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An initial increase in the glass temperature (<jats:italic>T<\/jats:italic><jats:sub>g<\/jats:sub>) with an increase in the alkyl side chain was observed due to the intensification of the dispersive interactions (van der Waals). Above the CAS, the \u2212CH<jats:sub>2<\/jats:sub>\u2212 increment has the same effect in both glass and liquid states, which leads to a plateau in the glass transition after nanostructuration. The melting temperature (<jats:italic>T<\/jats:italic><jats:sub>m<\/jats:sub>) of the [C<jats:sub><jats:italic>n<\/jats:italic><\/jats:sub>C<jats:sub>1<\/jats:sub>im][NTf<jats:sub>2<\/jats:sub>] and [C<jats:sub><jats:italic>n<\/jats:italic><\/jats:sub>C<jats:sub><jats:italic>n<\/jats:italic><\/jats:sub>im][NTf<jats:sub>2<\/jats:sub>] series presents a V\u2010shaped profile. For the short\u2010alkyl ILs, the \u2212CH<jats:sub>2<\/jats:sub>\u2212 increment affects the electrostatic ion pair interactions, which leads to an increase in the conformational entropy. The \u2212CH<jats:sub>2<\/jats:sub>\u2212 increment disturbs the packing ability of the ILs and leads to a higher entropy value (<jats:inline-graphic xmlns:xlink=\"http:\/\/www.w3.org\/1999\/xlink\" xlink:href=\"graphic\/cphc201501128-math-0001.png\" xlink:title=\"urn:x-wiley:14394235:media:cphc201501128:cphc201501128-math-0001\"\/>\n) and consequently a decrease in <jats:italic>T<\/jats:italic><jats:sub>m<\/jats:sub>. Above the CAS, the \u2212CH<jats:sub>2<\/jats:sub>\u2212 contribution to the melting temperature becomes more regular, as a consequence of the nanostructuration of the IL into polar and nonpolar domains. The dependence of the alkyl chain on the temperature, enthalpy, and entropy of melting in the ILs above the CAS is very similar to the one observed for the alkane series, which highlights the importance of the nonpolar alkyl domains on the ILs thermal behavior.<\/jats:p>","DOI":"10.1002\/cphc.201501128","type":"journal-article","created":{"date-parts":[[2016,2,18]],"date-time":"2016-02-18T08:03:29Z","timestamp":1455782609000},"page":"1512-1517","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":33,"title":["Nanostructuration Effect on the Thermal Behavior of Ionic Liquids"],"prefix":"10.1002","volume":"17","author":[{"given":"Ana S. M. C.","family":"Rodrigues","sequence":"first","affiliation":[{"name":"CIQ, Departamento de Qu\u00edmica e Bioqu\u00edmica Faculdade de Ci\u00eancias da Universidade do Porto, P-  4169-007 Porto Portugal"}]},{"given":"Lu\u00eds M. N. B. 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