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Solvation interaction and ion association in solutions of lithium perchlorate/4-methoxymethyl-ethylene carbonate (MEC) have been studied by using Infrared and Raman spectra as a function of concentration of lithium perchlorate. The splitting of ring deformation band and ring ether asymmetric stretching band, and the change of carbonyl stretching band suggest that there should be a strong interaction between Li + and the solvent molecules, and the site of solvation should be the oxygen atom of carbonyl group. The apparent solvation number of Li ＋ was calculated by using band fitting technique. The solvation number was decreased from 3.3 to 1.1 with increasing the concentration of LiClO 4 /MEC solutions. On the other hand, the band fitting for the 4 ClO -band revealed the presence of contact ion pair, and free 4 ClO -anion in the concentrated solutions.