Hybrids of carbon nanotubes (CNTs) and poly(3,4-ethylenedioxythiophene) (PEDOT) treated by tetrakis(dimethylamino)ethylene (TDAE) have large n-type voltages in response to temperature differences. The reduced carrier concentration by TDAE reduction and partially percolated CNT networks embedded in the PEDOT matrix result in high thermopower and low thermal conductivity. The high electron mobility in the CNTs helps to minimally reduce the electrical conductivity of the hybrid, resulting in a large figure-of-merit.
Electrical conductivity and thermopower of isotropic materials typically have inversely proportional correlation because both are strongly affected in the opposite way by the electronic carrier concentration. This behavior has been one of the major hurdles in developing high-performance thermoelectrics whose figure-of-merit enhances with large thermopower and high electrical conductivity. Here we report a promising method of simultaneously improving both properties with polyaniline (PANI) composites filled by carbon nanotubes (CNTs). With addition of double-wall CNTs (DWCNTs), the electronic mobility of PANI doped with camphorsulfonic acid (PANI-CSA) was raised from ∼0.15 to ∼7.3 cm(2)/(V s) (∼50 time improvement) while the carrier concentration was decreased from ∼2.1 × 10(21) to ∼5.6 × 10(20) cm(-3) (∼4 time reduction). The larger increase of mobility increased electrical conductivity despite the carrier concentration reduction that enlarges thermopower. The improvement in the carrier mobility could be attributed to the band alignment that attracts hole carriers to CNTs whose mobility is much higher than that of PANI-CSA. The electrical conductivity of the PANI-CSA composites with 30-wt % DWCNTs was measured to be ∼610 S/cm with a thermopower value of ∼61 μV/K at room temperature, resulting in a power factor value of ∼220 μW/(m K(2)), which is more than two orders higher than that of PANI-CSA as well as the highest among those of the previously reported PANI composites. Further study may result in high performance thermoelectric organic composites uniquely offering mechanical flexibility, light weight, low toxicity, and easy manufacturing. unlike conventional inorganic semiconductors.
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