Conceptual Model for the Adsorption of Organic Compounds from the Gas Phase to Liquid and Solid Surfaces

1997 ◽  
Vol 31 (12) ◽  
pp. 3600-3605 ◽  
Author(s):  
Kai-Uwe Goss
Keyword(s):  
Conceptual Model ◽  
Gas Phase ◽  
Organic Compounds ◽  
Solid Surfaces

The rate of photocatalytic oxidation of aromatic volatile organic compounds in the gas-phase

2008 ◽  
Vol 42 (34) ◽  
pp. 7844-7850 ◽  
Author(s):  
Aikaterini K. Boulamanti ◽  
Christos A. Korologos ◽  
Constantine J. Philippopoulos
Keyword(s):  
Volatile Organic Compounds ◽  
Gas Phase ◽  
Organic Compounds ◽  
Photocatalytic Oxidation ◽  
Volatile Organic

scholarly journals Pseudo steady states of HONO measured in the nocturnal marine boundary layer: a conceptual model for HONO formation on aqueous surfaces

2011 ◽  
Vol 11 (7) ◽  
pp. 3243-3261 ◽  
Author(s):  
P. Wojtal ◽  
J. D. Halla ◽  
R. McLaren
Keyword(s):  
Conceptual Model ◽  
Gas Phase ◽  
Formation Mechanism ◽  
Marine Boundary Layer ◽  
Steady States ◽  
Optical Absorption Spectroscopy ◽  
Aqueous Environment ◽  
Ambient Atmosphere ◽  
Mass Source ◽  
Aqueous Surfaces

Abstract. A complete understanding of the formation mechanism of nitrous acid (HONO) in the ambient atmosphere is complicated by a lack of understanding of processes occurring when aqueous water is present. We report nocturnal measurements of HONO, SO2 and NO2 by differential optical absorption spectroscopy over the ocean surface in a polluted marine environment. In this aqueous environment, we observed reproducible pseudo steady states (PSS) of HONO every night, that are fully formed shortly after sunset, much faster than seen in urban environments. During the PSS period, HONO is constant with time, independent of air mass source and independent of the concentration of NO2. The independence of HONO on the concentration of NO2 implies a 0° order formation process, likely on a saturated surface, with reversible partitioning of HONO to the gas phase, through vaporization and deposition to the surface. We observed median HONO/NO2 ratios starting at 0.13 at the beginning of the PSS period (with an apparent lower bound of 0.03), rising to median levels of ~0.30 at the end of the PSS period (with an upper bound >1.0). The implication of these numbers is that they suggest a common surface mechanism of HONO formation on terrestrial and aqueous surfaces, with an increase in the HONO/NO2 ratio with the amount of water available at the surface. The levels of HONO during the nocturnal PSS period are positively correlated with temperature, consistent with a partitioning of HONO from the surface to the gas phase with an apparent enthalpy of vaporization of ΔHSNL (HONO)=55.5±5.4 kJ mol−1. The formation mechanism on aqueous surfaces is independent of relative humidity (RH), despite observation of a negative HONO-RH correlation. A conceptual model for HONO formation on ambient aqueous surfaces is presented, with the main elements being the presence of a surface nanolayer (SNL), highly acidic and saturated with N(IV) precursors, production of HNO3, that diffuses to underlying water layers, and HONO, which partitions reversibly between the SNL and the gas phase. Implications of the conceptual model are discussed.

scholarly journals Condensational uptake of semivolatile organic compounds in gasoline engine exhaust onto pre-existing inorganic particles

2011 ◽  
Vol 11 (1) ◽  
pp. 3461-3492
Author(s):  
S.-M. Li ◽  
J. Liggio ◽  
L. Graham ◽  
G. Lu ◽  
J. Brook ◽  
...  
Keyword(s):  
Air Quality ◽  
Gas Phase ◽  
Organic Compounds ◽  
Gasoline Engine ◽  
Particle Mass ◽  
Seed Particle ◽  
Dilution Ratio ◽  
Ambient Conditions ◽  
Engine Exhaust ◽  
Inorganic Particles

Abstract. This paper presents the results of laboratory studies on the condensational uptake of gaseous organic compounds in the exhaust of a light-duty gasoline engine onto preexisting sulfate and nitrate seed particles. Significant condensation of the gaseous organic compounds in the exhaust occurs onto pre-existing inorganic particles on a time scale of 2–5 min. The amount of condensed organic mass (COM) is proportional to the seed particle mass, suggesting that the uptake is due to dissolution, not adsorption. The solubility decreases as a power function with increased dilution of the exhaust, ranging from 0.23 g/g at a dilution ratio of 81, to 0.025 g/g at a dilution ratio of 2230. The solubility increases nonlinearly with increasing concentration of the total hydrocarbons in the gas phase (THC), rising from 0.12 g/g to 0.26 g/g for a CTHC increase of 1 to 18 μg m−3, suggesting that more organics are partitioned into the particles at higher gas phase concentrations. In terms of gas-particle partitioning, the condensational uptake of THC gases in gasoline engine exhaust can account for up to 30% of the total gas+particle THC. By incorporating the present findings, regional air quality modelling results suggest that the condensational uptake of THC onto sulfate particles alone can be comparable to the primary particle mass under moderately polluted ambient conditions. These findings are important for modelling and regulating the air quality impacts of gasoline vehicular emissions.

scholarly journals Emissions of organic carbon and methane from petroleum and dairy operations in California's San Joaquin Valley

2013 ◽  
Vol 13 (10) ◽  
pp. 28225-28278 ◽  
Author(s):  
D. R. Gentner ◽  
T. B. Ford ◽  
A. Guha ◽  
K. Boulanger ◽  
J. Brioude ◽  
...  
Keyword(s):  
Spatial Distribution ◽  
Organic Carbon ◽  
Gas Phase ◽  
Organic Compounds ◽  
Methane Emissions ◽  
San Joaquin Valley ◽  
Motor Vehicles ◽  
Meteorological Model ◽  
Wide Range ◽  
Petroleum Extraction

Abstract. Petroleum and dairy operations are prominent sources of gas-phase organic compounds in California's San Joaquin Valley. Ground site measurements in Bakersfield and aircraft measurements of reactive gas-phase organic compounds were made in this region as part of the CalNex (California Research at the Nexus of Air Quality and Climate Change) project to determine the sources contributing to regional gas-phase organic carbon emissions. Using a combination of near-source and downwind data, we assess the composition and magnitude of emissions from these prominent sources that are relatively understudied compared to motor vehicles We also developed a statistical modeling method with the FLEXPART-WRF transport and meteorological model using ground-based data to assess the spatial distribution of emissions in the San Joaquin Valley. We present evidence for large sources of paraffinic hydrocarbons from petroleum extraction/processing operations and oxygenated compounds from dairy (and other cattle) operations. In addition to the small straight-chain alkanes typically associated with petroleum operations, we observed a wide range of branched and cyclic alkanes that have limited previous in situ measurements or characterization in emissions from petroleum operations. Observed dairy emissions were dominated by ethanol, methanol, and acetic acid, and methane. Dairy operations were responsible for the vast majority of methane emissions in the San Joaquin Valley; observations of methane were well-correlated with non-vehicular ethanol, and multiple assessments of the spatial distribution of emissions in the San Joaquin Valley highlight the dominance of dairy operations for methane emissions. The good agreement of the observed petroleum operations source profile with the measured composition of non-methane hydrocarbons in unrefined natural gas associated with crude oil suggests a fugitive emissions pathway during petroleum extraction, storage, or processing with negligible coincident methane emissions Aircraft observations of emission hotspots from operations at oil wells and dairies are consistent with the statistical source footprint determined via transport modeling and ground-based data. At Bakersfield, petroleum and dairy operations each comprised 22–23% of anthropogenic non-methane organic carbon and were each responsible for ~12% of potential precursors to ozone, but their direct impacts as potential SOA precursors were estimated to be minor. A comparison with the California Air Resources Board emission inventory supports the current relative emission rates of reactive organic gases from these sources in the region.

scholarly journals Characterization of secondary organic aerosol from heated-cooking-oil emissions: evolution in composition and volatility

2021 ◽  
Vol 21 (6) ◽  
pp. 5137-5149 ◽  
Author(s):  
Manpreet Takhar ◽  
Yunchun Li ◽  
Arthur W. H. Chan
Keyword(s):  
Gas Phase ◽  
Organic Compounds ◽  
Secondary Organic Aerosol ◽  
Carbon Number ◽  
Complex Mixture ◽  
Organic Aerosol ◽  
Oxidation Products ◽  
Atmospheric Evolution ◽  
Oxidative Aging ◽  
Cooking Oil

Abstract. Cooking emissions account for a major fraction of urban organic aerosol. It is therefore important to understand the atmospheric evolution in the physical and chemical properties of organic compounds emitted from cooking activities. In this work, we investigate the formation of secondary organic aerosol (SOA) from oxidation of gas-phase organic compounds from heated cooking oil. The chemical composition of cooking SOA is analyzed using thermal desorption–gas chromatography–mass spectrometry (TD–GC–MS). While the particle-phase composition of SOA is a highly complex mixture, we adopt a new method to achieve molecular speciation of the SOA. All the GC-elutable material is classified by the constituent functional groups, allowing us to provide a molecular description of its chemical evolution upon oxidative aging. Our results demonstrate an increase in average oxidation state (from −0.6 to −0.24) and decrease in average carbon number (from 5.2 to 4.9) with increasing photochemical aging of cooking oil, suggesting that fragmentation reactions are key processes in the oxidative aging of cooking emissions within 2 d equivalent of ambient oxidant exposure. Moreover, we estimate that aldehyde precursors from cooking emissions account for a majority of the SOA formation and oxidation products. Overall, our results provide insights into the atmospheric evolution of cooking SOA, a majority of which is derived from gas-phase oxidation of aldehydes.

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