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Solution-state NMR spectroscopy is an important method to study chemical structures, intramolecular local motions and translational and rotational motions of a whole molecule. NMR parameters of the solution-state NMR are chemical shift, spin-spin coupling constant, spectral pattern including line width, spin-lattice relaxation time (T1) and spin-spin relaxation time (T2). The assignment of the spectral signals is the starting task for advanced studies. Various two-dimensional (2D) NMR techniques can help to make assignments for complex compounds. Additionally, 2D-NMR techniques afford information on the intermolecular interactions or molecular diffusion. Generally, chemical structures of ionic liquids (IL) are not complex and the NMR spectra can be assigned easily using general rules. Once the assignment is fixed, we can obtain the precise data for the individual species for ILs. Multinuclear NMR techniques can be applied to magnetic active nuclei, and the nuclei relating to ILs are 1H, 2H, 7Li, 11B, 13C, 19F, 31P and others. In addition to general NMR spectra, self-diffusion coefficient (D) of each ion can be measured by the pulse-gradient spin-echo (PGSE) NMR method. The D’s of the individual ions in ILs are important to understand translational motion of ions. In this chapter, NMR studies for four ILs having a common anion bis(fluoromethylsulfonyl)amine (TFSA) will be described. The cations are N-ethyl-Nmethylimidazolium (EMIm), N,2-dimethyl-N-propylimidazolium (DMPIm), N-methyl-Npropylpyrrolidinium (P13), and N,N-diethyl-N-methyl-N-(2-methoxylethyl)ammonium (DEME). These ILs are important candidates to use as electrolytes in various batteries or cells. The basic properties of molecular weight (MW), viscosity () and cation and TFSA diffusion coefficients (Dcation and DTFSA) measured at 30°C are given in Table 1 for the four ILs. The experimental data have been published in our previous papers for individual ILs.1-4 In the present chapter, the individual experimental data for the four ILs are plotted on a sheet to clarify the cation properties. In addition, newly derived plots of Dcation versus correlation times of molecular motion are included. The chemical structures of the ions are shown. To study the translational and rotational motions of ILs by NMR spectroscopy, the D’s of the individual ions and the T1’s of the individual protons are important parameters in the

Translational and Rotational Motions for TFSA-Based Ionic Liquids Studied by NMR Spectroscopy