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Pentaglyme-K salt binary mixtures: phase behavior, solvate structures, and physicochemical properties

Toshihiko Mandai (Institutionen för teknisk fysik, Kondenserade materiens fysik) ; S. Tsuzuki ; K. Ueno ; K. Dokko ; M. Watanabe
Physical Chemistry Chemical Physics (1463-9076). Vol. 17 (2015), 4, p. 2838-2849.
[Artikel, refereegranskad vetenskaplig]

We prepared a series of binary mixtures composed of certain K salts (KX) and pentaglyme (G5) with different salt concentrations and anionic species ([X](-) : [(CF3SO2)(2)N](-) = [TFSA](-), [CF3SO3](-) = [TfO](-), [C4F9SO3](-) = [NfO](-), PF6-, SCN-), and characterized them with respect to their phase diagrams, solvate structures, and physicochemical properties. Their phase diagrams and thermal stability strongly implied the formation of equimolar complexes. Single-crystal X-ray crystallography was performed on certain equimolar complexes, which revealed that G5 molecules coordinate to K+ cations in a characteristic manner, like 18-crown-6 ether in the crystalline state, irrespective of the paired anions. The solvate structures in the molten state were elucidated by a combination of temperature-dependent Raman spectroscopy and X-ray crystallography. A drastic spectral variation was observed in the [K(G5)(1)][TfO] Raman spectra, indicating that solvate structures in the crystalline state break apart upon melting. The solvate stability of [K(G5)(1)]X is closely related to the ion-ion interaction of the parent salts. A stable solvate forms when the ion-dipole interaction between K+ and G5 overwhelms the ion-ion interaction between K+ and X-. Furthermore, the physicochemical properties of certain equimolar mixtures were evaluated. A Walden plot clearly reflects the ionic nature of the molten equimolar complexes. Judging from the structural characteristics and dissociativity, we classified [K(G5)(1)]X into two groups, good and poor solvate ionic liquids.

Denna post skapades 2015-01-29.
CPL Pubid: 211707


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Institutioner (Chalmers)

Institutionen för teknisk fysik, Kondenserade materiens fysik (1900-2015)


Teknisk fysik

Chalmers infrastruktur