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New insights into the thermal behaviour of organic ionic plastic crystals: magnetic resonance imaging of polycrystalline morphology alterations induced by solid-solid phase transitions

Romanenko, Konstantin, Pringle, Jennifer M., O'Dell, Luke A. and Forsyth, Maria 2015, New insights into the thermal behaviour of organic ionic plastic crystals: magnetic resonance imaging of polycrystalline morphology alterations induced by solid-solid phase transitions, Physical chemistry chemical physics, vol. 17, no. 29, pp. 18991-19000, doi: 10.1039/c5cp03294f.

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Title New insights into the thermal behaviour of organic ionic plastic crystals: magnetic resonance imaging of polycrystalline morphology alterations induced by solid-solid phase transitions
Author(s) Romanenko, Konstantin
Pringle, Jennifer M.ORCID iD for Pringle, Jennifer M. orcid.org/0000-0002-2729-2838
O'Dell, Luke A.ORCID iD for O'Dell, Luke A. orcid.org/0000-0002-7760-5417
Forsyth, MariaORCID iD for Forsyth, Maria orcid.org/0000-0002-4273-8105
Journal name Physical chemistry chemical physics
Volume number 17
Issue number 29
Start page 18991
End page 19000
Total pages 10
Publisher Royal Society of Chemistry
Place of publication Cambridge, Eng.
Publication date 2015-07-15
ISSN 1463-9084
Summary Organic ionic plastic crystals (OIPCs) show strong potential as solid-state electrolytes for lithium battery applications, demonstrating promising electrochemical performance and eliminating the need for a volatile and flammable liquid electrolyte. The ionic conductivity (σ) in these systems has recently been shown to depend strongly on polycrystalline morphology, which is largely determined by the sample's thermal history. [K. Romanenko et al., J. Am. Chem. Soc., 2014, 136, 15638]. Tailoring this morphology could lead to conductivities sufficiently high for battery applications, so a more complete understanding of how phenomena such as solid-solid phase transitions can affect the sample morphology is of significant interest. Anisotropic relaxation of nuclear spin magnetisation provides a new MRI based approach for studies of polycrystalline materials at both a macroscopic and molecular level. In this contribution, morphology alterations induced by solid-solid phase transitions in triisobutyl(methyl)phosphonium bis(fluorosulfonyl)imide (P1444FSI) and diethyl(methyl)(isobutyl)phosphonium hexafluorophosphate (P1224PF6) are examined using magnetic resonance imaging (MRI), alongside nuclear magnetic resonance (NMR) spectroscopy, diffusion measurements and conductivity data. These observations are linked to molecular dynamics and structural behaviour crucial for the conductive properties of OIPCs. A distinct correlation is established between the conductivity at a given temperature, σ(T), and the intensity of the narrow NMR signal that is attributed to a mobile fraction, fm(T), of ions in the OIPC. To explain these findings we propose an analogy with the well-studied relationship between permeability (k) and void fraction (θ) in porous media, with k(θ) commonly quantified by a power-law dependence that can also be employed to describe σ(fm).
Language eng
DOI 10.1039/c5cp03294f
Field of Research 030604 Electrochemistry
Socio Economic Objective 850602
HERDC Research category C1 Refereed article in a scholarly journal
ERA Research output type C Journal article
Copyright notice ©2015, Royal Society of Chemistry
Persistent URL http://hdl.handle.net/10536/DRO/DU:30074169

Document type: Journal Article
Collections: Institute for Frontier Materials
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Every reasonable effort has been made to ensure that permission has been obtained for items included in DRO. If you believe that your rights have been infringed by this repository, please contact drosupport@deakin.edu.au.