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PubMed2002

Carbon isotopic composition of fatty acids in the marine aerosols from the western North Pacific: implication for the source and atmospheric transport.

A combined molecular and isotopic approach was used in this study to reveal the source and transport of aerosols at a remote oceanic site. Fatty acid distributions and stable carbon isotopic compositions of individual fatty acids were determined in the aerosol samples collected at Chichi-Jima in the western North Pacific over a period of 41 months. Fatty acid concentration and isotopic composition delta13C (vs PDB) exhibited temporal variations. Concentrations of fatty acids (C12-C34) ranged from 7.6 to 20.7 ng/m3. The concentrations of lower molecular weight (LMW) fatty acids (C12 -C19) tend to decrease in winter and increase in summer, whereas the higher molecular weight (HMW) C20-34 fatty acids exhibited a reversed trend. Compound-specific isotopic analysis revealed that the LMW fatty acids exhibited consistently less negative delta13C values than the HMW fatty acids. However, both the LMW and HMW fatty acids displayed a similar trend of temporal variations in delta13C, suggesting thatthe fatty acids experienced similar atmospheric pathways and transport processes to the remote marine atmosphere, whereas the difference in absolute delta13C reflects the different sources of the fatty acids.

Aerosols↗

PubMed2004

Redox speciation of copper in rainwater: temporal variability and atmospheric deposition.

Copper speciation was determined in 68 rainwater samples collected in Wilmington, NC, from August 25, 2000, to September 24, 2002. Volume-weighted average concentrations of Cu(total), dissolved Cu(II), and dissolved Cu(I) were 5.3, 3.2, and 1.4 nM, respectively, with a significantly higher ratio of Cu(II)/Cu(I) in summer relative to winter events. The concentrations of all Cu species were higher in storms of continental origin relative to marine-dominated events, suggesting anthropogenic and/or terrestrial sources are important contributors of Cu in precipitation. Concentrations of strong Cu-complexing ligands were consistently lower than dissolved Cu concentrations, indicating a significant portion, but not all, of the dissolved Cu in rainwater is strongly complexed. A portion of these ligands, in addition to the sulfite and chloride in precipitation, may be Cu(I)-complexing ligands, which may explain the resistance of Cu(I) against oxidation in rainwater. Using our rainwater concentration data along with other published rainwater Cu concentrations and an estimate for total global annual rain, the total global flux of Cu removed from the atmosphere via wet deposition is 150 x 106 kg yr(-1). This represents complete removal of the estimated Cu input into the troposphere and indicates essentially all Cu released into the global atmosphere is removed by rain.

Air Pollutants↗

PubMed2003

Hygroscopic properties of two model humic-like substances and their mixtures with inorganics of atmospheric importance.

Water-soluble macromolecular polyacids can play a potentially important role in the hygroscopic properties of atmospheric aerosols. These acids have molecular structures similar to natural fulvic acids (FA) (or humic acids) and are referred to as humic-like substances (HULIS). In this study, the hygroscopicity of HULIS and the mixture of HULIS and sodium chloride (NaCl) and that of HULIS and ammonium sulfate (AS) aerosols at a mass ratio of 1:1 are studied using two natural FA: the Nordic Aquatic Fulvic Acid (NAFA) and the Suwannee River Fulvic Acid (SRFA) as model compounds in an electrodynamic balance. NAFA and SRFA both absorbed and desorbed water reversibly without crystallization and retained water at a relative humidity (RH) < 10%. NAFA and SRFA have a mass growth ratio of 1.25 and 1.45 from RH = 10% to RH = 90%, respectively. However, these results are different from those of another natural FA (the Nordic River Fulvic Acid Reference) in the literature. The differences are possibly due to the differences in the chemical composition of the natural FA, which depends on their sources and the isolation methods. These results suggest that a standardization of the isolation methods of HULIS is needed for better understanding of their atmospheric properties and environmental impacts. In general, the deliquescence and crystallization RH of FA-inorganic mixtures are comparable with those of their respective pure inorganic species. Since FA are less hygroscopic than NaCl and AS, all mixtures absorb less water compared to their respective pure inorganic species of equal particle mass. The FA-AS mixtures have a larger water uptake than the sum of those of the FA and AS individually following a simple additivity rule as noninteracting species at RH = 90%. This enhancement effect increases as the RH decreases. There is no such enhancement effect for the FA-NaCl mixtures until RH is below 90%. These results reveal that the effect of the interactions between FA and inorganic species on the water uptake of the mixtures, in general, is a function of RH.

Absorption↗

PubMed2004

Chasing quicksilver: modeling the atmospheric lifetime of Hg(0)(g) in the marine boundary layer at various latitudes.

The lifetime of elemental mercury in the marine boundary layer(MBL) has been studied using AMCOTS (Atmospheric Mercury Chemistry Over The Sea), a box model of MBL photochemistry including aerosols and detailed mercury chemistry. Recently measured Hg(0)(g) oxidation reactions have been included, and the studies were performed as a function of latitude, time of year, boundary layer liquid water content (LWC) and cloud optical depth. The results show that Hg has the shortest lifetime when air temperatures are low and sunlight and deliquescent aerosol particles are plentiful. Thus the modeled lifetime for clear-sky conditions is actually shorter at mid-latitudes and high latitudes than near the equator, and for a given latitude and time of year, cooler temperatures enhance the rate of Hg oxidation. Under typical summer conditions (for a given latitude) of temperature and cloudiness, the lifetime (tau) of Hg(0)(g) in the MBL is calculated to be around 10 days at all latitudes between the equator and 60 degrees N. This is much shorter than the generally accepted atmospheric residence time for Hg(0)(g) of a year or more. Given the relatively stable background concentrations of Hg(0)(g) which have been measured, continual replenishment of Hg(0)(g) must take place, suggesting a "multihop" mechanism for the distribution of Hg, rather than solely aeolian transport with little or no chemical transformation between source and receptor. Inclusion of an empirical Hg(0)(g) emission factor related to insolation was used to stabilize the Hg(0)(g) concentration in the model, and the emission rates necessarily agree well with estimated emission fluxes for the open ocean.

Aerosols↗

PubMed2005

Time trends of atmospheric PBDEs inferred from archived U.K. herbage.

Aerial portions of vegetation receive the bulk of their burden of persistent organic pollutants (POPs) from the atmosphere. Vegetation can therefore be a useful indicator of the changing atmospheric burden of POPs. Samples of archived pasture, collected from Rothamsted Experimental Station in the United Kingdom between 1930 and 2004, were analyzed for a range of polybrominated diphenyl ethers (PBDEs). PBDEs could not be routinely detected in the pre-1970 samples. Thereafter, the dominant congeners BDE 28, 47, 49, 99, 100, 153, 154, and 183 were frequently detected. The general trend was (a) a rise through the 1970s; (b) a minipeak in the mid-1980s, strongly influenced by one particularly high sample for 1984; (c) values remaining high through the late 1980s/1990s; (d) an indication of a more recent decline for all congeners (except BDE-28), consistent with recent restrictions on PBDE usage in Europe. These trends were compared to recent modeled estimates of U.K. PBDE emissions. The congener profiles of technical mixtures, U.K. air, soil, and pasture were compared and shown to be broadly similar. The implications for environmental release mechanisms are discussed.

Air Pollutants↗

PubMed2005

Field deployment of thin film passive air samplers for persistent organic pollutants: a study in the urban atmospheric boundary layer.

This paper reports on the first field deployment of rapidly equilibrating thin-film passive air samplers under ambient conditions. The POlymer-coated Glass (POG) samplers have a coating of ethylene vinyl acetate (EVA) less than 1 microm thick applied to a glass surface. This can be dissolved off after exposure and prepared for the quantification of persistent organic pollutants (POPs) that have partitioned into the film during field exposure. In this study, POGs were deployed at various heights on the CN Tower in Toronto, Canada, to investigate the vertical distribution of selected compounds (PCBs, PAHs, organochlorine pesticides) in the atmospheric boundary layer of an urban area. The feasibility of the method to detect POPs from a few cubic meters of air was demonstrated, indicating the potential for rapid, low-volume sampling of air for ambient levels of POPs. PAH levels declined sharply with height, confirming ground-level emissions in urban areas as sources of these compounds; PCBs did the same, although less strongly. Different sampling events detected different vertical distributions of OC pesticides which could be related to local or distantsources, and variations in POPs on the samplers in these different events/heights demonstrate the dynamic nature of sources and atmospheric mixing of POPs.

Air Movements↗

PubMed2004

Atmospheric deposition and fluxes of organochlorine pesticides and coplanar polychlorinated biphenyls in aquatic environments of Hong Kong, China.

Concentrations of organochlorine (OC) pesticides and coplanar (dioxin-like) polychlorinated biphenyls (PCBs) in bulk deposition were measured at the Mai Po Marshes Nature Reserve (MPMNR) and A Chau, which are both important habitats for waterbirds in Hong Kong. OC pesticides exempted from the Stockholm Convention were present in greater concentrations than those that have been restricted for use in the region. Among the OC pesticides, HCB, sigmaDDTs, and sigmaHCHs were detected. Concentrations of HCB were greater at MPMNR than at A Chau, and this finding suggests short-range transport of this compound, which is different from the other OC pesticides. Several environmental factors including seasonal variations in temperature, particulate matter, and rainfall may influence the flux of OC pesticides. Since sources of HCB often coexist with sources of polychlorinated dibenzo-p-dioxins and dibenzofurans (dioxins and furans), the presence of HCB may be a useful surrogate for monitoring airborne dioxins and for understanding their deposition potential. The contribution of atmospheric deposition to the OC pesticide input to the two study sites was small. Concentrations of most OC pesticides in surface waters were greater than would be predicted based on the inputs from atmospheric deposition and sedimentation. The mass balance calculation suggests a net flux of OC pesticides from bottom sediments to the overlying water column.

Air Movements↗

PubMed2005

Temperature dependence of atmospheric PCB concentrations.

An analysis of data from the U.S. Integrated Atmospheric Deposition Network (IADN) sites near the Great Lakes and a review of the literature shows that the temperature dependence of atmospheric PCB concentrations cannot be used to distinguish sites dominated by long-distance transport from those with local sources. We observe that calculations based on data sets with only approximately 25 measurements over a period of 1 year are unreliable indicators of the long-term temperature dependence at a given location, that temperature independence occurs at temperatures below freezing, and that low PCB concentrations can bias analyses toward a weaker temperature dependence. After accounting for these factors, a similar temperature dependence is observed at all IADN sites, and this temperature dependence increases for PCBs with increasing chlorination. Although previously described models do fit the data, the resulting calculated constants are not meaningful. Instead, a simple new model in which temperatures < 273 K are set equal to 273 K, and the Clausius-Clapeyron equation is used, can account for observed temperature dependence phenomena.

Atmosphere↗

PubMed2005

Comparison of atmospheric deposition of copper, nickel, cobalt, zinc, and cadmium recorded by Finnish peat cores with monitoring data and emission records.

This study aims to determine the extent to which the accumulation rates of Cu, Ni, Co, Zn, and Cd in peat cores agree with established histories of atmospheric emission from local pointsources. Metals accumulating in three Finnish peat cores with known metal deposition histories have been measured using inductively coupled plasma-sector field mass spectrometry. Samples were age-dated using both 210Pb and 14C (bomb pulse curve). At the Outokumpu (OUT) site as well as the low-background site Hietajärvi (HIJ), 210Pb age dates are in excellent agreement with the 14C bomb pulse curve method results, and the precision is between 1 and 10 years for most of the samples; at the Harjavalta (HAR) site, precision is > 6 years. Mean regional "background" concentrations have been calculated from deeper peat layers of the HIJ site (microg g(-1)): Cu, 1.3 +/- 0.2 (n = 62); Co, 0.25 +/- 0.04 (n = 71); Cd, 0.08 +/- 0.01 (n = 23); and Zn, 4 +/- 2 (n = 40). For layers accumulated within the past 100 years, accumulation rates (ARs) have been calculated. At sites with < 0.06 g m(-2) cumulative Ni inventory (HIJ and OUT), ARs of Cu and Co trace the known metal deposition histories very well. At HAR, where metal inventories are much greater, Cu and Co are mobile. ARs of Zn were between 3 and 30 mg m(-2) year(-1) and those of Cd between 24 and 140 microg m(-2) year(-1) at all sites and are independent of the chronology of their inputs from the atmosphere.

Air Pollutants↗

PubMed2005

Combustion products of plastics as indicators for refuse burning in the atmosphere.

Despite all of the economic problems and environmental discussions on the dangers and hazards of plastic materials, plastic production worldwide is growing at a rate of about 5% per year. Increasing techniques for recycling polymeric materials have been developed during the last few years; however, a large fraction of plastics are still being discarded in landfills or subjected to intentional or incidental open-fire burning. To identify specific tracer compounds generated during such open-fire combustion, both smoke particles from burning and plastic materials from shopping bags, roadside trash, and landfill garbage were extracted for gas chromatography-mass spectrometry analyses. Samples were collected in Concón, Chile, an area frequently affected by wildfire incidents and garbage burning, and the United States for comparison. Atmospheric samples from various aerosol sampling programs are also presented as supportive data. The major components of plastic extracts were even-carbon-chain n-alkanes (C16-C40), the plasticizer di-2-ethylhexyl phthalate, and the antioxidants and lubricants/antiadhesives Irganox 1076, Irgafos 168, and its oxidation product tris(2,4-di-tertbutylphenyl) phosphate. Major compounds in smoke from burning plastics include the non-source-specific n-alkanes (mainly even predominance), terephthalic acid, phthalates, and 4-hydroxybenzoic acid, with minor amounts of polycyclic aromatic hydrocarbons (including triphenylbenzenes) and tris(2,4-di-tert-butylphenyl)phosphate. 1,3,5-Triphenylbenzene and tris(2,4-di-tert-butylphenyl)- phosphate were found in detectable amounts in atmospheric samples where plastics and refuse were burned in open fires, and thus we propose these two compounds as specific tracers for the open-burning of plastics.

Aerosols↗

PubMed2006

Atmospheric chlorine chemistry in southeast Texas: impacts on ozone formation and control.

Recent evidence has demonstrated that chlorine radical chemistry can enhance tropospheric hydrocarbon oxidation and has the potential to enhance ozone formation in urban atmospheres. To assess these effects quantitatively, an August-September 2000 photochemical episode in southeast Texas was simulated using the comprehensive air quality model, with extensions (CAMx). During this episode, ambient measurements of a unique marker of atmospheric chlorine chemistry, 1-chloro-3-methyl-3butene-2-one (CMBO), were made and model performance was assessed by comparing modeled and observed CMBO mixing ratios. The model predicted ambient CMBO mixing ratios within the uncertainty limits associated with the emissions inventory, so the model was used to assess the impacts of chlorine chemistry on ozone formation. Based on the current emissions inventory, chlorine emissions have the potential to enhance 1-h-averaged ozone mixing ratios by 70 ppb, in very localized areas, during morning hours. Over wider areas, and at times of day when peak ozone concentrations are observed, the impacts of chlorine emissions on ozone concentrations are typically less than 10 ppb. Chlorine emissions also influenced changes in ozone concentrations due to hydrocarbon and NOx emission controls.

Air Pollutants↗

PubMed2005

Simultaneous determination of mono- and dicarboxylic acids, omega-Oxo-carboxylic acids, midchain ketocarboxylic acids, and aldehydes in atmospheric aerosol samples.

This paper describes a method for the simultaneous determination of monocarboxylic acids (C6-C34), dicarboxylic acids (C2-C24), omega-oxo-carboxylic acids (C2-C9), ketocarboxylic acids (pyruvic and pinonic acid), and select aldehydes (glyoxal, methylglyoxal, and nonanal) in atmospheric particles. Quantification of these compounds gives information on important chemical characteristics of aerosols for source apportioning of aerosol organics and for studying atmospheric processes leading to secondary organic aerosol formation. These target analytes were determined as their butyl ester or butyl acetal derivatives using gas-chromatography mass spectrometry. The method is modified from a method described by Kawamura. Kawamura's original method involved a water extraction step, which practically restricted the method to the determination of only those compounds that are water-soluble. Our method eliminates the water extraction step and combines extraction and derivatization of the target compounds in one step. A mixture of hexane/butanol/BF3 simultaneously derivatizes the polar function groups (i.e., -COOH, -C=O) and extracts the target analytes from the aerosol filter substrates. A prominent advantage of our method is improved recoveries for the more volatile analytes in the target compound classes as a result of eliminating the water evaporation step. Recoveries better than 66% were obtained for the target analytes, including the relatively volatile ones. This improvement for the light species has allowed detection of a new midchain ketocarboxylic acid, 4-oxopentanoic acid, which would have escaped detection by the Kawamura method because of its high susceptibility to evaporative loss. Examples are presented to demonstrate the use of this method in analysis of ambient aerosol samples.

Aerosols↗

PubMed2005

Atmospheric size distribution of PAHs: evidence of a high-volume sampling artifact.

The purpose of this study was to characterize atmospheric levels of four- to six-ring polycyclic aromatic hydrocarbons (PAHs) in the vicinity of a horizontal stud Söderberg aluminum smelter in terms of the size distribution of particulate matter (September to December 2002). It was found that the vast majority of the PAHs was associated with particle diameters less than 1 and 3 microm. A profile comparison of the PAH mixture--using benzo[a]pyrene (B[a]P) relative abundance ratios (PAH/B[a]P)--for the cascade impactor filters indicated the formation of a sampling artifact. Overall, the PAH stability scale generated in this study agrees with those produced experimentally for ozone and nitrogen dioxides or developed using other in situ measurement techniques. Correlations of the four- to six-ring PAHs with other atmospheric variables suggested that smelter plume conditions and particle characteristics may play a potentially important role in the overall PAH reactivity. To our knowledge, this is the first study to report a sampling artifact for the four- to six-ring PAHs during in situ high volume sampling under real world conditions.

Air Pollutants↗

PubMed2006

Atmospheric fate of dichlorvos: photolysis and OH-initiated oxidation studies.

The OH-initiated oxidation of dichlorvos (a widely used insecticide) has been investigated under atmospheric conditions at the large outdoor European photoreactor (EUPHORE) in Valencia, Spain. The rate constant of OH reaction with dichlorvos, k, was measured by using a conventional relative rate technique where 1,3,5-trimethylbenzene (TMB) and cyclohexane were taken as references. With the use of the rate constants of 5.67 x 10(-11) and of 6.97 x 10(-12) cm3 molecule(-1) s(-1) for the reactions OH + TMB and OH + cyclohexane, respectively, the resulting value of the OH reaction rate constant with dichlorvos was derived to be k = (2.6 +/- 0.3) x 10(-11) cm3 molecule(-1) s(-1). The tropospheric lifetime of dichlorvos with respect to reaction with OH radical has been estimated to be around 11 h. The major carbon-containing products observed for the OH reaction with dichlorvos in air under sunlight condition were phosgene and carbon monoxide. The formation of a very stable toxic primary product such as phosgene associated with the relatively short lifetime of dichlorvos may make the use of this pesticide even more toxic for humans when released into the atmosphere.

Atmosphere↗

PubMed2001

Browning evaluation of ready-to-eat apples as affected by modified atmosphere packaging.

The color and polyphenol oxidase (PPO) activity of fresh-cut Golden delicious apples were evaluated throughout cold storage under modified atmospheres. The shelf life of cut apples was extended to several weeks, especially when an initial atmosphere of 90.5% N(2) + 7% CO(2) + 2.5% O(2) and plastic pouches of 30 cm(3)/cm(2) x bar x 24 h were used. Under these conditions, a maximum 62% PPO activity depletion was observed. In all cases, the faster the initial PPO activity decays, the less the color changes. A fractional conversion first-order model was proposed for predicting color changes in minimally processed apples. Browning was better described through lightness (L) (k(L) = 0.017 - 0.07 day(-1)) and color difference (Delta E*) values (k(Delta E) = 0.015 - 0.073 day(-1)), which fitted the model with enough accuracy.

Atmosphere↗

PubMed2002

Atmospheric pressure ionization LC-MS-MS determination of urushiol congeners.

This paper describes atmospheric pressure ionization (API) LC-MS-MS determination of urushiols, 3-n-alkenyl- and -alkyl-substituted catechols responsible for poison oak dermatitis. Urushiol was isolated from Western poison oak according to the method of Elsohly et al. (1) (J. Nat. Prod. 1982, 45, 532-538)-the purified preparation contained C(17)- and C(15)-substituted urushiols with zero, one, two, and three double bonds as determined from GC-MS analysis of trimethylsilyl derivatives. Urushiol mixtures were separated on a C(18) reversed phase HPLC column with a methanol-water gradient with urushiols eluting in 100% methanol. Atmospheric pressure chemical ionization (APCI) produced primarily [M - H](-) and MH(+) molecule ions. Electrospray ionization (ESI) yielded [M - H](-) and adduct ions including [M + Cl](-). Daughter ions of [M - H](-) included quinoid radical anions ([M - H - H(2)](-) and m/z 122(-)) and a benzofuran phenate (m/z 135(-)). A suite of hydrocarbon fragments were produced by collision-induced dissociation of MH(+) directly or via an intermediate [MH - H(2)O](+) daughter ion. Six urushiol congeners, one not previously reported in poison oak, were determined by negative ion API-LC-MS-MS with detection limits of approximately 8 pg/microL (ESI) and approximately 800 pg/microL (APCI). API-LC-MS-MS was used to determine urushiol in surface wipes, air samples, and plant materials.

Atmospheric Pressure↗

PubMed1999

Carbohydrate and acid contents of Gala apples and Bartlett pears from regular and controlled atmosphere storage.

Gala apples and Bartlett pears were harvested over two crop seasons at different maturities and growing sources then stored in refrigerated storage alone and in controlled atmosphere storage (1% O(2) plus 1% CO(2) or 2% O(2) plus 3% CO(2)). Before and after storage of 45 or 90 days, the juice from the fruit was examined for carbohydrate and acid compositions and contents. For Gala apples, the type and length of storage had no significant effect on juice carbohydrate and acid contents and compositions, whereas the time of harvest greatly influenced both parameters. Storage atmosphere did not affect the carbohydrate and acid contents and compositions of Bartlett pear juice; however, the source of the fruit and subsequent amount of ripening did appear to significantly cause changes in the same parameters. The carbohydrate and acid compositions and contents of Gala apple juice were within the compositional range for worldwide apple juice. Bartlett pear juice contained significantly greater concentrations of citric acid than shown in previously published studies.

Atmosphere↗

PubMed2006

Exploration of the potential energy surfaces, prediction of atmospheric concentrations, and prediction of vibrational spectra for the HO2...(H2O)n (n = 1-2) hydrogen bonded complexes.

The hydroperoxy radical (HO2) plays a critical role in Earth's atmospheric chemistry as a component of many important reactions. The self-reaction of hydroperoxy radicals in the gas phase is strongly affected by the presence of water vapor. In this work, we explore the potential energy surfaces of hydroperoxy radicals hydrogen bonded to one or two water molecules, and predict atmospheric concentrations and vibrational spectra of these complexes. We predict that when the HO2 concentration is on the order of 10(8) molecules x cm(-3) at 298 K, that the number of HO2...H2O complexes is on the order of 10(7) molecules x cm(-3) and the number of HO2...(H2O)2 complexes is on the order of 10(6) molecules x cm(-3). Using the computed abundance of HO2...H2O, we predict that, at 298 K, the bimolecular rate constant for HO2...H2O + HO2 is about 10 times that for HO2 + HO2.

Atmosphere↗