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Eight plastic crystals of the types NEt  x  Me (4 −  x ) BEt 4  and NEt  y  Pr (4 −  y ) BEt 4  ( x =0–4,  y =1–3) were found in a new region of ionic plastic crystals. In this area, globular cations and anions are assembled by weak interactions. Based on the results of solid-state  1 H and  13 C nuclear magnetic resonance (NMR) measurements, it was revealed that the ions performed isotropic reorientations in the NEt  x  Me (4– x ) BEt 4  crystals ( x =0–4). Additionally, X-ray diffraction (XRD) of these compounds was able to identify the CsCl-type cubic structure. In contrast, the XRD reflections of NEt  y  Pr (4− y ) BEt 4  ( y =1–3) could be successfully fitted by distorted cubic lattices (trigonal symmetry). The NMR line shapes observed in these compounds were explained by overall molecular motions with large amplitudes (pseudo-isotropic reorientations). Differential scanning calorimetry (DSC) spectra of NEt  y  Pr (4 −  y ) BEt 4  ( y =1–3) showed a low entropy change (Δ S  mp ) of 6–8 J K −1  mol −1  at the melting point. Ionic diffusion was identified by electrical conductivity measurements of NEt  x  Me (4 −  x ) BEt 4  and NEt  y  Pr (4– y ) BEt 4  ( x =0–4,  y =1–3). In the case of NPr 4 BEt 4  crystals, ionic diffusion was also detected, although complex powder patterns and large Δ S  mp  values were observed by XRD and DSC measurements, respectively.

1 H and 13 C NMR and Electrical Conductivity Studies on New Ionic Plastic Crystals of Tetraalkylammonium Tetraethylborate