Investigating the water-soluble organic functionality of urban aerosols using two-dimensional correlation of solid-state 13C NMR and FTIR spectral data

Duarte, Regina M.B.O.; Freire, Sandra M.S.C.; Duarte, Armando C.

doi:10.1016/j.atmosenv.2015.06.043

Cited by 45 publications

(42 citation statements)

References 40 publications

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“…Apparently, in S. Paulo, the lowest levels of the WSOM/PM ratios were also observed during summer season, although no variation between seasons could be discern based on the obtained median WSOM/PM values. These results suggest that contributions of biomass burning combined with low temperature conditions (average value of 11 C, Table S1 in SI) could be important to ambient water-soluble OA in Aveiro during winter (e.g., Duarte et al, 2015), whereas the somewhat lower relative humidity and total precipitation and higher ambient temperatures (average value of 17 C) in S. Paulo during winter (Table S1 in SI) could contribute to the observed range of WSOM/PM ratios. Fig.…”

Section: Contribution Of Wsoc To Pm Massmentioning

confidence: 96%

“…One of the most important attributes of atmospheric OA for both climate and health impacts is their chemical composition. It has been shown that most OA mass at urban and anthropogenically influenced rural/remote areas is dominated by oxygenated species (e.g., Zhang et al, 2007;Duarte et al, 2007Duarte et al, , 2015Crilley et al, 2014;Lopes et al, 2015), and it contains both water-soluble and water-insoluble organic components. The water-soluble organic carbon (WSOC) fraction is usually below 70% of the organic carbon (OC) present in the air particulate matter (e.g., Duarte et al, 2007;Wozniak et al, 2012;Zhang et al, 2014;Lopes et al, 2015).…”

Section: Introductionmentioning

confidence: 99%

“…In the quest for untangle the complex molecular composition of the water-soluble component of OA, it has been shown that the WSOC consists of a highly diverse suite of oxygenated compounds, including dicarboxylic acids, keto-carboxylic acids, aliphatic aldehydes and alcohols, saccharides, saccharide anhydrides, aromatic acids, phenols, but also amines, amino acids, organic nitrates, and organic sulfates (e.g., Duarte et al, 2007Duarte et al, , 2008Duarte et al, , 2015Timonen et al, 2013;Ng et al, 2010;Cleveland et al, 2012;Shakya et al, 2012;Pietrogrande et al, 2013;Chalbot et al, 2014;Paglione et al, 2014;Lopes et al, 2015;Chalbot et al, 2016). A common ground of the available compositional datasets on aerosol WSOC is that they refer to studies carried out in urban, rural, and remote locations predominantly at North America and Europe, besides a few urban sites in Asia.…”

Section: Introductionmentioning

confidence: 99%

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Structural signatures of water-soluble organic aerosols in contrasting environments in South America and Western Europe

Duarte

Matos

Paula

et al. 2017

Environmental Pollution

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Section: Contribution Of Wsoc To Pm Massmentioning

confidence: 96%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Structural signatures of water-soluble organic aerosols in contrasting environments in South America and Western Europe

Duarte

Matos

Paula

et al. 2017

Environmental Pollution

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“…Carbon can be added to existing OM via oligomerization reactions, and the larger carbon chains present in the mixed and urban aerosols suggests that they have undergone oligomerization reactions more extensively than the marine and biomass burning aerosols. Protons that are more downfield in this region (1.4-1.8 ppm) are often attributed to an H-C group that is β to a carbon attached to heteroatoms (H-C-C-C-X, where X = N, S, or O) [14]. The presence of a large number of heteroatomic compounds identified in each of the mass spectra (CHON, CHOS, and CHONS) indicates some portion of the signal in this region represents these species as can be expected for OA and was noted previously (Section 3.2).…”

Section: H Nmr Analysismentioning

confidence: 99%

Detailed Source-Specific Molecular Composition of Ambient Aerosol Organic Matter Using Ultrahigh Resolution Mass Spectrometry and 1H NMR

2016

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Organic aerosols (OA) are universally regarded as an important component of the atmosphere that have far-ranging impacts on climate forcing and human health. Many of these impacts are related to OA molecular characteristics. Despite the acknowledged importance, current uncertainties related to the source apportionment of molecular properties and environmental impacts make it difficult to confidently predict the net impacts of OA. Here we evaluate the specific molecular compounds as well as bulk structural properties of total suspended particulates in ambient OA collected from key emission sources (marine, biomass burning, and urban) using ultrahigh resolution mass spectrometry (UHR-MS) and proton nuclear magnetic resonance spectroscopy ( 1 H NMR). UHR-MS and 1 H NMR show that OA within each source is structurally diverse, and the molecular characteristics are described in detail. Principal component analysis (PCA) revealed that (1) aromatic nitrogen species are distinguishing components for these biomass burning aerosols; (2) these urban aerosols are distinguished by having formulas with high O/C ratios and lesser aromatic and condensed aromatic formulas; and (3) these marine aerosols are distinguished by lipid-like compounds of likely marine biological origin. This study provides a unique qualitative approach for enhancing the chemical characterization of OA necessary for molecular source apportionment.

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“…They are key participants in the aqueous-phase chemistry of clouds and contribute to SOA formation through various reactions within the aqueous portion of the particle phase (Carlton et al, 2007;Ervens et al, 2004;Lim et al, 2010). Furthermore, since organic acids can be photochemical products, they can also serve as indicators of atmospheric transformation processes.…”

Section: Introductionmentioning

confidence: 99%

Understanding the primary emissions and secondary formation of gaseous organic acids in the oil sands region of Alberta, Canada

et al. 2017

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Abstract. Organic acids are known to be emitted from combustion processes and are key photochemical products of biogenic and anthropogenic precursors. Despite their multiple environmental impacts, such as on acid deposition and human-ecosystem health, little is known regarding their emission magnitudes or detailed chemical formation mechanisms. In the current work, airborne measurements of 18 gas-phase low-molecular-weight organic acids were made in the summer of 2013 over the oil sands region of Alberta, Canada, an area of intense unconventional oil extraction. The data from these measurements were used in conjunction with emission retrieval algorithms to derive the total and speciated primary organic acid emission rates, as well as secondary formation rates downwind of oil sands operations. The results of the analysis indicate that approximately 12 t day −1 of low-molecular-weight organic acids, dominated by C 1 -C 5 acids, were emitted directly from off-road diesel vehicles within open pit mines. Although there are no specific reporting requirements for primary organic acids, the measured emissions were similar in magnitude to primary oxygenated hydrocarbon emissions, for which there are reporting thresholds, measured previously (≈ 20 t day −1 ). Conversely, photochemical production of gaseous organic acids significantly exceeded the primary sources, with formation rates of up to ≈ 184 t day −1 downwind of the oil sands facilities. The formation and evolution of organic acids from a Lagrangian flight were modelled with a box model, incorporating a detailed hydrocarbon reaction mechanism extracted from the Master Chemical Mechanism (v3.3). Despite evidence of significant secondary organic acid formation, the explicit chemical box model largely underestimated their formation in the oil sands plumes, accounting for 39, 46, 26, and 23 % of the measured formic, acetic, acrylic, and propionic acids respectively and with little contributions from biogenic VOC precursors. The model results, together with an examination of the carbon mass balance between the organic acids formed and the primary VOCs emitted from oil sands operations, suggest the existence of significant missing secondary sources and precursor emissions related to oil sands and/or an incomplete mechanistic and quantitative understanding of how they are processed in the atmosphere.

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Investigating the water-soluble organic functionality of urban aerosols using two-dimensional correlation of solid-state 13C NMR and FTIR spectral data

Cited by 45 publications

References 40 publications

Structural signatures of water-soluble organic aerosols in contrasting environments in South America and Western Europe

Structural signatures of water-soluble organic aerosols in contrasting environments in South America and Western Europe

Detailed Source-Specific Molecular Composition of Ambient Aerosol Organic Matter Using Ultrahigh Resolution Mass Spectrometry and 1H NMR

Understanding the primary emissions and secondary formation of gaseous organic acids in the oil sands region of Alberta, Canada

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