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Mixed Micelles of Fluorinated and Hydrogenated Surfactants
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Physical Chemistry.
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Physical Chemistry.ORCID iD: 0000-0002-0231-3970
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Physical Chemistry.
2006 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 128, no 20, 6704-6712 p.Article in journal (Refereed) Published
Abstract [en]

The model mixed surfactant system of sodium perfluorooctanoate and sodium decyl sulfate was carefully reexamined by a combination of nuclear magnetic resonance methods. Over a wide range of sample compositions, detailed F-19 and H-1 chemical shift data in combination with self-diffusion coefficients for the perfluorooctanoate and decyl sulfate ions are collected. All data are analyzed together in a framework that uses a minimal number of initial assumptions to extract the monomer concentrations of both surfactants and the micellar chemical shifts of F-19 and H-1 as a function of relative concentration. The main conclusion drawn from this analysis is that there exists neither complete demixing nor complete mixing on molecular or micellar levels. Instead, the experimental data favor a single type of micelles within which fluorinated surfactants are preferentially coordinated by fluorinated ones and hydrogenated surfactants by hydrogenated ones. The data are quantitatively interpreted in the framework of the first approximation of the regular solution theory (also called the quasi-chemical treatment) leading to an energy of mixing of omega = W/kT = 0.98 between the constituting surfactant types. These findings may help to resolve a long controversy about micellar mixing-demixing in this particular mixture and in its relatives.

Place, publisher, year, edition, pages
2006. Vol. 128, no 20, 6704-6712 p.
Keyword [en]
Angle neutron-scattering, self-diffusion measurements, nuclear magnetic-resonance, order-parameter profile, sodium perfluorooctanoate, hydrocarbon surfactants, aggregation number, aqueous-solutions, chemical-shifts, fluorocarbon surfactants
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-5687DOI: 10.1021/ja061029rISI: 000237590500045Scopus ID: 2-s2.0-33646721758OAI: oai:DiVA.org:kth-5687DiVA: diva2:10134
Note
QC 20100914Available from: 2006-05-10 Created: 2006-05-10 Last updated: 2017-12-14Bibliographically approved
In thesis
1. Molecular Association Studied by NMR Spectroscopy
Open this publication in new window or tab >>Molecular Association Studied by NMR Spectroscopy
2006 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

This Thesis presents studies of molecular association in aqueous solution and at the liquid/solid interface. The investigated molecular systems range from self-aggregating surfactants to hydration water in contact with micelles or individual molecules. In most studies, combinations of various NMR methods were applied. These vary from simple chemical shift and intensity measurements to more elaborate self-diffusion and intermolecular cross-relaxation experiments.

Non-ideal mixed micelles of fluorinated and hydrogenated surfactants were studied by an experimental procedure that allows an analysis in terms of micellar structure, using a minimal number of initial assumptions. Quantitative conclusions about micro-phase separation within mixed micelles were obtained within the framework of the regular solution theory. Additionally, NMR was introduced and developed as a powerful method for studying adsorption of surfactants at solid interfaces. Adsorption isotherms for pure and mixed surfactant systems and non-ideal mixing behavior of fluorinated and hydrogenated surfactants at solid surfaces were quantified. Fluorosurfactant-protein association was investigated using the methods described.

Intermolecular cross-relaxation rates between solute and solvent molecules were recorded at several different magnetic fields. The results reveal strong frequency dependence for both small molecules and micelles. This finding demonstrates that intermolecular cross-relaxation is not solely controlled by fast local motions, but also by long-range translational dynamics. Data analysis in terms of recently developed relaxation models provides information about the hydrophobic hydration and micellar structure.

Place, publisher, year, edition, pages
Stockholm: KTH, 2006. 52 p.
Series
Trita-FYK, 0602
Keyword
NMR, spin relaxation, self-diffusion, intermolecular cross-relaxation, chemical shift, fluorinated surfactants, hydrogenated surfactant, micelle, non-ideal mixing, adsorption, hydration, surfactant-protein association
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-3947 (URN)91-7178-345 8 (ISBN)
Public defence
2006-05-19, F3, Lindstedtsv. 26, Stockholm, 10:00
Opponent
Supervisors
Note
QC 20100914Available from: 2006-05-10 Created: 2006-05-10 Last updated: 2010-09-14Bibliographically approved

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Furó, István

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