Role of defects in the high ionic conductivity of choline triflate plastic crystal and its acid-containing compositions

Rana, Usman Ali, Vijayaraghavan, R., Doherty, Cara M., Chandra, Amreesh, Efthimiadis, Jim, Hill, Anita J., MacFarlane, D.R. and Forsyth, Maria 2013, Role of defects in the high ionic conductivity of choline triflate plastic crystal and its acid-containing compositions, Journal of physical chemistry C, vol. 117, no. 11, pp. 5532-5543.

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Title Role of defects in the high ionic conductivity of choline triflate plastic crystal and its acid-containing compositions
Author(s) Rana, Usman Ali
Vijayaraghavan, R.
Doherty, Cara M.
Chandra, Amreesh
Efthimiadis, Jim
Hill, Anita J.
MacFarlane, D.R.
Forsyth, Maria
Journal name Journal of physical chemistry C
Volume number 117
Issue number 11
Start page 5532
End page 5543
Total pages 12
Publisher American Chemical Society
Place of publication Washington, D.C.
Publication date 2013
ISSN 1932-7447
1932-7455
Summary We present an investigation of the organic ionic plastic crystal choline triflate, both in its pure state and in mixtures with triflic acid. High ionic conductivity behavior was observed in these materials in the solid state with Arrhenius behavior evident in all cases suggesting a single, thermally activated conduction mechanism of ionic transport. The activation energies (E a) in phases II and I were very low (?16-17 kJ mol-1), consistent with plasticlike mechanical properties throughout the wide range of temperatures (0-130 C) investigated here. Positron annihilation lifetime spectroscopy (PALS) indicated that the thermally generated defects play a significant role in the high ionic conductivities in these phases. High-resolution powder XRD studies showed a structural transformation from monoclinic to cubic at the II ? I phase transformation in all samples. The acid-containing samples exhibited an additional phase (phase III) and displayed structural transformations from orthorhombic to monoclinic to cubic with increasing temperature in the phase III ? II ? I transition. This system exhibited unusual behavior, with the addition of acid leading to apparently less mobility of the matrix ions (as seen by NMR spectroscopy and the decrease in low-temperature conductivity) despite a higher proton reduction activity than previously reported. The combination of high-resolution XRD, PALS, and solid-state NMR techniques at varying temperature suggests a thermally activated, defect-assisted conductivity mechanism of ionic transport in these materials.
Language eng
Field of Research 099999 Engineering not elsewhere classified
Socio Economic Objective 970109 Expanding Knowledge in Engineering
HERDC Research category C1 Refereed article in a scholarly journal
Copyright notice ©2013, American Chemical Society
Persistent URL http://hdl.handle.net/10536/DRO/DU:30057701

Document type: Journal Article
Collection: Institute for Frontier Materials
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