A lithium isotope concentration device 10 is provided with a treatment tank 1 partitioned into a supply tank 11 and a recovery tank 12 by an electrolyte membrane 2 having lithium-ion conductivity, the electrolyte membrane 2 being cooled by a cooling device 6 via a Li-containing aqueous solution ASi in the supply tank 11 to obtain a low temperature at which the 6Li isotope separation coefficient is larger, and a positive voltage being applied, by a power supply 5 connected between electrodes 31, 32 provided on both surfaces of the electrolyte membrane 2, to the supply tank 11-side electrode 31.
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