Origin of n type properties in single wall carbon nanotube films with anionic surfactants investigated by experimental and theoretical analyses.

We investigated the origin of n-type thermoelectric properties in single-wall carbon nanotube (SWCNT) films with anionic surfactants via experimental analyses and first-principles calculations. Several types of anionic surfactants were employed to fabricate SWCNT films via drop-casting, followed by heat treatment at various temperatures. In particular, SWCNT films with sodium dodecylbenzene sulfonate (SDBS) surfactant heated to 350 °C exhibited a longer retention period, wherein the n-type Seebeck coefficient lasted for a maximum of 35 days. In x-ray photoelectron spectroscopy, SWCNT films with SDBS surfactant exhibited a larger amount of sodium than oxygen on the SWCNT surface. The electronic band structure and density of states of SWCNTs with oxygen atoms, oxygen molecules, water molecules, sulfur atoms, and sodium atoms were analyzed using first-principles calculations. The calculations showed that sodium atoms and oxygen molecules moved the Fermi level closer to the conduction and valence bands, respectively. The water molecules, oxygen, and sulfur atoms did not affect the Fermi level. Therefore, SWCNT films exhibited n-type thermoelectric properties when the interaction between the sodium atoms and the SWCNTs was larger than that between the oxygen molecules and the SWCNTs.

Facile preparation of air-stable n-type thermoelectric single-wall carbon nanotube films with anionic surfactants.

Thermoelectric generators based on single-wall carbon nanotubes (SWCNTs) have great potential for use in wearable and skin electronics because of their lightweight and mechanically soft structure. However, the fabrication of air-stable n-type thermoelectric SWCNTs using conventional processes is challenging. Herein, we propose a facile process for fabricating air-stable n-type SWCNT films with anionic surfactants via drop casting followed by heat treatment. We examined different surfactants (Sodium Dodecyl Sulfate, Sodium Dodecylbenzene Sulfonate, and Sodium Cholate) and heat-treatment temperatures. The optimal SWCNT film maintained the n-type Seebeck coefficient for 35 days. Moreover, to further extend the n-type Seebeck coefficient maintenance, we periodically reheated the SWCNT film with a surfactant that had returned to the p-type Seebeck coefficient. The reheated film recovered the n-type Seebeck coefficient, and the effect of the reheating treatment lasted for several reheating cycles. Finally, we elucidated a simple mechanism for realizing an air-stable n-type Seebeck coefficient based on spectroscopic analyses of the SWCNT films.

Effects of different electrolytes and film thicknesses on structural and thermoelectric properties of electropolymerized poly(3,4-ethylenedioxythiophene) films.

The effects of the type of electrolyte and film thickness on the structural and thermoelectric properties of poly(3,4-ethylenedioxythiophene) (PEDOT) thin films on indium-tin-oxide (ITO) substrates prepared using electropolymerization were investigated. Two electrolytes were prepared using two different solvents: a water/methanol solvent (protic solvent) and acetonitrile (aprotic solvent) with 3,4-ethylenedioxythiophene (EDOT) and LiCF3SO3, typically included in electrolytes as dopants. The electrochemical properties of the two electrolytes were analyzed; it was found that the polymerization process for EDOT on an ITO substrate varied based on the electrolyte used. When the electropolymerization time was increased, the surface morphology of the PEDOT films prepared using the water/methanol solvent appeared to contain grains approximately 100 nm in size whereas the PEDOT films prepared using acetonitrile appeared to contain aggregated grains connected by polymeric networks. Even though there were differences in the surface morphology and chemical bonds determined using Fourier-transform infrared spectroscopy/attenuated total reflectance analysis, the thermoelectric properties were strongly dependent on the film thickness and were only weakly dependent on the type of electrolyte used. The highest power factor was 41.3 µW (m-1 K-2) for a PEDOT film with a thickness of 0.5 µm prepared using the water/methanol solvent electrolyte.