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Free-standing poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT: PSS)/Bi2Te3 thermoelectric (TE) composite films have been successfully prepared by a simple physical mixing method with different contents of Bi2Te3. x-Ray diffraction (XRD) and scanning electron microscopy were used to analyze the phase composition and microstructure of the composite films. Their TE performance from 100 K to 300 K was systematically investigated. The maximum electrical conductivity of the composite polymer film reached up to 421 S/cm when the film contained 10 wt.% Bi2Te3, corresponding to the highest power factor of 9.9 μW/m/K2, while their Seebeck coefficient fluctuated smoothly in a tiny range (14.2 μV/K to 18.6 μV/K). In addition, a relatively low thermal conductivity of 0.07 ± 0.02 W/m/K has been obtained. The maximum figure of merit of the composite reached up to 0.04 at room temperature, which is a relatively high value in the organic TE field.

Significant enhancement of thermoelectric (TE) performance was observed for free-standing poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT: PSS) composite films obtained from a PEDOT:PSS aqueous solution by simultaneous addition of dimethyl sulfoxide (DMSO) and different concentrations of urea. The electrical conductivity was enhanced from 8.16 S cm−1 to over 400 S cm−1, and the maximum Seebeck coefficient reached a value of 18.81 μV K−1 at room temperature. The power factor of the PEDOT:PSS composite films reached 8.81 μW m−1 K−2. The highest thermoelectric figure of merit (ZT) in this study was 0.024 at room temperature, which is at least one order of magnitude higher than most polymers and bulk Si. These results indicate that the obtained composite films are a promising thermoelectric material for applications in thermoelectric refrigeration and thermoelectric microgeneration.

The electrical conductivity and Seebeck coefficient of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) films were simultaneously improved by adding an ionic liquid (IL) into a polymer solution of the polymers. The maximum electrical conductivity of such a PEDOT:PSS/IL film reached 174 S cm−1, more than an order of magnitude higher than that of pure PEDOT:PSS film, and the maximum Seebeck coefficient was up to 30 μV K−1, more than twice the value for pure PEDOT:PSS film. This behavior is different from conventional thermoelectric (TE) materials, whose TE properties are strongly correlated, such as increasing electrical conductivity with increasing carrier concentration, usually resulting in a logarithmic decrease in Seebeck coefficient. Atomic force microscopy images of the PEDOT:PSS/IL films indicated that the ILs induced formation of a particular three-dimensional structure of highly conducting PEDOT grains, resulting in improvement of the TE performance of PEDOT:PSS films.