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Duarte, R. Water-Soluble Organic Aerosols. Encyclopedia. Available online: https://encyclopedia.pub/entry/8112 (accessed on 01 July 2024).
Duarte R. Water-Soluble Organic Aerosols. Encyclopedia. Available at: https://encyclopedia.pub/entry/8112. Accessed July 01, 2024.
Duarte, Regina. "Water-Soluble Organic Aerosols" Encyclopedia, https://encyclopedia.pub/entry/8112 (accessed July 01, 2024).
Duarte, R. (2021, March 18). Water-Soluble Organic Aerosols. In Encyclopedia. https://encyclopedia.pub/entry/8112
Duarte, Regina. "Water-Soluble Organic Aerosols." Encyclopedia. Web. 18 March, 2021.
Water-Soluble Organic Aerosols
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This entry is adapted from the peer-reviewed paper 10.3390/app11062539

Water-soluble organic aerosols (OA) are an important component of atmospheric particulate matter and one of the key drivers that impact both climate and human health. Understanding these processes involving water-soluble OA depends on how well the chemical composition of this aerosol component is decoded. Yet, obtaining such a detailed chemical information faces several challenges, of which the complexity of the sample matrix is one of the most demanding issues. A number of different advanced multidimensional analytical techniques are available today with the potential to tackel the complex chemical nature of water-soluble OA, allowing the untargeted profilling of new chemical structures without the need for use of databases or libraries. This critical review is aimed at nonspecialists who are interested in learning more about the potential and impact of such multidimensional non-targeted analytical strategies in water-soluble OA research.

organic aerosols air particles water-soluble organic matter 2D NMR spectroscopy high-resolution mass spectrometry EEM fluorescence spectroscopy 2D chromatographic separation

1. Introduction

The study and characterization of atmospheric aerosols, as well as their effects on radiative climate forcing, atmospheric chemistry, air quality and visibility, and human health, are some of the most predominant research topics in atmospheric chemistry [1][2]. Atmospheric particulate matter (PM) can be directly emitted into the atmosphere (primary aerosols) from a diversity of natural and anthropogenic sources, including biomass burning, incomplete combustion of fossil fuels, volcanic eruptions, and wind-driven or traffic-related suspension of road, soil, and mineral dust, sea salt, and biological materials [1]. Nonetheless, atmospheric PM can also be formed in the atmosphere (secondary aerosols) through gas-to-particle conversion processes of gaseous species (i.e., nucleation, condensation, and heterogeneous and multiphase chemical reactions) [1][3]. Furthermore, primary and secondary aerosols may undergo chemical and physical transformations, being subjected to transport, cloud processing, and removal from the atmosphere [4]. This multitude of emission sources and formation/processing mechanisms contribute to the diversity and complexity of the chemical composition (i.e., carbonaceous and inorganic components) and physical properties (i.e., concentration, size distribution, and surface area) of atmospheric PM, which in turn influences climate and health effects, further adding a layer of complexity.

Although the composition of the inorganic aerosol component has been thoroughly described in the literature, in-depth knowledge of its organic counterpart is particularly more difficult to achieve due to the structural diversity and complexity of this aerosol component. The organic aerosols (OA) fraction can be the predominant component of suspended PM mass, accounting for ~20–50% of the total fine particulate mass at continental mid-latitudes and reach 90% in tropical forested areas [5][6]. The interest of the atmospheric research community on this OA component has been fueled by the realization that an important fraction of the OA is water-soluble. In Northern Hemisphere midlatitudes, the ubiquitous water-soluble organic matter (WSOM) represents 10% to 80% of the total particulate organics [7][8][9][10], whereas lower percentage values (up to 13%) have been reported for Southern Hemisphere locations [11]. The aerosol WSOM plays a key role in cloud formation and properties [12][13], Earth’s radiative balance [14][15], and atmospheric chemistry [14][16]. Atmospheric deposition of aerosol WSOM can also affect carbon and nitrogen biogeochemical cycles in aquatic ecosystems [17][18][19]. Aerosol WSOM in fine inhalable air particles may also exert adverse health effects by generating reactive oxygen and nitrogen species [20][21] or by promoting a moderate pro-inflammatory status [7]. Understanding these dynamic processes involving aerosol WSOM depends on how well one can identify its organic constituents.

2. Coping with Water-Soluble OA Complexity

As mentioned above, the water-soluble OA fraction covers a huge variety of molecular structures with different physicochemical properties and sources. Nevertheless, according to Nozière et al. [22], not all atmospheric issues require the identification of all organic compounds present in OA samples. Depending on the purpose of the investigation, different levels of organic compositional information can be distinguished [22][23]: (i) functional group analysis is typically employed when interested in understanding specific properties of OA (e.g., chemistry, optical properties or structural average parameters of OAs); (ii) resolve the chemical composition of OA into different organic components (e.g., hydrocarbon-like OA (HOA), oxidized OA (OOA), and biomass-burning OA (BBOA)) in real time is usually chosen for capturing the characteristic chemical and physical properties of OA in a rapidly changing environment; (iii) target analysis of molecular markers is typically used when monitoring known OA formation processes or sources; and (iv) identification of up to three specific organic compounds when studying unknown OA formation processes or sources. For over two decades, these different levels of OA analysis have been dedicated to the quantification and characterization of the aerosol WSOM component. These efforts have been accompanied by numerous laboratory and field studies focused on the characterization of WSOM sources, as well as its mechanisms of formation and rates of its atmospheric transformations. Currently, these issues are still poorly known, although the major sources of these compounds are considered to be biomass burning and secondary formation (involving both anthropogenic and biogenic volatile organic compounds). To further enhance the diversity and complexity of this OA fraction, the atmospheric WSOM and their precursor gases can also be modified in the atmosphere by oxidative processes and, thereby, becoming less volatile, more hygroscopic and, consequently, more water-soluble [24][25].

Several procedures and methodologies have been developed to study the chemical composition of the aerosol WSOM [8][9][10][11][26][27][28][29][30][31][32][33][34]. These studies are usually carried out using a combination of total organic carbon analysis, isolation and fractionation procedures, and characterization of molecular fragments and intermolecular bonds by different analytical techniques. Such studies have demonstrated that this fraction 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 [11][28][30][33][35][36][37][38][39][40][41][42]. Despite the advances in understanding the atmospheric importance of the aerosol WSOM component, there are still several fundamental questions related to the complexity of its chemical composition, mechanisms of formation, atmospheric fate, and reactivity [15][22]. Determining the molecular composition and structure of aerosol WSOM is warranted to further increase the current understanding of its role in various atmospheric processes. Furthermore, due to its dynamic nature, the establishment of general models for the structure of the water-soluble fraction of OA still is far from being fully accomplished [26], and further studies are needed to understand their actual impact on a regional and global scale. As reviewed by Nozière et al. [22] and Duarte and Duarte [43], a universal technique for OA analysis does not exist. Several different offline and online analytical methodologies have been developed and applied to mitigate the complexity of OA, as well as to unravel the structure and composition of this aerosol component. Analytical strategies combining one- or two-dimensional chromatographic separation and a detector (e.g., diode array, fluorescence, nuclear magnetic resonance (NMR), or mass spectrometry (MS)) or involving two or more stages of MS (i.e., tandem MS) or frequency (i.e., NMR spectroscopy) or wavelength (i.e., excitation–emission matrix (EEM) fluorescence spectroscopy) dimensions are here defined as multidimensional.

References

  1. Pöschl, U. Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects. Angew. Chem. Int. Ed. 2005, 44, 7520–7540.
  2. Heal, M.R.; Kumar, P.; Harrison, R.M. Particles, air quality, policy and health. Chem. Soc. Rev. 2012, 41, 6606.
  3. Hallquist, M.; Wenger, J.C.; Baltensperger, U.; Rudich, Y.; Simpson, D.; Claeys, M.; Dommen, J.; Donahue, N.M.; George, C.; Goldstein, A.H.; et al. The formation, properties and impact of secondary organic aerosol: Current and emerging issues. Atmos. Chem. Phys. 2009, 9, 5155–5236.
  4. Zhang, R.; Wang, G.; Guo, S.; Zamora, M.L.; Ying, Q.; Lin, Y.; Wang, W.; Hu, M.; Wang, Y. Formation of Urban Fine Particulate Matter. Chem. Rev. 2015, 115, 3803–3855.
  5. Kanakidou, M.; Seinfeld, J.H.; Pandis, S.N.; Barnes, I.; Dentener, F.J.; Facchini, M.C.; Van Dingenen, R.; Ervens, B.; Nenes, A.; Nielsen, C.J.; et al. Organic aerosol and global climate modelling: A review. Atmos. Chem. Phys. 2005, 5, 1053–1123.
  6. Jimenez, J.L.; Canagaratna, M.R.; Donahue, N.M.; Prevot, A.S.H.; Zhang, Q.; Kroll, J.H.; DeCarlo, P.F.; Allan, J.D.; Coe, H.; Ng, N.L.; et al. Evolution of Organic Aerosols in the Atmosphere. Science 2009, 326, 1525–1529.
  7. Almeida, A.S.; Ferreira, R.M.P.; Silva, A.M.S.; Duarte, A.C.; Neves, B.M.; Duarte, R.M.B.O. Structural Features and Pro-Inflammatory Effects of Water-Soluble Organic Matter in Inhalable Fine Urban Air Particles. Environ. Sci. Technol. 2020, 54, 1082–1091.
  8. Lopes, S.P.; Matos, J.T.V.; Silva, A.M.S.; Duarte, A.C.; Duarte, R.M.B.O. 1 H NMR studies of water- and alkaline-soluble organic matter from fine urban atmospheric aerosols. Atmos. Environ. 2015, 119, 374–380.
  9. Duarte, R.M.B.O.; Freire, S.M.S.C.; Duarte, A.C. Investigating the water-soluble organic functionality of urban aerosols using two-dimensional correlation of solid-state 13C NMR and FTIR spectral data. Atmos. Environ. 2015, 116, 245–252.
  10. Duarte, R.M.B.O.; Piñeiro-Iglesias, M.; López-Mahía, P.; Muniategui-Lorenzo, S.; Moreda-Piñeiro, J.; Silva, A.M.S.; Duarte, A.C. Comparative study of atmospheric water-soluble organic aerosols composition in contrasting suburban environments in the Iberian Peninsula Coast. Sci. Total Environ. 2019, 648, 430–441.
  11. Duarte, R.M.B.O.; Matos, J.T.V.; Paula, A.S.; Lopes, S.P.; Pereira, G.; Vasconcellos, P.; Gioda, A.; Carreira, R.; Silva, A.M.S.; Duarte, A.C.; et al. Structural signatures of water-soluble organic aerosols in contrasting environments in South America and Western Europe. Environ. Pollut. 2017, 227, 513–525.
  12. Padró, L.T.; Tkacik, D.; Lathem, T.; Hennigan, C.J.; Sullivan, A.P.; Weber, R.J.; Huey, L.G.; Nenes, A. Investigation of cloud condensation nuclei properties and droplet growth kinetics of the water-soluble aerosol fraction in Mexico City. J. Geophys. Res. 2010, 115, D09204.
  13. Müller, A.; Miyazaki, Y.; Tachibana, E.; Kawamura, K.; Hiura, T. Evidence of a reduction in cloud condensation nuclei activity of water-soluble aerosols caused by biogenic emissions in a coolerate forest. Sci. Rep. 2017, 7, 1–9.
  14. Laskin, A.; Laskin, J.; Nizkorodov, S.A. Chemistry of Atmospheric Brown Carbon. Chem. Rev. 2015, 115, 4335–4382.
  15. Moise, T.; Flores, J.M.; Rudich, Y. Optical Properties of Secondary Organic Aerosols and Their Changes by Chemical Processes. Chem. Rev. 2015, 115, 4400–4439.
  16. George, C.; Ammann, M.; D’Anna, B.; Donaldson, D.J.; Nizkorodov, S.A. Heterogeneous photochemistry in the atmosphere. Chem. Rev. 2015, 115, 4218–4258.
  17. Iavorivska, L.; Boyer, E.W.; De Walle, D.R. Atmospheric deposition of organic carbon via precipitation. Atmos. Environ. 2016, 146, 153–163.
  18. Witkowska, A.; Lewandowska, A.; Falkowska, L.M. Parallel measurements of organic and elemental carbon dry (PM1, PM2.5) and wet (rain, snow, mixed) deposition into the Baltic Sea. Mar. Pollut. Bull. 2016, 104, 303–312.
  19. Bao, H.; Niggemann, J.; Luo, L.; Dittmar, T.; Kao, S.J. Aerosols as a source of dissolved black carbon to the ocean. Nat. Commun. 2017, 8.
  20. Verma, V.; Fang, T.; Xu, L.; Peltier, R.E.; Russell, A.G.; Ng, N.L.; Weber, R.J. Organic aerosols associated with the generation of reactive oxygen species (ROS) by water-soluble PM2.5. Environ. Sci. Technol. 2015, 49, 4646–4656.
  21. Samara, C. On the redox activity of urban aerosol particles: Implications for size distribution and relationships with organic aerosol components. Atmosphere 2017, 8, 205.
  22. Nozière, B.; Kalberer, M.; Claeys, M.; Allan, J.; D’Anna, B.; Decesari, S.; Finessi, E.; Glasius, M.; Grgić, I.; Hamilton, J.F.; et al. The molecular identification of organic compounds in the atmosphere: State of the art and challenges. Chem. Rev. 2015, 115, 3919–3983.
  23. Duarte, R.M.B.O.; Duarte, A.C. NMR Studies of Organic Aerosols. In Annual Reports on NMR Spectroscopy; Webb, G.A., Ed.; Academic Press: Oxford, UK, 2017; Volume 92, pp. 83–135. ISBN 978-0-12-812084-2.
  24. Maksymiuk, C.S.; Gayahtri, C.; Gil, R.R.; Donahue, N.M. Secondary organic aerosol formation from multiphase oxidation of limonene by ozone: Mechanistic constraints via two-dimensional heteronuclear NMR spectroscopy. Phys. Chem. Chem. Phys. 2009, 11, 7810–7818.
  25. Brege, M.; Paglione, M.; Gilardoni, S.; Decesari, S.; Cristina Facchini, M.; Mazzoleni, L.R. Molecular insights on aging and aqueous-phase processing from ambient biomass burning emissions-influenced Po Valley fog and aerosol. Atmos. Chem. Phys. 2018, 18, 13197–13214.
  26. Duarte, R.M.B.O.; Duan, P.; Mao, J.; Chu, W.; Duarte, A.C.; Schmidt-Rohr, K. Exploring water-soluble organic aerosols structures in urban atmosphere using advanced solid-state 13C NMR spectroscopy. Atmos. Environ. 2020, 230, 117503.
  27. Matos, J.T.V.; Freire, S.M.S.C.; Duarte, R.M.B.O.; Duarte, A.C. Profiling water-soluble organic matter from urban aerosols using comprehensive two-dimensional liquid chromatography. Aerosol Sci. Technol. 2015, 49.
  28. Matos, J.T.V.; Duarte, R.M.B.O.; Lopes, S.P.; Silva, A.M.S.; Duarte, A.C. Persistence of urban organic aerosols composition: Decoding their structural complexity and seasonal variability. Environ. Pollut. 2017, 231, 281–290.
  29. Willoughby, A.S.; Wozniak, A.S.; Hatcher, P.G. Detailed source-specific molecular composition of ambient aerosol organic matter using ultrahigh resolution mass spectrometry and 1H NMR. Atmosphere 2016, 7, 79.
  30. Duarte, R.M.B.O.; Santos, E.B.H.; Pio, C.A.; Duarte, A.C. Comparison of structural features of water-soluble organic matter from atmospheric aerosols with those of aquatic humic substances. Atmos. Environ. 2007, 41, 8100–8113.
  31. Sannigrahi, P.; Sullivan, A.P.; Weber, R.J.; Ingall, E.D. Characterization of water-soluble organic carbon in urban atmospheric aerosols using solid-state C-13 NMR spectroscopy. Environ. Sci. Technol. 2006, 40, 666–672.
  32. Decesari, S.; Mircea, M.; Cavalli, F.; Fuzzi, S.; Moretti, F.; Tagliavini, E.; Facchini, M.C. Source Attribution of Water-Soluble Organic Aerosol by Nuclear Magnetic Resonance Spectroscopy. Environ. Sci. Technol. 2007, 41, 2479–2484.
  33. Duarte, R.M.B.O.; Silva, A.M.S.; Duarte, A.C. Two-Dimensional NMR Studies of Water-Soluble Organic Matter in Atmospheric Aerosols. Environ. Sci. Technol. 2008, 42, 8224–8230.
  34. Matos, J.T.V.; Freire, S.M.S.C.; Duarte, R.M.B.O.; Duarte, A.C. Natural organic matter in urban aerosols: Comparison between water and alkaline soluble components using excitation–emission matrix fluorescence spectroscopy and multiway data analysis. Atmos. Environ. 2015, 102, 1–10.
  35. Paglione, M.; Saarikoski, S.; Carbone, S.; Hillamo, R.; Facchini, M.C.; Finessi, E.; Giulianelli, L.; Carbone, C.; Fuzzi, S.; Moretti, F.; et al. Primary and secondary biomass burning aerosols determined by proton nuclear magnetic resonance (1H-NMR) spectroscopy during the 2008 EUCAARI campaign in the Po Valley (Italy). Atmos. Chem. Phys. 2014, 14, 5089–5110.
  36. Wozniak, A.S.; Willoughby, A.S.; Gurganus, S.C.; Hatcher, P.G. Distinguishing molecular characteristics of aerosol water soluble organic matter from the 2011 trans-North Atlantic US GEOTRACES cruise. Atmos. Chem. Phys. 2014, 14, 8419–8434.
  37. Ng, N.L.; Canagaratna, M.R.; Zhang, Q.; Jimenez, J.L.; Tian, J.; Ulbrich, I.M.; Kroll, J.H.; Docherty, K.S.; Chhabra, P.S.; Bahreini, R.; et al. Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry. Atmos. Chem. Phys. 2010, 10, 4625–4641.
  38. Cleveland, M.J.; Ziemba, L.D.; Griffin, R.J.; Dibb, J.E.; Anderson, C.H.; Lefer, B.; Rappenglück, B. Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy. Atmos. Environ. 2012, 54, 511–518.
  39. Shakya, K.M.; Place, P.F.; Griffin, R.J.; Talbot, R.W. Carbonaceous content and water-soluble organic functionality of atmospheric aerosols at a semi-rural New England location. J. Geophys. Res. Atmos. 2012, 117, 1–13.
  40. Timonen, H.; Carbone, S.; Aurela, M.; Saarnio, K.; Saarikoski, S.; Ng, N.L.; Canagaratna, M.R.; Kulmala, M.; Kerminen, V.-M.; Worsnop, D.R.; et al. Characteristics, sources and water-solubility of ambient submicron organic aerosol in springtime in Helsinki, Finland. J. Aerosol Sci. 2013, 56, 61–77.
  41. Chalbot, M.-C.G.; Brown, J.; Chitranshi, P.; Gamboa da Costa, G.; Pollock, E.D.; Kavouras, I.G. Functional characterization of the water-soluble organic carbon of size-fractionated aerosol in the southern Mississippi Valley. Atmos. Chem. Phys. 2014, 14, 6075–6088.
  42. Willoughby, A.S.; Wozniak, A.S.; Hatcher, P.G. A molecular-level approach for characterizing water-insoluble components of ambient organic aerosol particulates using ultrahigh-resolution mass spectrometry. Atmos. Chem. Phys. 2014, 14, 10299–10314.
  43. Duarte, R.M.B.O.; Duarte, A.C. A critical review of advanced analytical techniques for water-soluble organic matter from atmospheric aerosols. TrAC Trends Anal. Chem. 2011, 30, 1659–1671.
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