The isotope separation between 7Li and 6Li was examined on several inorganic ion-exchangers that are selective
for lithium ions. The isotope separation coefficient, S(7/6), was measured by the batch method. The hydration
property of lithium ions in the amorphous ion-exchangers was examined by the solid NMR and for crystalline
ones either by the solid NMR or the X-ray diffraction analysis. The ion-exchangers that have high lithium
ion selectivity had a tendency to enrich 6Li and resultant high S(7/6). The observed S(7/6) increased with
increasing the degree of dehydration in the solid phase. The ion-exchangers that sorbed lithium ions in
completely dehydrated state exhibited a high isotope separation coefficient, and the highest value of 1.04 was
attained on cubic-HNbO3. The observed S(7/6) were accounted for the statistical isotope reduced partition
function ratio (RPFR) of the vibrational mode for the isotopes of interest, f(7/6). The observed S(7/6) for
cubic-HNbO3 was accounted for in the Raman spectrum data that reflect the vibrational energy state. The
value 1.04 observed on cubic-HNbO3 was in consistent with the theoretical prediction. In addition, the theoretical
(highest) 7Li/6Li isotope separation coefficient was estimated to be around 1.05 at 25 °C between aqueous
solution and HMO3 (M = Sb, Nb, and Ta) in which lithium ions were sorbed in the completely dehydrated
state.