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Thermoelectric properties of the layered cobalt oxide system LixCoO2 wereinvestigated in a wide range of Li composition, 0.98 >= x >= 0.35. Single-phasebulk samples of LixCoO2 were successfully obtained through electrochemicaldeintercalation of Li from the pristine LiCoO2 phase. While LixCoO2 with x >=0.94 is semiconductive, the highly Li-deficient phase (0.75 >= x >= 0.35)exhibits metallic conductivity. The magnitude of Seebeck coefficient at 293 K(S293K) significantly depends on the Li content (x). The S293K value is aslarge as +70 ~ +100 uV/K for x >= 0.94, and it rapidly decreases from +90 uV/Kto +10 uV/K as x is lowered within a Li composition range of 0.75 >= x >= 0.50.This behavior is in sharp contrast to the results of x <= 0.40 for which theS293K value is small and independent of x (+10 uV/K), indicating that adiscontinuous change in the thermoelectric characteristics takes place at x =0.40 ~ 0.50. The unusually large Seebeck coefficient and metallic conductivityare found to coexist in a narrow range of Li composition at about x = 0.75. Thecoexistence, which leads to an enhanced thermoelectric power factor, may beattributed to unusual electronic structure of the two-dimensional CoO2 block.

Impact of lithium composition on the thermoelectric properties of the layered cobalt oxide system LixCoO2