Recently, with the miniaturization of electronic devices, problems with regard to the size and capacity of batteries have arisen. Energy harvesting is receiving significant attention to solve these problems. In particular, the thermoelectric generator (TEG) is being studied for its ability to harvest waste heat energy. However, studies on organic TEGs conducted thus far have mostly used conductive polymers, making the application range of TEGs relatively narrow. In this study, we fabricated organic TEGs using carbonaceous nanomaterials (i.e., graphene nanoplatelet (GNP) and single-walled carbon nanotube (SWNT)) with polyelectrolytes (i.e., poly(vinyl alcohol) (PVA) and poly (diallyldimethyl ammonium chloride) (PDDA)) via layer-by-layer (LbL) coating on polymeric substrates. The thermoelectric performance of the carbonaceous multilayer structure was measured, and it was confirmed that the thermoelectric performance of the TEG in this study was not significantly different from that of the existing organic TEG fabricated using the conductive polymers. The 10 bilayer SWNT thin films with polyelectrolyte exhibited a thermopower of −14 μV·K−1 and a power factor of 25 μW·m−1K−2. Moreover, by simply changing the electrolyte, p- or n-type TEGs could be easily fabricated with carbonaceous nanomaterials via the LbL process. Also, by just changing the electrolyte, p- or n-type of TEGs could be easily fabricated with carbonaceous nanomaterials with a layer-by-layer process.
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