scholarly journals Distinguishing molecular characteristics of aerosol water soluble organic matter from the 2011 trans-North Atlantic US GEOTRACES cruise

2014 ◽  
Vol 14 (5) ◽  
pp. 6427-6470 ◽  
Author(s):  
A. S. Wozniak ◽  
A. S. Willoughby ◽  
S. C. Gurganus ◽  
P. G. Hatcher
Keyword(s):  
Organic Matter ◽  
North Atlantic ◽  
North American ◽  
Water Soluble ◽  
Molecular Characteristics ◽  
Molecular Formula ◽  
North African ◽  
Air Mass ◽  
Air Mass Trajectories ◽  
Two Samples

Abstract. The molecular characteristics of aerosol organic matter (OM) determines to a large extent its impacts on the atmospheric radiative budget and ecosystem function in terrestrial and aquatic environments, yet the molecular details of aerosol OM from different sources are not well established. Aerosol particulate samples having North American-influenced, North African-influenced, and marine (minimal recent continental influence) air mass back trajectories were collected as part of the 2011 trans-North Atlantic US GEOTRACES cruise and analyzed for their water soluble OM (WSOM) molecular characteristics using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Principal component analysis (PCA) separated the samples into five groups defined by distinct molecular formula characteristics. An abundance of nitrogen containing compounds with molecular formulas consistent with amino acid derivatives defined the two samples comprising the Primary Marine group suggesting a primary marine biological source to their WSOM in spite of their North American-influenced air mass trajectories. A second group of samples (Aged Marine) having primarily marine air mass trajectories was characterized by an abundance of low O / C (0.15–0.45) sulfur containing compounds consistent with organosulfate compounds formed via secondary aging reactions in the atmosphere. Several samples having North American-influenced air mass trajectories formed another group again characterized by organosulfate and nitrooxyorganosulfate type compounds with higher O / C ratios (0.5–1.0) than the Aged Marine samples reflecting the combustion influence from the North American continent. All the samples having North African-influenced air mass trajectories grouped together in the PCA and were characterized by a lack of heteroatom (N, S, P) containing molecular formulas covering a wide O / C range (0.15–0.90) reflecting the desert source of this WSOM. The two marine groups showed molecular formulas that, on average, had higher O / C ratios and lower O / C ratios and modified aromaticity indices than the two continentally-influenced groups suggesting these properties are characteristic of marine vs. continental aerosol WSOM. The final sample group, the Mixed Source samples, showed intermediate molecular characteristics suggesting no dominant continental or marine source. The source-specific OM details described here will aid efforts to link aerosol OM source with molecular characteristics and impacts in the environment.

scholarly journals Distinguishing molecular characteristics of aerosol water soluble organic matter from the 2011 trans-North Atlantic US GEOTRACES cruise

2014 ◽  
Vol 14 (16) ◽  
pp. 8419-8434 ◽  
Author(s):  
A. S. Wozniak ◽  
A. S. Willoughby ◽  
S. C. Gurganus ◽  
P. G. Hatcher
Keyword(s):  
Organic Matter ◽  
North Atlantic ◽  
North American ◽  
Water Soluble ◽  
Molecular Characteristics ◽  
Molecular Formula ◽  
North African ◽  
Air Mass ◽  
Air Mass Trajectories ◽  
Two Samples

Abstract. The molecular characteristics of aerosol organic matter (OM) determines to a large extent its impacts on the atmospheric radiative budget and ecosystem function in terrestrial and aquatic environments, yet the OM molecular details of aerosols from different sources are not well established. Aerosol particulate samples with North American-influenced, North African-influenced, and marine (minimal recent continental influence) air mass back trajectories were collected as part of the 2011 trans-North Atlantic US GEOTRACES cruise and analyzed for their water soluble OM (WSOM) molecular characteristics using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Principal component analysis (PCA) separated the samples into five groups defined by distinct molecular formula characteristics. An abundance of nitrogen containing compounds with molecular formulas consistent with amino acid derivatives defined the two samples comprising the primary marine group (henceforth referred to as Primary Marine), which suggest a primary marine biological source to their WSOM in spite of their North American-influenced air mass trajectories. A second group of samples (aged marine, henceforth referred to as Aged Marine) with marine air mass trajectories was characterized by an abundance of low O / C (0.15–0.45) sulfur containing compounds consistent with organosulfate compounds formed via secondary aging reactions in the atmosphere. Several samples having North American-influenced air mass trajectories formed another group again characterized by organosulfate and nitrooxyorganosulfate type compounds with higher O / C ratios (0.5–1.0) than the Aged Marine samples reflecting the combustion influence from the North American continent. All the samples with North African-influenced air mass trajectories were grouped together in the PCA and were characterized by a lack of heteroatom (N, S, P) containing molecular formulas covering a wide O / C range (0.15–0.90) reflecting the desert source of this WSOM. The two marine groups showed molecular formulas that, on average, had higher H / C ratios and lower O / C ratios and modified aromaticity indices than the two continentally influenced groups, which suggests that these properties are characteristic of marine vs. continental aerosol WSOM. The final sample group, the mixed source samples (henceforth referred to as Mixed Source), showed intermediate molecular characteristics, which suggests no dominant continental or marine source. The source-specific OM details described here will aid efforts to link aerosol OM source with molecular characteristics and impacts in the environment.

scholarly journals Molecular characterization of water soluble organic nitrogen in marine rainwater by ultra-high resolution electrospray ionization mass spectrometry

2012 ◽  
Vol 12 (7) ◽  
pp. 3557-3571 ◽  
Author(s):  
K. E. Altieri ◽  
M. G. Hastings ◽  
A. J. Peters ◽  
D. M. Sigman
Keyword(s):  
Mass Spectrometry ◽  
Organic Matter ◽  
High Resolution ◽  
Electrospray Ionization ◽  
Organic Nitrogen ◽  
Warm Season ◽  
Cold Season ◽  
Water Soluble ◽  
Air Mass ◽  
Soluble Organic Nitrogen

Abstract. Atmospheric water soluble organic nitrogen (WSON) is a subset of the complex organic matter in aerosols and rainwater, which impacts cloud condensation processes and aerosol chemical and optical properties and may play a significant role in the biogeochemical cycle of N. However, its sources, composition, connections to inorganic N, and variability are largely unknown. Rainwater samples were collected on the island of Bermuda (32.27° N, 64.87° W), which experiences both anthropogenic and marine influenced air masses. Samples were analyzed by ultra-high resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry to chemically characterize the WSON. Elemental compositions of 2281 N containing compounds were determined over the mass range m/z+ 50 to 500. The five compound classes with the largest number of elemental formulas identified, in order from the highest number of formulas to the lowest, contained carbon, hydrogen, oxygen, and nitrogen (CHON+), CHON compounds that contained sulfur (CHONS+), CHON compounds that contained phosphorus (CHONP+), CHON compounds that contained both sulfur and phosphorus (CHONSP+), and compounds that contained only carbon, hydrogen, and nitrogen (CHN+). Compared to rainwater collected in the continental USA, average O:C ratios of all N containing compound classes were lower in the marine samples whereas double bond equivalent values were higher, suggesting a reduced role of secondary formation mechanisms. Despite their prevalence in continental rainwater, no organonitrates or nitrooxy-organosulfates were detected, but there was an increased presence of organic S and organic P containing compounds in the marine rainwater. Cluster analysis showed a clear chemical distinction between samples collected during the cold season (October to March) which have anthropogenic air mass origins and samples collected during the warm season (April to September) with remote marine air mass origins. This, in conjunction with patterns identified in van Krevelen diagrams, suggests that the cold season WSON is a mixture of organic matter with both marine and anthropogenic sources while in the warm season the WSON appears to be dominated by marine sources. These findings indicate that, although the concentrations and percent contribution of WSON to total N is fairly consistent across diverse geographic regions, the chemical composition of WSON varies strongly as a function of source region and atmospheric environment.

ORGANIC COMPOUNDS FORMED BY THE HYDROGEN PEROXIDE XIDATION OF SOILS

1977 ◽  
Vol 57 (3) ◽  
pp. 223-231 ◽  
Author(s):  
S. M. GRIFFITH ◽  
M. SCHNITZER
Keyword(s):  
Hydrogen Peroxide ◽  
Fatty Acids ◽  
Organic Matter ◽  
Aromatic Compounds ◽  
Water Soluble ◽  
Mineralogical Analysis ◽  
Two Samples ◽  
Subsurface Soil ◽  
Phenolic Extraction ◽  
Soil Constituents

Two samples taken from tropical volcanic surface soils and one sample from a Canadian Podzol subsurface soil were oxidized with H2O2 under conditions usually employed for the removal of organic matter from soils prior to mineralogical analyses. Between 65 and 82% of the C but only between 23 and 36% of the N in the initial organic matter in the three soils was oxidized to volatile and water-soluble products. Among the latter, small amounts of about 40 different aliphatic and aromatic compounds were identified, most of which were phenolic. Extraction with organic solvents removed n-alkanes and n-fatty acids from H2O2-resistant organic matter, but most of the latter consisted of humic substances strongly bonded to or absorbed on inorganic soil constituents. H2O2-resistant fractions accounted in the case of two soils, initially rich in organic matter, for 12.0 and 7.5% of the air-dry weights of peroxidized soils. The presence of such substantial amounts of H2O2-resistant organic matter may interfere with the dispersion and mineralogical analysis of peroxidized soils, especially those with high initial organic matter contents.

Relationships among aerosol water soluble organic matter, iron and aluminum in European, North African, and Marine air masses from the 2010 US GEOTRACES cruise

2013 ◽  
Vol 154 ◽  
pp. 24-33 ◽  
Author(s):  
Andrew S. Wozniak ◽  
Rachel U. Shelley ◽  
Rachel L. Sleighter ◽  
Hussain A.N. Abdulla ◽  
Peter L. Morton ◽  
...  
Keyword(s):  
Organic Matter ◽  
Water Soluble ◽  
Soluble Organic Matter ◽  
North African ◽  
Air Masses ◽  
European North ◽  
Marine Air

scholarly journals Influence of the North Atlantic Oscillation on air pollution transport

2012 ◽  
Vol 12 (2) ◽  
pp. 869-877 ◽  
Author(s):  
T. Christoudias ◽  
A. Pozzer ◽  
J. Lelieveld
Keyword(s):  
North Atlantic Oscillation ◽  
North Atlantic ◽  
North American ◽  
Trace Gases ◽  
Water Soluble ◽  
The Arctic ◽  
Pollution Transport ◽  
The North ◽  
The North Atlantic ◽  
The North Atlantic Oscillation

Abstract. We examined the influence of the North Atlantic Oscillation (NAO) on the atmospheric dispersion of pollution by computing the emission, transport and removal of idealized insoluble gaseous and water-soluble aerosol tracers, tagged by the continent of origin. We simulated a period of 50 yr (1960–2010), using the ECHAM5/MESSy1 atmospheric chemistry (EMAC) general circulation model. The model accounts for anthropogenic, biogenic and biomass burning sources, removal of trace gases through OH oxidation, and precipitation, sedimentation and deposition of aerosols. The model is shown to reproduce the observed spatial features of the NAO, moisture transports and precipitation. During high NAO phase seasons the axis of maximum westerly North American trace gas transports extends relatively far to the north and east over Europe. The NAO phase is significantly correlated with North American insoluble gas and soluble aerosol tracer concentrations over the northwestern Atlantic Ocean and across northern Europe, and with European trace gases and aerosols over Africa and north of the Arctic circle. We find a strong anti-correlation between the phase of the NAO and European pollutant gas concentration over western and central Europe.

scholarly journals Influence of the North Atlantic Oscillation on air pollution transport

2011 ◽  
Vol 11 (9) ◽  
pp. 25967-25989
Author(s):  
T. Christoudias ◽  
A. Pozzer ◽  
J. Lelieveld
Keyword(s):  
North Atlantic Oscillation ◽  
North Atlantic ◽  
North American ◽  
Trace Gases ◽  
Water Soluble ◽  
The Arctic ◽  
Pollution Transport ◽  
The North ◽  
The North Atlantic ◽  
The North Atlantic Oscillation

Abstract. We examined the influence of the North Atlantic Oscillation (NAO) on the atmospheric dispersion of pollution by computing the emission, transport and removal of insoluble gaseous and water-soluble aerosol tracers, tagged by the continent of origin. We simulated a period of 50 yr (1960–2010), using the ECHAM/MESSy atmospheric chemistry (EMAC) general circulation model. The model accounts for anthropogenic, biogenic and biomass burning sources, removal of trace gases through OH oxidation, and precipitation, sedimentation and deposition of aerosols. The model is shown to reproduce the observed spatial features of the NAO, moisture transports and precipitation. During high NAO phase seasons the axis of maximum westerly North American trace gas transports extends relatively far to the north and east over Europe. The NAO phase is significantly correlated with North American tracer concentrations over the northwestern Atlantic Ocean and across northern Europe, and with European trace gases and aerosols beyond the arctic circle. Our results indicate marked differences and partly reversed correlations for the insoluble gas and the soluble aerosol tracers. We find a strong anti-correlation over western and central Europe between European pollutant gas and aerosol concentrations and the phase of the NAO.

scholarly journals Molecular characterization of water soluble organic nitrogen in marine rainwater by ultra-high resolution electrospray ionization mass spectrometry

2011 ◽  
Vol 11 (11) ◽  
pp. 31283-31321
Author(s):  
K. E. Altieri ◽  
M. G. Hastings ◽  
A. J. Peters ◽  
D. M. Sigman
Keyword(s):  
Mass Spectrometry ◽  
Organic Matter ◽  
High Resolution ◽  
Electrospray Ionization ◽  
Organic Nitrogen ◽  
Warm Season ◽  
Cold Season ◽  
Water Soluble ◽  
Air Mass ◽  
Soluble Organic Nitrogen

Abstract. Atmospheric water soluble organic nitrogen (WSON) is a subset of the complex organic matter in aerosols and rainwater, which impacts cloud condensation processes and aerosol chemical and optical properties, and may play a significant role in the biogeochemical cycle of N. However, its sources, composition, connections to inorganic N, and variability are largely unknown. Rainwater samples were collected on the island of Bermuda (32.27° N, 64.87° W), which experiences both anthropogenic and marine influenced air masses. Samples were analyzed by ultra-high resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry to chemically characterize the WSON. Elemental compositions of 2455 N containing compounds were determined over the mass range m/z+ 50 to 500. The five compound classes with the largest number of elemental formulas identified, in order from the highest number of formulas to the lowest, contained carbon, hydrogen, oxygen, and nitrogen (CHON+), CHON compounds that contained sulfur (CHONS+), CHON compounds that contained phosphorous (CHONP+), CHON compounds that contained both sulfur and phosphorous (CHONSP+), and compounds that contained only carbon, hydrogen, and nitrogen (CHN+). No organonitrates or nitrooxy-organosulfates were detected, but there was an increased presence of organic S and organic P containing compounds in the marine rainwater. Compared to rainwater collected in the continental USA, average O:C ratios of all N containing compound classes were lower in the marine samples whereas double bond equivalent values were higher, suggesting a reduced role of secondary formation mechanisms. Cluster analysis showed a clear chemical distinction between samples collected during the cold season (October to March) which have anthropogenic air mass origins and samples collected during the warm season (April to September) with remote marine air mass origins. This, in conjunction with patterns identified in van Krevelen diagrams, suggests that the cold season WSON is a mixture of organic matter with both marine and anthropogenic sources while in the warm season the WSON appears to be dominated by marine sources. These findings indicate that, although the concentrations and percent contribution of WSON to total N is fairly consistent across diverse geographic regions, the chemical composition of WSON varies strongly as a function of source region and atmospheric environment.

Aerosol water soluble organic matter characteristics over the North Atlantic Ocean: Implications for iron-binding ligands and iron solubility

2015 ◽  
Vol 173 ◽  
pp. 162-172 ◽  
Author(s):  
Andrew S. Wozniak ◽  
Rachel U. Shelley ◽  
Stephanie D. McElhenie ◽  
William M. Landing ◽  
Patrick G. Hatcher
Keyword(s):  
Organic Matter ◽  
Atlantic Ocean ◽  
North Atlantic ◽  
North Atlantic Ocean ◽  
Water Soluble ◽  
Iron Binding ◽  
Soluble Organic Matter ◽  
Iron Solubility ◽  
The North ◽  
The North Atlantic

scholarly journals Impact of North America on the aerosol composition in the North Atlantic free troposphere

2017 ◽  
Vol 17 (12) ◽  
pp. 7387-7404 ◽  
Author(s):  
M. Isabel García ◽  
Sergio Rodríguez ◽  
Andrés Alastuey
Keyword(s):  
Organic Matter ◽  
North America ◽  
North Atlantic ◽  
North American ◽  
Sea Salt ◽  
Free Troposphere ◽  
Aerosol Composition ◽  
The North ◽  
The North Atlantic

Abstract. In the AEROATLAN project we study the composition of aerosols collected over  ∼  5 years at Izaña Observatory (located at  ∼  2400 m a.s.l. in Tenerife, the Canary Islands) under the prevailing westerly airflows typical of the North Atlantic free troposphere at subtropical latitudes and midlatitudes. Mass concentrations of sub-10 µm aerosols (PM10) carried by westerly winds to Izaña, after transatlantic transport, are typically within the range 1.2 and 4.2 µg m−3 (20th and 80th percentiles). The main contributors to background levels of aerosols (PM10 within the 1st–50th percentiles  =  0.15–2.54 µg m−3) are North American dust (53 %), non-sea-salt sulfate (14 %) and organic matter (18 %). High PM10 events (75th–95th percentiles  ≈  4.0–9.0 µg m−3) are prompted by dust (56 %), organic matter (24 %) and non-sea-salt sulfate (9 %). These aerosol components experience a seasonal evolution explained by (i) their spatial distribution in North America and (ii) the seasonal shift of the North American outflow, which migrates from low latitudes in winter (∼  32° N, January–March) to high latitudes in summer (∼  52° N, August–September). The westerlies carry maximum loads of non-sea-salt sulfate, ammonium and organic matter in spring (March–May), of North American dust from midwinter to mid-spring (February–May) and of elemental carbon in summer (August–September). Our results suggest that a significant fraction of organic aerosols may be linked to sources other than combustion (e.g. biogenic); further studies are necessary for this topic. The present study suggests that long-term evolution of the aerosol composition in the North Atlantic free troposphere will be influenced by air quality policies and the use of soils (potential dust emitter) in North America.

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