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Surface Partitioning in Organic-Inorganic Mixtures Contributes to the Size-Dependence of the Phase-State of Atmospheric Nanoparticles
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics. Swedish University for Agricultural Sciences, Department of Chemistry and Biotechnology. (Molecular and Condensed Matter Physics)
Stockholm Univ, Dept Environm Sci & Analyt Chem ACES, SE-10691 Stockholm, Sweden;Stockholm Univ, Bolin Ctr Climate Res, SE-10691 Stockholm, Sweden.
Uppsala University, Disciplinary Domain of Science and Technology, Biology, Department of Cell and Molecular Biology, Computational Biology and Bioinformatics. Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics. (Molecular and Condensed Matter Physics)
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics. (Molecular and Condensed Matter Physics)
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2016 (English)In: Environmental Science & Technology, ISSN 0013-936X, Vol. 50, no 14, 7434-7442 p.Article in journal (Refereed) Published
Abstract [en]

Atmospheric particulate matter is one of the main factors governing the Earth's radiative budget, but its exact effects on the global climate are still uncertain. Knowledge on the molecular-scale surface phenomena as well as interactions between atmospheric organic and inorganic compounds is necessary for understanding the role of airborne nanoparticles in the Earth system. In this work, surface composition of aqueous model systems containing succinic acid and sodium chloride or ammonium sulfate is determined using a novel approach combining X-ray photoelectron spectroscopy, surface tension measurements and thermodynamic modeling. It is shown that succinic acid molecules are accumulated in the surface, yielding a 10-fold surface concentration as compared with the bulk for saturated succinic acid solutions. Inorganic salts further enhance this enrichment due to competition for hydration in the bulk. The surface compositions for various mixtures are parametrized to yield generalizable results and used to explain changes in surface tension. The enhanced surface partitioning implies an increased maximum solubility of organic compounds in atmospheric nanoparticles. The results can explain observations of size-dependent phase-state of atmospheric nanoparticles, suggesting that these particles can display drastically different behavior than predicted by bulk properties only.

Place, publisher, year, edition, pages
2016. Vol. 50, no 14, 7434-7442 p.
National Category
Atom and Molecular Physics and Optics Physical Chemistry Meteorology and Atmospheric Sciences
Identifiers
URN: urn:nbn:se:uu:diva-265223DOI: 10.1021/acs.est.6b00789ISI: 000380295700019PubMedID: 27326704OAI: oai:DiVA.org:uu-265223DiVA: diva2:865678
Funder
Swedish Research CouncilSwedish Foundation for Strategic Research Carl Tryggers foundation EU, European Research Council, ERC-StG-27882 ATMOGAIN
Available from: 2015-10-29 Created: 2015-10-26 Last updated: 2016-09-13Bibliographically approved
In thesis
1. Exploring the Surface of Aqueous Solutions: X-ray photoelectron spectroscopy studies using a liquid micro-jet
Open this publication in new window or tab >>Exploring the Surface of Aqueous Solutions: X-ray photoelectron spectroscopy studies using a liquid micro-jet
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The surface behavior of biologically or atmospherically relevant chemical compounds in aqueous solution has been studied using surface-sensitive X-ray photoelectron spectroscopy (XPS). The aim is to provide information on the molecular-scale composition and distribution of solutes in the surface region of aqueous solutions. In the first part, the distribution of solutes in the surface region is discussed, where in particular single molecular species are studied. Concentration-dependent studies on succinic acid and various alkyl-alcohols, where also parameters such as pH and branching are varied, are analyzed using different approaches that allow the quantification of surface concentrations. Furthermore, due to the sensitivity of XPS to the chemical state, reorientation of linear and branched alkyl-alcohols at the aqueous surface as a function of concentration is observed. The results are further discussed in terms of hydrophilic and hydrophobic interactions in the interfacial region, where the three-dimensional hydrogen bonded water structure terminates. In the second part, mixed solutions of compounds, both ionic and molecular, are inspected. Again concentration, but also co-dissolution of other chemical compounds, are varied and differences in the spatial distribution and composition of the surface region are discussed. It is found that the guanidinium ion has an increased propensity to reside at the surface, which is explained by strong hydration in only two dimensions and only weak interactions between the aromatic π-system and water. Ammonium ions, on the other hand, which require hydration in three dimensions, are depleted from the surface region. The presence of strongly hydrated electrolytes out-competes neutral molecules for hydrating water molecules leading to an enhanced abundance of molecules, such as succinic acid, in the interfacial region. The partitioning is quantified and discussed in the context of atmospheric science, where the impact of the presented results on organic loading of aerosol particles is emphasized.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2015. 88 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1313
Keyword
X-ray Photoelectron spectroscopy, liquid micro-jet, air-water interface, inorganic salt, carboxylic acid, alcohol, isomers, hydration.
National Category
Atom and Molecular Physics and Optics Condensed Matter Physics Chemical Sciences
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-265210 (URN)978-91-554-9399-8 (ISBN)
Public defence
2015-12-18, Häggsalen, Ångströmslaboratoriet, Lägerhyddsvägen 1, Uppsala, 10:15 (English)
Opponent
Supervisors
Available from: 2015-11-27 Created: 2015-10-25 Last updated: 2016-01-13

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Werner, Josephina

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