How to explain microemulsions formed by solvent mixtures without conventional surfactants
Identifieur interne : 000493 ( Pmc/Curation ); précédent : 000492; suivant : 000494How to explain microemulsions formed by solvent mixtures without conventional surfactants
Auteurs : Thomas N. Zemb [France] ; Michael Klossek [Allemagne] ; Tobias Lopian [France, Allemagne] ; Julien Marcus [Allemagne] ; Sebastian Schöettl [Allemagne] ; Dominik Horinek [Allemagne] ; Sylvain F. Prevost [France] ; Didier Touraud [Allemagne] ; Olivier Diat [France] ; Stjepan Mar Elja [Australie] ; Werner Kunz [France, Allemagne]Source :
- Proceedings of the National Academy of Sciences of the United States of America [ 0027-8424 ] ; 2016.
Abstract
Beginning over 40 y ago, a curious type of microemulsions—as transparent dispersion of two immiscible liquids separated by an interfacial film—at thermodynamic equilibrium has been described as “pre-Ouzo,” “detergentless,” or surfactant-free microemulsions. The experiments in ternary systems containing one hydrotropic cosolvent were ambiguous, and therefore, there was no need to come up with a general theory. Recent evidence obtained by specific deuteration in neutron scattering established the need for the extension of self-assembly theories based on Derjaguin-Landau-Verwey-Overbeck theory (DLVO), bending, or phase transfer energy. Here, we introduce a general free energy expression for weak self-assembly, where solvation effects and entropy compete without the influence of film bending, that explains all experimental results for this class of microemulsions.
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DOI: 10.1073/pnas.1515708113
PubMed: 27044068
PubMed Central: 4843454
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Zemb</name><affiliation wicri:level="1"><nlm:aff id="aff1"><institution>ICSM (Institut de Chimie Séparative de Marcoule), UMR 5257 (Commissariat a l’energie atomique et aux energies alternatives/CNRS/Ecole Nationale Supérieure de Chimie de Montpellier, Université de Montpellier), 30207 Bagnols sur Cèze</institution>,<country>France</country>;</nlm:aff><country xml:lang="fr">France</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Klossek, Michael" sort="Klossek, Michael" uniqKey="Klossek M" first="Michael" last="Klossek">Michael Klossek</name><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Lopian, Tobias" sort="Lopian, Tobias" uniqKey="Lopian T" first="Tobias" last="Lopian">Tobias Lopian</name><affiliation wicri:level="1"><nlm:aff id="aff1"><institution>ICSM (Institut de Chimie Séparative de Marcoule), UMR 5257 (Commissariat a l’energie atomique et aux energies alternatives/CNRS/Ecole Nationale Supérieure de Chimie de Montpellier, Université de Montpellier), 30207 Bagnols sur Cèze</institution>,<country>France</country>;</nlm:aff><country xml:lang="fr">France</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Marcus, Julien" sort="Marcus, Julien" uniqKey="Marcus J" first="Julien" last="Marcus">Julien Marcus</name><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Schoettl, Sebastian" sort="Schoettl, Sebastian" uniqKey="Schoettl S" first="Sebastian" last="Schöettl">Sebastian Schöettl</name><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Horinek, Dominik" sort="Horinek, Dominik" uniqKey="Horinek D" first="Dominik" last="Horinek">Dominik Horinek</name><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Prevost, Sylvain F" sort="Prevost, Sylvain F" uniqKey="Prevost S" first="Sylvain F." last="Prevost">Sylvain F. 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Zemb</name><affiliation wicri:level="1"><nlm:aff id="aff1"><institution>ICSM (Institut de Chimie Séparative de Marcoule), UMR 5257 (Commissariat a l’energie atomique et aux energies alternatives/CNRS/Ecole Nationale Supérieure de Chimie de Montpellier, Université de Montpellier), 30207 Bagnols sur Cèze</institution>,<country>France</country>;</nlm:aff><country xml:lang="fr">France</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Klossek, Michael" sort="Klossek, Michael" uniqKey="Klossek M" first="Michael" last="Klossek">Michael Klossek</name><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Lopian, Tobias" sort="Lopian, Tobias" uniqKey="Lopian T" first="Tobias" last="Lopian">Tobias Lopian</name><affiliation wicri:level="1"><nlm:aff id="aff1"><institution>ICSM (Institut de Chimie Séparative de Marcoule), UMR 5257 (Commissariat a l’energie atomique et aux energies alternatives/CNRS/Ecole Nationale Supérieure de Chimie de Montpellier, Université de Montpellier), 30207 Bagnols sur Cèze</institution>,<country>France</country>;</nlm:aff><country xml:lang="fr">France</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Marcus, Julien" sort="Marcus, Julien" uniqKey="Marcus J" first="Julien" last="Marcus">Julien Marcus</name><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Schoettl, Sebastian" sort="Schoettl, Sebastian" uniqKey="Schoettl S" first="Sebastian" last="Schöettl">Sebastian Schöettl</name><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Horinek, Dominik" sort="Horinek, Dominik" uniqKey="Horinek D" first="Dominik" last="Horinek">Dominik Horinek</name><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Prevost, Sylvain F" sort="Prevost, Sylvain F" uniqKey="Prevost S" first="Sylvain F." last="Prevost">Sylvain F. Prevost</name><affiliation wicri:level="1"><nlm:aff id="aff3">European Synchrotron Radiation Facility (ESRF), 38043 Grenoble, CEDEX 9,<country>France</country>;</nlm:aff><country xml:lang="fr">France</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Touraud, Didier" sort="Touraud, Didier" uniqKey="Touraud D" first="Didier" last="Touraud">Didier Touraud</name><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Diat, Olivier" sort="Diat, Olivier" uniqKey="Diat O" first="Olivier" last="Diat">Olivier Diat</name><affiliation wicri:level="1"><nlm:aff id="aff1"><institution>ICSM (Institut de Chimie Séparative de Marcoule), UMR 5257 (Commissariat a l’energie atomique et aux energies alternatives/CNRS/Ecole Nationale Supérieure de Chimie de Montpellier, Université de Montpellier), 30207 Bagnols sur Cèze</institution>,<country>France</country>;</nlm:aff><country xml:lang="fr">France</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Mar Elja, Stjepan" sort="Mar Elja, Stjepan" uniqKey="Mar Elja S" first="Stjepan" last="Mar Elja">Stjepan Mar Elja</name><affiliation wicri:level="1"><nlm:aff id="aff4">Department of Applied Mathematics, Research School of Physics & Engineering,<institution>Australian National University</institution>, Canberra, ACT 0200,<country>Australia</country></nlm:aff><country xml:lang="fr">Australie</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Kunz, Werner" sort="Kunz, Werner" uniqKey="Kunz W" first="Werner" last="Kunz">Werner Kunz</name><affiliation wicri:level="1"><nlm:aff id="aff1"><institution>ICSM (Institut de Chimie Séparative de Marcoule), UMR 5257 (Commissariat a l’energie atomique et aux energies alternatives/CNRS/Ecole Nationale Supérieure de Chimie de Montpellier, Université de Montpellier), 30207 Bagnols sur Cèze</institution>,<country>France</country>;</nlm:aff><country xml:lang="fr">France</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation><affiliation wicri:level="1"><nlm:aff id="aff2">Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author></analytic><series><title level="j">Proceedings of the National Academy of Sciences of the United States of America</title><idno type="ISSN">0027-8424</idno><idno type="eISSN">1091-6490</idno><imprint><date when="2016">2016</date></imprint></series></biblStruct></sourceDesc></fileDesc><profileDesc><textClass></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en"><title>Significance</title><p>Beginning over 40 y ago, a curious type of microemulsions—as transparent dispersion of two immiscible liquids separated by an interfacial film—at thermodynamic equilibrium has been described as “pre-Ouzo,” “detergentless,” or surfactant-free microemulsions. The experiments in ternary systems containing one hydrotropic cosolvent were ambiguous, and therefore, there was no need to come up with a general theory. Recent evidence obtained by specific deuteration in neutron scattering established the need for the extension of self-assembly theories based on Derjaguin-Landau-Verwey-Overbeck theory (DLVO), bending, or phase transfer energy. Here, we introduce a general free energy expression for weak self-assembly, where solvation effects and entropy compete without the influence of film bending, that explains all experimental results for this class of microemulsions.</p></div></front></TEI><pmc article-type="research-article"><pmc-comment>The publisher of this article does not allow downloading of the full text in XML form.</pmc-comment>
<front><journal-meta><journal-id journal-id-type="nlm-ta">Proc Natl Acad Sci U S A</journal-id><journal-id journal-id-type="iso-abbrev">Proc. Natl. Acad. Sci. U.S.A</journal-id><journal-id journal-id-type="hwp">pnas</journal-id><journal-id journal-id-type="pmc">pnas</journal-id><journal-id journal-id-type="publisher-id">PNAS</journal-id><journal-title-group><journal-title>Proceedings of the National Academy of Sciences of the United States of America</journal-title></journal-title-group><issn pub-type="ppub">0027-8424</issn><issn pub-type="epub">1091-6490</issn><publisher><publisher-name>National Academy of Sciences</publisher-name></publisher></journal-meta><article-meta><article-id pub-id-type="pmid">27044068</article-id><article-id pub-id-type="pmc">4843454</article-id><article-id pub-id-type="publisher-id">201515708</article-id><article-id pub-id-type="doi">10.1073/pnas.1515708113</article-id><article-categories><subj-group subj-group-type="heading"><subject>Physical Sciences</subject><subj-group><subject>Chemistry</subject></subj-group></subj-group></article-categories><title-group><article-title>How to explain microemulsions formed by solvent mixtures without conventional surfactants</article-title><alt-title alt-title-type="short">Hydration stabilizes detergentless microemulsions</alt-title></title-group><contrib-group><contrib contrib-type="author"><name><surname>Zemb</surname><given-names>Thomas N.</given-names></name><xref ref-type="aff" rid="aff1"><sup>a</sup></xref><xref ref-type="corresp" rid="cor1"><sup>1</sup></xref></contrib><contrib contrib-type="author"><name><surname>Klossek</surname><given-names>Michael</given-names></name><xref ref-type="aff" rid="aff2"><sup>b</sup></xref></contrib><contrib contrib-type="author"><name><surname>Lopian</surname><given-names>Tobias</given-names></name><xref ref-type="aff" rid="aff1"><sup>a</sup></xref><xref ref-type="aff" rid="aff2"><sup>b</sup></xref></contrib><contrib contrib-type="author"><name><surname>Marcus</surname><given-names>Julien</given-names></name><xref ref-type="aff" rid="aff2"><sup>b</sup></xref></contrib><contrib contrib-type="author"><name><surname>Schöettl</surname><given-names>Sebastian</given-names></name><xref ref-type="aff" rid="aff2"><sup>b</sup></xref></contrib><contrib contrib-type="author"><name><surname>Horinek</surname><given-names>Dominik</given-names></name><xref ref-type="aff" rid="aff2"><sup>b</sup></xref></contrib><contrib contrib-type="author"><contrib-id contrib-id-type="orcid" authenticated="false">http://orcid.org/0000-0002-6008-1987</contrib-id><name><surname>Prevost</surname><given-names>Sylvain F.</given-names></name><xref ref-type="aff" rid="aff3"><sup>c</sup></xref></contrib><contrib contrib-type="author"><name><surname>Touraud</surname><given-names>Didier</given-names></name><xref ref-type="aff" rid="aff2"><sup>b</sup></xref></contrib><contrib contrib-type="author"><name><surname>Diat</surname><given-names>Olivier</given-names></name><xref ref-type="aff" rid="aff1"><sup>a</sup></xref></contrib><contrib contrib-type="author"><name><surname>Marčelja</surname><given-names>Stjepan</given-names></name><xref ref-type="aff" rid="aff4"><sup>d</sup></xref></contrib><contrib contrib-type="author"><name><surname>Kunz</surname><given-names>Werner</given-names></name><xref ref-type="aff" rid="aff1"><sup>a</sup></xref><xref ref-type="aff" rid="aff2"><sup>b</sup></xref><xref ref-type="corresp" rid="cor1"><sup>1</sup></xref></contrib><aff id="aff1"><sup>a</sup><institution>ICSM (Institut de Chimie Séparative de Marcoule), UMR 5257 (Commissariat a l’energie atomique et aux energies alternatives/CNRS/Ecole Nationale Supérieure de Chimie de Montpellier, Université de Montpellier), 30207 Bagnols sur Cèze</institution>,<country>France</country>;</aff><aff id="aff2"><sup>b</sup>Institut für Physikalische und Theoretische Chemie,<institution>Universität Regensburg</institution>, 93053 Regensburg,<country>Germany</country>;</aff><aff id="aff3"><sup>c</sup>European Synchrotron Radiation Facility (ESRF), 38043 Grenoble, CEDEX 9,<country>France</country>;</aff><aff id="aff4"><sup>d</sup>Department of Applied Mathematics, Research School of Physics & Engineering,<institution>Australian National University</institution>, Canberra, ACT 0200,<country>Australia</country></aff></contrib-group><author-notes><corresp id="cor1"><sup>1</sup>To whom correspondence may be addressed. Email: <email>thomas.zemb@icsm.fr</email> or <email>Werner.Kunz@chemie.uni-regensburg.de</email>.</corresp><fn fn-type="edited-by"><p>Edited by Monica Olvera de la Cruz, Northwestern University, Evanston, IL, and approved February 26, 2016 (received for review August 7, 2015)</p></fn><fn fn-type="con"><p>Author contributions: T.N.Z., D.H., S.M., and W.K. designed research; T.N.Z., M.K., T.L., J.M., S.S., D.H., S.F.P., D.T., O.D., S.M., and W.K. performed research; S.F.P. and O.D. contributed new reagents/analytic tools; T.N.Z., M.K., T.L., J.M., S.S., D.H., S.F.P., O.D., and S.M. analyzed data; and T.N.Z., S.M., and W.K. wrote the paper.</p></fn></author-notes><pub-date pub-type="ppub"><day>19</day><month>4</month><year>2016</year></pub-date><pub-date pub-type="epub"><day>1</day><month>4</month><year>2016</year></pub-date><pub-date pub-type="pmc-release"><day>1</day><month>4</month><year>2016</year></pub-date><pmc-comment> PMC Release delay is 0 months and 0 days and was based on the
<volume>113</volume><issue>16</issue><fpage>4260</fpage><lpage>4265</lpage><permissions><license license-type="open-access"><license-p>Freely available online through the PNAS open access option.</license-p></license></permissions><self-uri xlink:title="pdf" xlink:href="pnas.201515708.pdf"></self-uri><abstract abstract-type="executive-summary"><title>Significance</title><p>Beginning over 40 y ago, a curious type of microemulsions—as transparent dispersion of two immiscible liquids separated by an interfacial film—at thermodynamic equilibrium has been described as “pre-Ouzo,” “detergentless,” or surfactant-free microemulsions. The experiments in ternary systems containing one hydrotropic cosolvent were ambiguous, and therefore, there was no need to come up with a general theory. Recent evidence obtained by specific deuteration in neutron scattering established the need for the extension of self-assembly theories based on Derjaguin-Landau-Verwey-Overbeck theory (DLVO), bending, or phase transfer energy. Here, we introduce a general free energy expression for weak self-assembly, where solvation effects and entropy compete without the influence of film bending, that explains all experimental results for this class of microemulsions.</p></abstract><abstract><p>Ternary solutions containing one hydrotrope (such as ethanol) and two immiscible fluids, both being soluble in the hydrotrope at any proportion, show unexpected solubilization power and allow strange but yet unexplained membrane enzyme activity. We study the system ethanol-water-octanol as a simple model of such kinds of ternary solutions. The stability of “detergentless” micelles or microemulsions in such mixtures was proposed in the pioneering works of Barden and coworkers [Smith GD, Donelan CE, Barden RE (1977) <italic>J Colloid Interface Sci</italic> 60(3):488–496 and Keiser BA, Varie D, Barden RE, Holt SL (1979) <italic>J Phys Chem</italic> 83(10):1276–1281] in the 1970s and then, neglected, because no general explanation for the observations was available. Recent direct microstructural evidence by light, X-ray, and neutron scattering using contrast variation reopened the debate. We propose here a general principle for solubilization without conventional surfactants: the balance between hydration force and entropy. This balance explains the stability of microemulsions in homogeneous ternary mixtures based on cosolvents.</p></abstract><kwd-group><kwd>microemulsions</kwd><kwd>aggregation</kwd><kwd>micelles</kwd><kwd>hydrotrope</kwd><kwd>hydration force</kwd></kwd-group><funding-group><award-group id="gs1"><funding-source id="sp1">European Cooperation in Science and Technology (COST)<named-content content-type="funder-id">501100000921</named-content></funding-source><award-id rid="sp1">CM-1101</award-id></award-group><award-group id="gs2"><funding-source id="sp2">Agence Nationale de la Recherche (L' Agence Nationale de la Recherche)<named-content content-type="funder-id">501100001665</named-content></funding-source><award-id rid="sp2">Labex Chemisyst</award-id></award-group><award-group id="gs3"><funding-source id="sp3">EC | European Research Council (ERC)<named-content content-type="funder-id">501100000781</named-content></funding-source><award-id rid="sp3">320915 REE-CYCLE</award-id></award-group><award-group id="gs4"><funding-source id="sp4">Centre National d'Etudes Spatiales (National Centre for Space Research, France)<named-content content-type="funder-id">501100002830</named-content></funding-source><award-id rid="sp4">LIA RECYCLING</award-id></award-group></funding-group><counts><page-count count="6"></page-count></counts></article-meta></front></pmc></record>Pour manipuler ce document sous Unix (Dilib)
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