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Although 1,4-DIO and 1,3-DIO molecules are structural isomers, our results point out that 1,4-DIO cannot be strongly hydrogen-bonded with the ring H atoms. The solvation of [TFSI]- by cycloethers through the dipole-dipole interaction promotes hydrogen bonding between the ring H atoms and cycloethers. Thus, 1,4-DIO with the lowest dipole moment cannot easily eliminate [TFSI]- from the imidazolium ring. This results in the weakest hydrogen bonds of 1,4-DIO with the ring H atoms. 2D-NMR of 1H1H rotating-frame nuclear Overhauser effect spect