The fabrication of flexible high-performance organic/inorganic thermoelectric (TE) composite films has been a hot spot for researchers in recent years. In this work, dynamic 3-phase interfacial electropolymerization of aniline, together with physical mixing with single-walled carbon nanotubes (SWCNTs), was adopted to prepare polyaniline/SWCNT (PANI/SWCNT) TE composites. The dimethyl sulfoxide (DMSO) added into the electrochemical polymerization system affords strong capability in improving the TE performance of composite films. Moreover, varying loadings of SWCNTs can also conveniently tune the TE performance of composites. Hence, the resultant composites afford the highest power factor (PF) of 236.4 ± 5.9 μW m–1 K–2 at room temperature. This work demonstrates that the introduction of DMSO into the electrolyte and the electrochemical polymerization are highly effective in fabricating high-performance PANI/SWCNT TE composites.

Electrochemical polymerization has proven very effective in fabricating flexible organic/inorganic composite films with high thermoelectric (TE) performance. In this work, dynamic three-phase interfacial electropolymerization of 3,4-ethylenedioxythiophene (EDOT) combined with physical mixing of single-walled carbon nanotubes (SWCNT) and tellurium nanowires was employed to prepare PEDOT/Te/SWCNT thermoelectric composites. When the loadings of Te and SWCNT were changed, the electropolymerized PEDOT exhibited great capability of improving TE properties of the resultant composites with a highest electrical conductivity (σ) of 900.3 ± 20.5 S cm–1 and Seebeck coefficient (S) of 43.4 ± 0.6 μV K–1, affording maximum power factor (PF) of 169.8 ± 7.8 μW m–1 K–2 at room temperature.

Aerogels are promising in the preparation of high-performance thermoelectric (TE) materials due to their ultralow thermal conductivity. However, the TE performance of aerogels remains unsatisfactory. Herein, polyaniline/single-walled carbon nanotubes (PANI/SWCNT) composite aerogel with high thermoelectric performance is synthesized through dynamic three-phase interfacial electrochemical polymerization of aniline and subsequent physical mixing of PANI with SWCNTs followed by liquid nitrogen quenching and freeze-drying. By adjusting the content of SWCNTs, the PANI/SWCNT aerogel (50 wt% SWCNTs) achieves a high power factor (PF) of 73.33 ± 2.03 μW m −1 K −2 . The ultralow thermal conductivity of around 2.30 × 10 −2 W m −1 K −1 for the composite aerogel is superior to that of most conventional organic TE materials, rendering an excellent figure of merit (ZT) value of ≈0.95 at room temperature and great potential in improving TE performance of organic and organic/inorganic composites. Thermal treatment of the composite aerogel further enhances the PF to 96.28 ± 1.89 μW m −1 K −2 . This work provides an effective method in the formation of PANI/SWCNT TE composites and it puts forward insights into the preparation of other high-performance TE composites.

Poly(aniline-co-pyrrole) formed on SWCNTs via electropolymerization affords a greatly enhanced power factor of 111.4 ± 3.2 μW m−1 K−2 at room temperature.

With increasing popularity and great application prospects of flexible wearable electronics, organic thermoelectric (TE)­materials have become one hotspot in view of energy recycling and environment protection. However, diversifying application scenarios and frequent movements impose inevitable damage to materials. Herein, the polyethylene (PE) matrix is used in compositing with poly­(3,4-ethylenedioxythiophene) and single-walled carbon nanotubes, forming a unique conductive penetration network and endowing the composites with a maximal room-temperature power factor of 158.81 μW m–1 K–2 with 20 wt % of PE. The introduction of PE not only reduces thermal conductivity (out-of-plane) but also provides the composites with self-healing and good mechanical properties. The compounding method and penetration structure reported in this work are universal and enlightening in developing highly efficient TE composites with cost-effectiveness and good comprehensive properties for low-grade waste heat utilization.