Freely Shapable and 3D Porous Carbon Nanotube Foam Using Rapid Solvent Evaporation Method for Flexible Thermoelectric Power Generators

A rapid solvent evaporation method based on the triple point of a processing solvent is presented to prepare carbon nanotube (CNT) foam with a porous structure for thermoelectric (TE) power generators. The rapid solvent evaporation process allows the preparation of CNT foam with various sizes and shapes. The obtained highly porous CNT foam with porosity exceeding 90% exhibits a low thermal conductivity of 0.17 W m−1 K−1 with increased phonon scattering, which is 100 times lower than that of a CNT film with a densely packed network. The aforementioned structural and thermal properties of the CNT foam are advantageous to develop a sufficient temperature gradient between the hot and cold parts to enhance TE output characteristics. To improve the electrical conductivity and Seebeck coefficient further, p‐ and n‐molecular dopants are easily introduced into the CNT foam, and the optimized condition is investigated based on the TE properties. Finally, optimized p‐ and n‐doped CNT foams are used to fabricate a vertical and flexible TE power generator with a combination of series and parallel mixed circuits. The maximum output power and output power per weight of the TE generator reach 1.5 µW and 82 µW g−1, respectively, at a temperature difference of 13.9 K. As a flexible thermoelectric (TE) material, freely shapable and 3D porous carbon nanotube (CNT) foam is prepared via a rapid solvent evaporation method. The porous and vertical CNT structure exhibits low thermal conductivity owing to the increased phonon scattering effect. The flexible TE power generator exhibits a maximum output power of 1.5 µW at a temperature difference of 13.9 K.