Adding ethylene glycol (EG) to a poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) solution improves the crystallinity of the PEDOT and the ordering of the PEDOT nanocrystals in solid films. The carrier-mobility enhancement is confirmed by using ion-gel transistors combined with in situ UV-vis-NIR spectroscopy.

The thermoelectric properties of poly(3,4-ethylenedioxythiophene) (PEDOT)-based materials have attracted attention recently because of their remarkable electrical conductivity, power factor, and figure of merit. In this review, we summarize recent efforts toward improving the thermoelectric properties of PEDOT-based materials. We also discuss thermoelectric measurement techniques and several unsolved problems with the PEDOT system such as the effect of water absorption from the air and the anisotropic thermoelectric properties. In the last part, we describe our work on improving the power output of thermoelectric modules by using PEDOT, and we outline the potential applications of polymer thermoelectric generators.

We report organic thermoelectric modules screen-printed on paper by using conducting polymer poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) and silver paste. Our large-area devices provided sufficient power to illuminate light-emitting diodes. This is the first example of thermoelectric modules containing conducting polymers being used to power practical devices. The stability of this proof-of-concept module was tested at 100 C for over 100 h without any encapsulation. We showed that the decrease in device performance was caused not by the deterioration of the materials but by degradation of the interface between the conducting polymers and silver paste. These results suggest that organic thermoelectric modules could be used to harvest heat energy at low temperature, although the stability of the interface must be improved.

We reported general methods for studying the thermoelectric properties of a polymer film in both the in-plane and through-plane directions. The bench-mark PEDOT/PSS films have highly anisotropic carrier transport properties and thermal conductivity. The anisotropic carrier transport properties can be explained by the lamellar structure of the PEDOT/PSS films where the PEDOT nanocrystals could be isolated by the insulating PSS in the through-plane direction. The anisotropic thermal conductivity was mainly attributed to the lattice contribution from PSS because the polymer chain is oriented along the substrate.

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Thermoelectric power generation from waste heat is an important component of future sustainable development. Ion-conducting materials are promising candidates because of their high Seebeck coefficients. This study demonstrates that ionic hydrogels based on imidazolium chloride salts exhibit outstanding Seebeck coefficients of up to 10 mV K −1 . Along with their relatively high ionic conductivities (1.6 mS cm −1 ) and extremely low thermal conductivities (∼0.2 W m −1 K −1 ), these hydrogels have good potential for use in heat recovery systems. The voltage behavior in response to temperature difference (stable or transient) differs significantly depending on the metal electrode material. We evaluated the electrode-dependent temperature sensitivity of the double layer capacitance of these hydrogels, which revealed that the thermally induced polarization of ions at the interface is one of the main contributors to the thermovoltage. Our results demonstrate the potential capability for ion and metal interactions to be used as an effective baseline for exploring ionic thermoelectric materials and devices. The developed thermoelectric supercapacitor exhibits reversible charging−discharging behavior under repeated disconnecting−connecting of an external load with a constant temperature difference, which offers a novel strategy for heat-to-electricity energy conversion from steady-temperature heat sources.

We report an increase in the thermoelectric power factor of poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) from 23 ± 5 to 225 ± 130 µW/(m·K2) in high-humidity conditions. This enhancement was caused mainly by an increase in the apparent Seebeck coefficient, which could be related to morphological change after water absorption or electrochemical reaction of PEDOT in air. Our results demonstrate a positive effect of water in the PEDOT:PSS system and indicate the need for well-controlled measurement conditions, particularly humidity, in evaluating the performance of conducting organic materials.

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