Journal
JOURNAL OF PHYSICAL CHEMISTRY B
Volume 121, Issue 21, Pages 5439-5446Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcb.7b02780
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Funding
- Australian Research Council (ARC) [DP170100269]
- Monash University
- ARC
- US National Science Foundation [DMR 1057764]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1507764] Funding Source: National Science Foundation
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Understanding the short-range molecular motions of organic ionic plastic crystals is critical for the application of these materials as solid-state electrolytes in electrochemical devices, such as lithium batteries. However, The theory of short-range-motions was originally developed for simple molecular plastic crystals and does not take account of strong interionic interactions that are present in organic ionic plastic crystals. Here we report a fundamental investigation of the dynamic behavior of an archetypal example triethyl(methyl)-phosphonium bis(fluorosulfonyl)amide ([P-1222][FSI]) through calorimetry, impedance spectroscopy, synchrotron X-ray diffraction, and solid-state NMR and Raman spettroscopies. For the first time, we shaw the presence of conformational dynamics in the solid state for the FSI anion. We relate the dynamics to a unique second-order displacive phase transition of [P-1222][FSI]. This detailed analysis suggests a new disorder mechanism involving cooperative motion between the cation and FSI anion in the plastic crystal due to strong interionic interactions.
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