Remarkable Conversion Between n- and p-Type Reduced Graphene Oxide on Varying the Thermal Annealing Temperature

To allow for the use of graphene in various nanoelectronic applications, the methods for the large-scale production of graphene with controllable electrical properties need to be developed. Here, we report the results of a fundamental study on the remarkable conversion between n- and p-type reduced graphene oxide (rGO) with changes in the thermal annealing temperature. It was found that the charge carriers in rGO for temperatures of 300–450 °C and 800–1000 °C are electrons (n-type), whereas for temperatures of 450–800 °C, they are holes (p-type). This is because the individual oxygen functional groups present on rGO are determined by the annealing temperature. We found that the predominance of electron-withdrawing groups (i.e., carboxyl, carbonyl, and sp3-bonded hydroxyl, ether, and epoxide groups) resulted in p-type rGO, although that of electron-donating groups (sp2-bonded hydroxyl, ether and epoxide groups) lead to n-type rGO. In addition, as a proof of concept, a flexible thermoelectric device consist...