Analysis of Organic Anionic Surfactants in Fine and Coarse Fractions of Freshly Emitted Sea Spray Aerosol

Cochran, Richard E.; Laskina, Olga; Jayarathne, Thilina; Laskin, Alexander; Laskin, Julia; Lin, Peng; Sultana, Camille M.; Lee, Christopher; Moore, Kathryn A.; Cappa, Christopher D.; Bertram, Timothy H.; Prather, Kimberly A.; Grassian, Vicki H.; Stone, Elizabeth A.

doi:10.1021/acs.est.5b04053

Cited by 160 publications

(267 citation statements)

References 67 publications

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“…The dicarboxylic acids were chosen due to their abundance in SSA as well as fundamental importance in their tendency to be surface-active, although less than monocarboxylic acids. 21,26,27,32−34 In general, surface-active chemical species Figure 3. This is due to the preferential molecular partitioning up to the air−droplet interface.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…20 In this study, we extend the chemical systems that cover a wide range of viscosities and RH range to improve our understanding of surface tension of SSA-relevant particles that contain both single-and multicomponent systems, chosen due to relevance to the atmosphere and importance as fundamental model systems. 21 By extending the experimental range of surface tension measurements, these data provide significant insight toward the development of accurate models by providing much-needed direct surface tension measurements of various chemical systems, but on a single particle basis. 22 To further validate our methodology, we made comparisons of single particle surface tension versus RH to bulk surface tension versus solute mole percentage, by also using a force tensiometer to perform bulk solution surface tension measurements of the same chemical system.…”

Section: ■ Introductionmentioning

confidence: 99%

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Direct Surface Tension Measurements of Individual Sub-Micrometer Particles Using Atomic Force Microscopy

Lee

Estillore²,

Morris

et al. 2017

J. Phys. Chem. A

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Understanding the role of sea spray aerosol (SSA) on climate and the environment is of great interest due to their high number concentration throughout the Earth's atmosphere. Despite being of fundamental importance, direct surface tension measurements of SSA relevant sub-micrometer particles are rare, largely due to their extremely small volumes. Herein, atomic force microscopy (AFM) is used to directly measure the surface tension of individual sub-micrometer SSA particle mimics at ambient temperature and varying relative humidity (RH). Specifically, we probed both atmospherically relevant and fundamentally important model systems including electrolyte salts, dicarboxylic acids, and saccharides as single components and mixtures. Our results show that the single particle surface tension depends on RH or solute mole percentage and chemical composition. Moreover, for liquid droplets at and below 100 Pa s in viscosity, or at corresponding RH, we show good agreement between the AFM single particle and the bulk solution surface tension measurements at overlapping concentration ranges. Thus, direct surface tension measurements of individual particles using AFM is shown over a wide range of chemical systems as a function of RH, solute mole percentage, and viscosity than previously reported.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Direct Surface Tension Measurements of Individual Sub-Micrometer Particles Using Atomic Force Microscopy

Lee

Estillore²,

Morris

et al. 2017

J. Phys. Chem. A

Self Cite

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“…Subsequent enzymatic digestion then leads to formation of saturated and unsaturated fatty acids. 29,48,49 In addition, longer-chain fatty acids can further decompose to short chain fatty acid derivatives. 50, 51 Moreover, fatty acids are also known components of the EPS matrix 15 surrounding the cells in biofilms.…”

Section: Resultsmentioning

confidence: 99%

“…Therefore, compounds with higher O/C ratios, such as saccharides, probably gave little to no signal intensity in the acquired mass spectra despite high concentrations in the EPS matrix as they are known to exhibit a poor ionization efficiency. 17,18,29,55 Therefore, changes in the abundance of such compounds due to 5 photochemistry cannot be discussed here.…”

Section: Resultsmentioning

confidence: 99%

Interfacial photochemistry of biogenic surfactants: a major source of abiotic volatile organic compounds

et al. 2017

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15Films of biogenic compounds exposed to the atmosphere are ubiquitously found on surfaces of cloud droplets, aerosol particles, buildings, plants, soils, and the ocean. These air/water interfaces host countless amphiphilic compounds concentrated there with respect to bulk water, leading to a unique chemical environment. Here, photochemical processes at the air/water interface of biofilmcontaining solutions were studied, demonstrating abiotic VOC production from authentic biogenic 20 surfactants under ambient conditions. Using a combination of online-APCI-HRMS and PTR-ToF-MS, unsaturated and functionalized VOCs were identified and quantified, giving emission fluxes comparable to previous field and laboratory observations. Interestingly, VOC fluxes increased with the decay of microbial cells in the samples, indicating that cell lysis due to cell death was the main source for surfactants, and VOC production. In particular, irradiation of samples containing solely 25 biofilm cells without matrix components exhibited the strongest VOC production upon irradiation. In agreement with previous studies, LC-MS measurements of the liquid phase suggested the presence of fatty acids and known photosensitizers, possibly inducing the observed VOC production via peroxy-radical chemistry. Up to now such VOC emissions were directly accounted to high biological activity in surface waters. However, the obtained results suggest that abiotic photochemistry can 30 lead to similar emissions into the atmosphere, especially in less biologically-active regions.Furthermore, chamber experiments suggested that oxidation (O 3 /OH-radicals) of the photochemically-produced VOCs leads to aerosol formation and growth, possibly affecting 2 atmospheric chemistry and climate-related processes, such as cloud formation or the Earth's radiation budget. 3 IntroductionAir/water interfaces are omnipresent in the ambient atmosphere, reaching from the nm-scale for single aerosol particles to the surface of the ocean, which covers more than 70% of the Earth's surface. In the past, it was shown that unique photochemical reactions with significant implications for atmospheric processes can occur at such interfaces, leading to the formation of volatile organic 5 compounds (VOCs) 1-5 and secondary organic aerosols, 6 or acting as sinks for reactive species, such as NO 2 or ozone. [7][8][9][10] This interfacial photochemistry is exclusively due to the presence of surfactants which tend to concentrate in surface layers with respect to the underlying bulk water. Additionally, such surfactants also increase the propensity of less surface-active compounds to enrich there as well, creating a unique chemical environment, affecting not only chemistry but also trace-gas 10 exchange. 5,[10][11][12][13][14][15][16] A major source of biogenic surfactants in the ambient environment are so-called biofilms, loosely defined as a population of microorganisms (i.e., fungi, algae, archaea) that accumulate at an interface. In addition, such microorganisms can also form cel...

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“…Phospholipids, glycolipids and triacylglycerides are mainly released during cell lysis of the phytoplankton. [13,14] Coastal and oligotrophic slicks are typically rich in these and other lipids. [12] There is evidence to show that naturally derived surfactants, such as fatty acids and their derivatives, may accumulate in the sea surface microlayer, showing a greater affinity than other soluble organic molecules for the air-water interface.…”

Section: Introductionmentioning

confidence: 99%

Impact of anions on the surface organisation of lipid monolayers at the air–water interface

Wang

2017

Environ. Chem.

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Environmental context. Lipids released from lysis of phytoplankton cells are enriched in the sea surface microlayer. Such surface-active organics can be transferred through bursting bubbles to sea-spray aerosols where they can influence atmospheric chemistry. The results presented here suggest that phospholipids combine more readily with SO 4 2À than with Br À , leading to enrichment of organic-coated sulfate salts in marine aerosols.Abstract. Inorganic salts and organic matter are known to be present at higher levels in the sea surface microlayer and marine aerosols; however, the impact of common anions on their surface properties is not well understood. Here, a 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) monolayer was enriched with the sodium and ammonium salts of different anions (Br À , Cl À , NO 3 À , SO 4 2À , CH 3 COO À , and HCO 3 À ), and the effects on the surface properties of the monolayer were investigated. The monolayer phase behaviour and the structure of the lipid phases were studied by surface pressure-area (p-A) isotherms and infrared reflection-absorption spectroscopy (IRRAS). The presence of salts in the subphase was found to increase the surface pressure of the DPPC monolayer at a fixed area per molecule. The effect of the anions follows the order of the Hofmeister series. The higher concentration of salt solution caused the p-A isotherm to shift to larger area. The IRRAS spectra demonstrate that the ordering of the DPPC molecules in the liquid condensed phase remains essentially unaffected, even at higher electrolyte concentrations. DPPC molecules combined with SO 4 2À could be transferred from the ocean to sea spray aerosol. The present study finds that the anions have significant influence on the surface organisation and, consequently, the interfacial properties, of the surface-active species at the air-water interface, a finding that has further implications for atmospheric aerosol nucleation.

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Analysis of Organic Anionic Surfactants in Fine and Coarse Fractions of Freshly Emitted Sea Spray Aerosol

Cited by 160 publications

References 67 publications

Direct Surface Tension Measurements of Individual Sub-Micrometer Particles Using Atomic Force Microscopy

Direct Surface Tension Measurements of Individual Sub-Micrometer Particles Using Atomic Force Microscopy

Interfacial photochemistry of biogenic surfactants: a major source of abiotic volatile organic compounds

Impact of anions on the surface organisation of lipid monolayers at the air–water interface

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