) SOA production globally, and cause up to - 0.1 W m(-2) additional top-of-the-atmosphere radiative cooling.
Najdeno v: osebi
Ključne besede: atmospheric aerosol, atmospheric chemistry, volatile organic compounds, secondary organic aerosols
Objavljeno: 12.04.2021; Ogledov: 183; Prenosov: 0
.pdf Polno besedilo (638,71 KB)

Modeling the multiday evolution and aging of secondary organic aerosol during MILAGRO 2006
Jose L. Jimenez, Peter F. DeCarlo, Rahul A. Zaveri, Katja Džepina, Christopher D. Cappa, Rainer Volkamer, Sasha Madronich, 2011, izvirni znanstveni članek

Opis: In this study, we apply several recently proposed models to the evolution of secondary organic aerosols (SOA) and organic gases advected from downtown Mexico City at: an altitude of similar to 3.5 km during three days of aging, in a way that is directly comparable to simulations in regional and global models. We constrain the model with and compare its results to available observations. The model SOA formed from oxidation of volatile organic compounds (V-SOA) when using a non-aging SOA parameterization cannot explain the observed SOA concentrations in aged pollution, despite the increasing importance of the low-NO, channel. However, when using an aging SOA parameterization, V-SOA alone is similar to the regional aircraft observations, highlighting the wide diversity in current V-SOA formulations. When the SOA formed from oxidation of semivolatile and intermediate volatility organic vapors (SI-SOA) is computed following Robinson et al. (2007) the model matches the observed SOA mass, but its 0/C is similar to 2 x too low. With the parameterization of Grieshop et al. (2009), the total SOA mass is similar to 2 x too high, but 0/C and volatility are closer to the observations. Heating or dilution cause the evaporation of a substantial fraction of the model SOA; this fraction is reduced by aging although differently for heating vs dilution. Lifting of the airmass to the free-troposphere during dry convection substantially increases SOA by condensation of semivolatile vapors; this effect is reduced by aging.
Najdeno v: osebi
Ključne besede: Mexico-city, volatility, semivolatile, transport, campaign
Objavljeno: 11.04.2021; Ogledov: 166; Prenosov: 0
.pdf Polno besedilo (3,95 MB)

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
Povzetek najdenega: ...SOA formation in Mexico City described by Volkamer et al. (2006), during a photochemically active...
Ključne besede: polycyclic aromatic-hydrocarbons, positive matrix factorization, mass-spectrometry, volatility measurements
Objavljeno: 11.04.2021; Ogledov: 192; Prenosov: 0
.pdf Polno besedilo (1,18 MB)

Implementation of a Markov Chain Monte Carlo method to inorganic aerosol modeling of observations from the MCMA-2003 campaign
F. M. San Martini, E. J. Dunlea, R. M. Volkamer, T. B. Onasch, J. Jayne, M. R. Canagaratna, D. Worsnop, C. E. Kolb, J. H. Shorter, Katja Džepina, 2006, izvirni znanstveni članek

Opis: A Markov Chain Monte Carlo model for integrating the observations of inorganic species with a thermodynamic equilibrium model was presented in Part I of this series. Using observations taken at three ground sites, i. e. a residential, industrial and rural site, during the MCMA-2003 campaign in Mexico City, the model is used to analyze the inorganic particle and ammonia data and to predict gas phase concentrations of nitric and hydrochloric acid. In general, the model is able to accurately predict the observed inorganic particle concentrations at all three sites. The agreement between the predicted and observed gas phase ammonia concentration is excellent. The NOz concentration calculated from the NOy, NO and NO2 observations is of limited use in constraining the gas phase nitric acid concentration given the large uncertainties in this measure of nitric acid and additional reactive nitrogen species. Focusing on the acidic period of 9-11 April identified by Salcedo et al. ( 2006), the model accurately predicts the particle phase observations during this period with the exception of the nitrate predictions after 10: 00 a. m. ( Central Daylight Time, CDT) on 9 April, where the model underpredicts the observations by, on average, 20%. This period had a low planetary boundary layer, very high particle concentrations, and higher than expected nitrogen dioxide concentrations. For periods when the particle chloride observations are consistently above the detection limit, the model is able to both accurately predict the particle chloride mass concentrations and provide well-constrained HCl ( g) concentrations. The availability of gas-phase ammonia observations helps constrain the predicted HCl ( g) concentrations. When the particles are aqueous, the most likely concentrations of HCl ( g) are in the sub-ppbv range. The most likely predicted concentration of HCl ( g) was found to reach concentrations of order 10 ppbv if the particles are dry. Finally, the atmospheric relevance of HCl ( g) is discussed in terms of its indicator properties for the possible influence of chlorine-mediated photochemistry in Mexico City.
Najdeno v: osebi
Ključne besede: secondary organic aerosols, Mexico City, MCMA-2003 field campaign, thermodynamic equilibrium
Objavljeno: 11.04.2021; Ogledov: 190; Prenosov: 0
.pdf Polno besedilo (1,37 MB)

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