Journal of Atmospheric Chemistry

Current research reports and chronological list of recent articles.


The international scientific Journal of Atmospheric Chemistry is devoted to the study of the chemistry of the atmosphere, with particular emphasis on the region below about 100 km. The strongly interdisciplinary nature of atmospheric chemistry means that it embraces a great variety of sciences.

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Journal of Atmospheric Chemistry - Abstracts



Identification and quantification of carbonyl-containing α-pinene ozonolysis products using O - tert -butylhydroxylamine hydrochloride

Abstract

The yields of carbonyl-containing reaction products from the ozonolysis of α-pinene have been investigated using concentrations of ozone found in the indoor environment ([O3] ≤ 100 ppb). An impinger was used to collect gas-phase oxidation products in water, where the derivatization agent O-tert-butylhydroxylamine hydrochloride (TBOX) and gas chromatography-mass spectrometry were used to identify carbonyl-containing species. Seven carbonyl-containing products were observed. The yield of the primary product, pinonaldehyde was measured to be 76 %. Using cyclohexane as a hydroxyl radical (∙OH) scavenger, the yield of pinonaldehyde decreased to 46 %, indicating the influence secondary OH radicals have on α-pinene ozonolysis products. Furthermore, the use of TBOX, a small molecular weight derivatization agent, allowed for the acquisition of the first mass spectral data of oxopinonaldehyde, a tricarbonyl reaction product of α-pinene ozonolysis. The techniques described herein allow for an effective method for the collection and identification of terpene oxidation products in the indoor environment.


Datum: 01.09.2017


Macroseepage of methane and light alkanes at the La Brea tar pits in Los Angeles

Abstract

Geologic seepage of methane and light (C2-C5) alkanes was measured at the La Brea Tar Pits in Los Angeles. Samples were collected using flux chambers with stainless steel canisters and analyzed using gas chromatography. Average seepage rates from individual seepage sites were 970 ± 330 mg/h of methane, 14.0 ± 5.5 mg/h of ethane, 9.1 ± 3.7 mg/h of propane, 3.7 ± 1.6 mg/h of i-butane, 0.33 ± 0.16 mg/h of n-butane, 260 ± 120 μg/h of i-pentane, and 5.3 ± 1.9 μg/h of n-pentane, while maximum seepage rates exceeded 17 g/h of methane, 270 mg/h of ethane, 190 mg/h of propane, 95 mg/h of i-butane, 10 mg/h of n-butane, 7 mg/h of i-pentane, and 0.1 mg/h of n-pentane. These absolute fluxes have an additional unknown amount of error associated with them due to sampling methodology, and should be taken as the lower limit of emissions. Samples collected revealed generally dry gas, with high methane emissions relative to the light alkanes. Overall emissions from the tar pits were found to come not only from the active geologic seepage, but also from the outgassing of the standing asphalt at the site. Using the gas ratios, which are negligibly affected by errors introduced by sampling methodology, observed in this study, daily emissions of C2 – C5 alkanes from the La Brea area were estimated to be 4.7 ± 1.6 Mg, which represents 2–3 % of total emissions in the entire Los Angeles region.


Datum: 01.09.2017


Uptake of nitrogen dioxide (NO 2 ) on acidic aqueous humic acid (HA) solutions as a missing daytime nitrous acid (HONO) surface source

Abstract

A comprehensive kinetic study of a potential daytime nitrous acid (HONO) source reaction, the photoenhanced reduction reaction of the nitrogen dioxide (NO2) on acidic humic acid (HA), was completed using a wetted-wall flow tube (WWFT) (Fickert et al.: J. Phys. Chem. A. 102, 10689, 1998) photoreactor integrated with a high sensitivity HONO analyser (Wall et al.: J. Atmos. Chem. 55, 31–54, 2006; Huang et al.: Atmos. Environ. 36, 2225–2235, 2002). The nature of this reaction, is of great interest since recently observed, unpredictably high HONO daytime concentrations demand its ordinarily proposed heterogeneous source to proceed 60 times more rapidly at noon than during the night (Kleffmann et al.: ChemPhysChem 8, 1137–1144, 2007). This study investigated the nature of the reduction reaction with simulated colloidal HA aqueous solutions characteristic of anaerobic environmental conditions, varying in acidity, concentration and composition. Typical urban NO2 levels were investigated. Increasing photoenhanced HONO production with weakening solution acidity was detected due to increased deprotonation of the carboxyl groups within the humic acid. It was deduced that the acidic HA substrate contains numerous feasible chromophoric sensitizer units capable of photochemically reducing NO2 to HONO, owing to its ‘biofilm’ (Donlan, 2002) function under UV exposure. The mechanism was found to be more effective for HA standards with higher levels of ‘bioactivity’ (refractivity). Using a complex mathematical model developed, incorporating both chemistry and diffusion, reaction probability datasets were produced from the experimental data, providing evidence that this is, indeed, an environmentally important daytime HONO surface source reaction. The parameters required to scale up the data of the photoreactor to that of a regional rural/urban scale were assessed.


Datum: 01.09.2017


Ozone structure over the equatorial Andes from balloon-borne observations and zonal connection with two tropical sea level sites

Abstract

In this paper we present first-time measurements of ozone profiles from a high altitude station in Quito, Ecuador (0.19°S, 78.4°W, and 2391 masl) taken from June 2014 to September 2015. We interpret ozone observations in the troposphere, tropopause, and stratosphere through a zonal comparison with data from stations in the Atlantic and Pacific (Natal and San Cristobal from the SHADOZ network). Tropospheric ozone concentrations above the Andes are lower than ozone over San Cristobal and Natal for similar time periods. Ozone variability and pollution layers are also reduced in the troposphere above the Andes. We explain these differences in terms of reduced contributions from the boundary layer and from horizontal transport. In the tropical tropopause layer, ozone is well-mixed up to near the cold point tropopause level. In this regard, our profiles do not show constraints to deep mixing above 14 km, as has been consistently observed at other tropical stations. Total column ozone and stratospheric column ozone are comparable among the three sites. However, the contribution of tropospheric column ozone to total column ozone is significantly lower above the Andes. Our comparisons provide a connection between observations from tropical stations in equatorial South America separated by the wide continental mass. Identified differences in ozone throughout the atmospheric column demonstrate the global benefit of having an ozone sounding station at the equatorial Andes in support of global monitoring networks.


Datum: 01.09.2017


Modeling of hygroscopicity parameter kappa of organic aerosols using quantitative structure-property relationships

Abstract

The hygroscopicity of organic aerosol in the atmosphere can be represented by a semi-empirical single parameter, κ. In this work we test possibilities for developing quantitative structure-property relationship (QSPR) models for κ based on chemical similarity. Models were developed in two ways: by manually assessing the suitability of several plausible physico-chemical descriptors; and by systematically evaluating hundreds of constitutional (e.g. number of particular atoms, bond types, molecular weight,...), topological, electrostatic, geometrical and quantum-chemical descriptors with the QSPR modelling software CODESSA (COmprehensive DEscriptors for Structural and Statistical Analysis). A set of 74 compounds with measured κ values was taken from the literature and prediction capabilities of the developed models were evaluated by leave-one-out cross-validation procedure. A 5-parameter linear regression model obtained with CODESSA was found to be the most suitable. Among the five descriptors, the two providing the highest contributions to the total variance were found to be (i) the final heat of formation divided by the number of atoms (69 %) and (ii) the ratio of molecular weight and molecular volume (16 %), although other topological and electrostatic descriptors were also of non-negligible importance for prediction of κ. The squared correlation coefficient and the root mean square error of a leave-one-out cross-validation procedure were 0.80 and 0.037, respectively. The results show that quantitative structure-property relationship approaches are useful for modeling κ.


Datum: 01.09.2017


Erratum to: Uptake of nitrogen dioxide (NO 2 ) on acidic aqueous humic acid (HA) solutions as a missing daytime nitrous acid (HONO) surface source


Datum: 01.09.2017


Water-soluble inorganic ions of size-differentiated atmospheric particles from a suburban site of Mexico City

Abstract

During the MILAGRO campaign, March 2006, eight-stage cut impactors were used to sample atmospheric particles at Tecámac (T1 supersite), towards the northeast edge of the Mexico City Metropolitan Area, collecting fresh local emissions and aged pollutants produced in Mexico City. Particle samples were analyzed to determine total mass concentrations of Ca2+, Mg2+, NH4 +, K+, Cl, SO4 2−, and NO3 . Average concentrations were 22.1 ± 7.2 μg m−3 for PM10 and 18.3 ± 6.2 μg m−3 for PM1.8. A good correlation between PM10 and PM1.8, without influence from wind patterns, indicates that local emissions are more important than the city’s pollution transported to the site, despite the fact that Tecámac is just 40 km away from Mexico City. A lack of diurnal patterns in the PM2.5/PM1.8 ratio supports this conclusion. The inorganic composition of particles suggests that vehicles, soil resuspension, and industries are the main pollutant sources. Finally, the particles were found to be neutralized, in agreement with observations in the Mexico City Metropolitan Area.


Datum: 21.08.2017


Long-term high-frequency measurements of dibromomethane in the atmosphere at algae-rich and algae-poor coastal sites

Abstract

Dibromomethane (CH2Br2), a natural stratospheric ozone depleting substance, is mostly emitted from the ocean, but the relative importance of coastal (or macroalgae) and open ocean emissions is unknown. We made long-term high-frequency measurements of CH2Br2 concentrations at two remote coastal sites in Japan, on the subtropical Hateruma Island (poor in macroalgae) and at Cape Ochiishi (rich in macroalgae). CH2Br2 concentrations at Hateruma showed prominent seasonal variation, being lower in summer (around 0.94 ppt) than in winter (around 1.23 ppt). In contrast, CH2Br2 concentrations at Ochiishi were highly variable, often exceeding 2 ppt in the summer but with minimum baseline concentrations close to those from Hateruma; in the winter the concentrations were almost constant at about 1.3 ppt. Analysis of the data suggested that (1) emissions from macroalgae were not likely to extend offshore, but instead were localized near the shore, (2) strong macroalgal emissions of CH2Br2 were almost limited to the summer, but it was not reflected in the seasonality of the baseline concentrations of CH2Br2 in the atmosphere, and therefore (3) macroalgal or coastal emissions of CH2Br2 in the temperate zone might have a rather limited contribution to the global CH2Br2 sources. These findings are especially important for the understanding of the tropospheric and stratospheric bromine budget.


Datum: 16.08.2017


Atmospheric hydroperoxides measured over a rural site in central Japan during spring: helicopter-borne measurements

Abstract

Measurements of the concentrations of H2O2 and methyl hydroperoxide (MHP), O3, and SO2 over Imizu City, Toyama Prefecture, Japan were performed in March using a helicopter. H2O2 concentrations were higher at an altitude of approximately 2,400 m (8,000 ft). The H2O2 concentrations (< 0.8 ppb) in the spring were much lower than those observed during the summer observations. MHP was also higher in the high-altitude atmosphere. Lower concentrations of H2O2 were observed when high air pollutants were actively transported from Asian continent. The concentrations of H2O2 were mostly lower than those of SO2; this condition is called oxidant limitation. If H2O2 concentration rises in cold months, the acidification of cloud water may be accelerated at high elevations in central Japan where air pollution is actively transported.


Datum: 04.08.2017


Concentrations of metallic elements in long-range-transported aerosols measured simultaneously at three coastal sites in China and Japan

Abstract

To determine the effects of long-range transport of aerosols from an upwind area in East Asia to a downwind area in Japan, we chemically analyzed aerosols collected simultaneously on Tuoji Island (Shandong Province, China), Fukue Island (Nagasaki Prefecture, Japan), and Cape Hedo (Okinawa Prefecture, Japan). We focused on changes in the metallic composition of PM2.5 aerosols during long-range transport. The average mass concentrations of PM2.5 at the three sites decreased in the order Tuoji Island > Fukue Island ≈ Cape Hedo (48.3 ± 4.5, 13.9 ± 1.5, and 13.2 ± 0.9 μg/m3, respectively). The fraction of coarse particles in total suspended particles estimated by (1–PM2.5/TSP) was highest on Cape Hedo, indicating that the contribution of sea salts was increased by long-range transport of the aerosols over the ocean. Enrichment factor analysis revealed that at all three sites, Al, K, Ca, Mn, Fe, Co, Sr, and Ba originated from soil; whereas Cr, Ni, Cu, Zn, As, Mo, Ag, Cd, Sn, Sb, Tl, and P appeared to be of anthropogenic origin. Na was the most abundant element on Cape Hedo, indicating the addition of sea salts during aerosol transport. The V concentration was highest at Fukue Island, which was ascribed to V emission from ships. Sixty-one percent of the V on Fukue Island and 62% of the V on Cape Hedo were determined to have originated from ships, implicating of data obtained on dates during which backward trajectory analysis indicated that the same air mass passed over Tuoji Island, Fukue Island, and Cape Hedo in that order.


Datum: 07.06.2017


A nocturnal atmospheric loss of CH 2 I 2 in the remote marine boundary layer

Abstract

Ocean emissions of inorganic and organic iodine compounds drive the biogeochemical cycle of iodine and produce reactive ozone-destroying iodine radicals that influence the oxidizing capacity of the atmosphere. Di-iodomethane (CH2I2) and chloro-iodomethane (CH2ICl) are the two most important organic iodine precursors in the marine boundary layer. Ship-borne measurements made during the TORERO (Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOC) field campaign in the east tropical Pacific Ocean in January/February 2012 revealed strong diurnal cycles of CH2I2 and CH2ICl in air and of CH2I2 in seawater. Both compounds are known to undergo rapid photolysis during the day, but models assume no night-time atmospheric losses. Surprisingly, the diurnal cycle of CH2I2 was lower in amplitude than that of CH2ICl, despite its faster photolysis rate. We speculate that night-time loss of CH2I2 occurs due to reaction with NO3 radicals. Indirect results from a laboratory study under ambient atmospheric boundary layer conditions indicate a k CH2I2+NO3 of ≤4 × 10−13 cm3 molecule−1 s−1; a previous kinetic study carried out at ≤100 Torr found k CH2I2+NO3 of 4 × 10−13 cm3 molecule−1 s−1. Using the 1-dimensional atmospheric THAMO model driven by sea-air fluxes calculated from the seawater and air measurements (averaging 1.8 +/− 0.8 nmol m−2 d−1 for CH2I2 and 3.7 +/− 0.8 nmol m−2 d−1 for CH2ICl), we show that the model overestimates night-time CH2I2 by >60 % but reaches good agreement with the measurements when the CH2I2 + NO3 reaction is included at 2–4 × 10−13 cm3 molecule−1 s−1. We conclude that the reaction has a significant effect on CH2I2 and helps reconcile observed and modeled concentrations. We recommend further direct measurements of this reaction under atmospheric conditions, including of product branching ratios.


Datum: 01.06.2017


Photochemical activation of chlorine by iron-oxide aerosol

Abstract

The photochemical activation of chlorine by dissolved iron in artificial sea-salt aerosol droplets and by highly dispersed iron oxide (Fe2O3) aerosol particles (mainly hematite, specific surface ~150 m2 g−1) exposed to gaseous HCl, was investigated in humidified air in a Teflon simulation chamber. Employing the radical-clock technique, we quantified the production of gaseous atomic chlorine (Cl) from the irradiated aerosol. When the salt aerosol contained Fe2O3 at pH 6, no significant Cl production was observed, even if the dissolution of iron was forced by “weathering” (repeatedly freezing and thawing for five times). Adjusting the pH in the stock suspension to 2.6, 2.2, and 1.9 and equilibrating for one week resulted in a quantifiable amount of dissolved iron (0.03, 0.2, and 0.6 mmol L−1, respectively) and in gaseous Cl production rates of ~1.6, 6, and 8 × 1021 atoms cm−2 h−1, respectively. In a further series of experiments, the pure Fe2O3 aerosol was exposed to various levels of gaseous hydrogen chloride (HCl). The resulting Cl production rates ranged from 8 × 1020 Cl atoms cm−2 h−1 (at ~4 ppb HCl) to 5 × 1022 Cl atoms cm−2 h−1 (at ~350 ppb HCl) and confirmed the uptake and conversion of HCl to atomic Cl (at HCl to Cl conversion yields of 2–5 %, depending on the relative humidity). The Fe2O3 experiments indicate that iron-induced Cl formation may be important for highly soluble combustion-aerosol particles in marine environments in the presence of gaseous HCl.


Datum: 01.06.2017


Introduction to special issue on natural halocarbons in the atmosphere


Datum: 01.06.2017


Emission estimates of methyl chloride from industrial sources in China based on high frequency atmospheric observations

Abstract

Methyl Chloride (CH3Cl) is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion (Carpenter et al. 2014). In the global CH3Cl budget, the atmospheric CH3Cl emissions is predominantly maintained by natural sources, of which magnitudes have been relatively well-constrained. However, significant uncertainties still remain in the CH3Cl emission strengths from anthropogenic sources. High-frequency and high-precision in situ measurements of atmospheric CH3Cl concentrations obtained since 2008 at Gosan station (a remote background site in the East Asia) reveal significant pollution events superimposed on the seasonally varying regional background levels. Back trajectory statistics showed that air masses corresponding to the observed CH3Cl enhancement largely originated from regions of intensive industrial activities in China. Based on an inter-species correlation method, estimates of CH3Cl emissions from manufacturing industries including coal combustion, use of feedstocks, or process agents in chemical production for China (2008–2012) are 297 ± 71 Gg yr.−1 in 2008 to 480 ± 99 Gg yr.−1 in 2009, followed by a gradual decrease of about 25% between 2009 and 2012 (398 ± 92 Gg yr.−1 for 2010; 286 ± 68 Gg yr.−1 for 2011; 358 ± 92 Gg yr.−1 for 2012). The annual average of industrial CH3Cl emissions for 2008–2012 (363 ± 85 Gg yr.−1) in China is comparable to the known total global anthropogenic CH3Cl emissions accounting only for coal combustion and indoor biofuel use. This may suggest that unless emissions from the chemical industry are accounted for, global anthropogenic emissions of CH3Cl have been substantially underestimated. In particular, since industrial production and use of CH3Cl have not been regulated under the Montreal Protocol (MP) or its successor amendments, continuous monitoring of Chinese CH3Cl outflow is important to properly evaluate its anthropogenic emissions.


Datum: 01.06.2017


Seasonal variation of bromocarbons at Hateruma Island, Japan: implications for global sources

Abstract

High-frequency measurements of dibromomethane (CH2Br2) and bromoform (CHBr3) at Hateruma Island, in the subtropical East China Sea, were performed using automated preconcentration gas chromatography/mass spectrometry. Their baseline concentrations, found in air masses from the Pacific Ocean, were 0.65 and 0.26 ppt, respectively, in summer and 1.08 and 0.87 ppt, respectively, in winter. Air masses transported from Southeast Asia were rich in bromocarbons, suggesting strong emissions in this area. The passage of cold fronts from the Asian continent was associated with sharp increases in observed concentrations of bromocarbons derived from coastal regions of the continent. Comparison of the relationships between [CH2Br2]/[CHBr3] and [CHBr3] in the Hateruma Island data with those in monthly mean data from 14 globally distributed U.S. National Oceanic and Atmospheric Administration ground stations suggested that these gases are produced primarily from a common process on a global scale.


Datum: 01.06.2017


Seasonal variation of volatile organic iodine compounds in the water column of Funka Bay, Hokkaido, Japan

Abstract

Volatile organic iodine compounds (VOIs) emitted from the ocean surface to the air play an important role in atmospheric chemistry. Shipboard observations were conducted in Funka Bay, Hokkaido, Japan, bimonthly or monthly from March 2012 to December 2014, to elucidate the seasonal variations of VOI concentrations in seawater and their sea-to-air iodine fluxes. The bay water exchanges with the open ocean water of the North Pacific twice a year (early spring and autumn). Vertical profiles of CH2I2, CH2ClI, CH3I, and C2H5I concentrations in the bay water were measured bimonthly or monthly within an identified water mass. The VOI concentrations began to increase after early April at the end of the diatom spring bloom, and represented substantial peaks in June or July. The temporal variation of the C2H5I profile, which showed a distinct peak in the bottom layer from April to July, was similar to the PO4 3− variation profile. Correlation between C2H5I and PO4 3− concentrations (r = 0.93) suggests that C2H5I production was associated with degradation of organic matter deposited on the bottom after the spring bloom. CH2I2 and CH2ClI concentrations increased substantially in the surface and subsurface layers (0–60 m) in June or July resulted in a clear seasonal variation of the sea-to-air iodine flux of the VOIs (high in summer or autumn and low in spring).


Datum: 01.06.2017


Halogenation processes linked to red wood ant nests ( Formica spp.) and tectonics

Abstract

We investigated and evaluated the occurrence of fault zone tracer gases (CO2, He, Rn), volatile organohalogens (CH3Cl, CHCl3, CHBr3), alkanes and limonene in soil and nest gases of red wood ants (RWA) in comparison to ambient air, in a seismically active area. In this new approach, we compared RWA-free areas to RWA-areas by combining different investigation and analytical methods. In soil gas, the fault zone tracer gas Rn was surprisingly highly correlated to limonene, suggesting a combination of biotic production of limonene and abiotic degassing of Rn in a seismically active area; moderate correlations were found with trihalomethanes and other halocarbons. In RWA nests a variety of elevated concentrations of haloforms were found, while remaining below the atmospheric background values in RWA-free areas. The evidence of CHCl3 in RWA nests is the first record. Its average concentrations in nests of F. rufa and F. polyctena were up to 3 fold higher than atmospheric background and up to 28–70 fold higher compared to e.g. volcanic emissions being considered as one of its main geogenic sources. Thus, RWA nests could possibly be an additional source for CHCl3 liberation. Consequently, apart from RWA being bioindicators for seismically active degassing faults, they might also be used as bioindicators for CHCl3 formation in forest soils. Although we cannot yet differentiate between a geogenic/abiotic and a biotic formation. RWA nests will have to be reconsidered for halocarbon formation in future quantifications of geochemical cycles at global scale, since they impact organic soil chemistry through biotic and/or abiotic pathways. Therefore, further larger-scale research in different tectonic settings but also in well-known CHCl3 “hot spot” study areas such as the Klosterhede area (Denmark) should focus directly on gas sampling from confirmed active fault systems. Nests of other ant species should be addressed to compare seasonal, diurnal and nocturnal variations of degassing procedures in relation to earth tides, different geologic settings, and tectonic events such as earthquakes and on quantifying the fluxes to the atmosphere.


Datum: 01.06.2017


Future emissions of marine halogenated very-short lived substances under climate change

Abstract

Halogenated Very Short-lived Substances (VSLS), such as bromoform, dibromomethane and methyl iodide, are naturally produced in the oceans and are involved in ozone depletion in the troposphere and the stratosphere. The effect of climate change on the oceanic emissions of these compounds is not well quantified. Based on present-day observed global oceanic and atmospheric concentrations, and historic and future data from three CMIP5 models, past and future sea-to-air fluxes of these VSLS are calculated. The simulations are used to infer possible effects of projected changes of physical forcing on emissions in different oceanic regimes. CMIP5 model output for 1979–2100 from the historical scenario and the RCP scenarios 2.6 and 8.5 are used as input data for the emission calculations. Of the parameters that have the main influence on the sea-to-air fluxes, the global sea surface temperatures show a steady increase during the twenty-first century, while the projected changes of sea surface wind speed is very small. The calculated emissions based on the historical CMIP5 model runs (1979–2005) increased over the 26 year period and agree well with the emissions based on ERA-Interim data. The future sea-to-air fluxes of VSLS generally increase during the twenty-first century under the assumption of constant concentration fields in the ocean and atmosphere. The multi-model mean global emissions of bromoform increase by 29.4% (9.0%) between 1986 and 2005 and 2081–2100 under RCP 8.5 (2.6) and dibromomethane and methyl iodide emissions increase by 23.3% (6.4%) and 5.5% (1.5%), respectively. Uncertainties of the future emission estimates, driven by ongoing environmental changes such as changing oceanic productivity (not considered in this study) are discussed.


Datum: 01.06.2017


Effect of temperature on the methyl chloride production rate in a marine phytoplankton, Phaeodactylum tricornutum

Abstract

Methyl halides such as methyl chloride (CH3Cl) are known to be important carriers of halogen from the ocean to the atmosphere, and the halogens they release into the stratosphere by photolysis catalyze ozone depletion. Marine phytoplankton have been reported as a source of CH3Cl, but the effects of environmental temperature on the CH3Cl production by phytoplankton have not been investigated. In this study, we investigated the effects of temperature on the production of CH3Cl in the culture of a marine diatom, Phaeodactylum tricornutum CCMP 630, incubated at 10, 15, 20, 25, and 30 °C. CH3Cl concentrations in cultured samples were determined using purge and trap gas chromatograph–mass spectrometry. Phytoplankton growth was monitored by measuring the chlorophyll a concentrations. CH3Cl production was observed for several weeks at four different temperatures ranging from 10 to 25 °C. The CH3Cl production from P. tricornutum was increased with increasing temperature from 10 to 25 °C, and the maximum production rate for CH3Cl was 0.21~0.26 μmol (g chlorophyll a)−1 d−1 at 25 °C, which was several times higher than that at 10 °C (~0.03 μmol (g chlorophyll a)−1 d−1). The Arrhenius equation was successfully used to characterize the effects of temperature on the production rates of CH3Cl in the culture of P. tricornutum. Our results suggest that water temperature directly affects CH3Cl production derived from P. tricornutum and that water temperature would be a significant factor for estimating the emissions of CH3Cl from marine environments.


Datum: 01.06.2017


Chemical characteristics of atmospheric bulk deposition in a semi-rural area of the Po Valley (Italy)

Abstract

This study provides an analysis of a five-year time series chemical composition of the bulk deposition (2009–2013), collected within a farm surrounded by industrial and urban settlements in a semi-rural area of the Po Valley, with the aim of characterizing potential emission sources affecting precipitation composition at the site. Most monitoring efforts in this region, recognized as one of the most polluted in the world both due to the intense industrialisation and urbanisation as well as to frequent air stagnation conditions, are presently devoted more to gaseous and particulate pollutants than to precipitation chemistry. The bulk deposition samples were very concentrated in chemical species, both acidic and alkaline, high compared to other polluted sites in the world and to locations in the same district. The mean ions concentrations (in μeq l−1) are: NO3 (243) > SO4 2− (220) > PO4 3− (176) > Cl (153) > NO2 (29) > F (2.6); NH4 + (504) > Ca2+ (489) > K+ (151) > Na+ (127) > Mg2+ (127). pH data shows a trend toward slightly alkaline conditions attributed to the large presence of ammonium and crustal elements, in spite of high concentrations of nitrates and sulphates. The relevant concentrations of Ca2+ and Mg2+ further suggests that these alkaline conditions might be due to the correspondingly significant concentrations of carbonates/bicarbonates in our dataset. While back-trajectories analysis suggests the stronger importance of local resuspension over long-range transport, statistical analyses on ion composition highlight the key role exerted by agricultural activity, especially in the case of NH4 +, K+, Ca2+ and PO4 3− (especially linked to fertilisation practices and soil resuspension due to mechanical operations). Apart from Na+ and Cl ions which correlate well as expected, indicating their likely common origin from marine salt, the identification of the origin of the other ions is very complex due to the contribution of diverse local sources, such as industrial and residential settlements.


Datum: 10.05.2017






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