Foldable Thermoelectric Materials: Improvement of the Thermoelectric Performance of Directly Spun CNT Webs by Individual Control of Electrical and Thermal Conductivity

We suggest the fabrication of foldable thermoelectric (TE) materials by embedding conducting polymers into Au-doped CNT webs. The CNT bundles, which are interconnected by a direct spinning method to form 3D networks without interfacial contact resistance, provide both high electrical conductivity and high carrier mobility. The ZT value of the spun CNT web is significantly enhanced through two simple processes. Decorating the porous CNT webs with Au nanoparticles increases the electrical conductivity, resulting in an optimal ZT of 0.163, which represents a more than 2-fold improvement compared to the ZT of pristine CNT webs (0.079). After decoration, polyaniline (PANI) is integrated into the Au-doped CNT webs both to improve the Seebeck coefficient by an energy-filtering effect and to decrease the thermal conductivity by the phonon-scattering effect. This leads to a ZT of 0.203, which is one of the highest ZT values reported for organic TE materials. Moreover, Au-doped CNT/PANI web is ultralightweight, free-standing, thermally stable, and mechanically robust, which makes it a viable candidate for a hybrid TE conversion device for wearable electronics. When a 20 K temperature gradient is applied to the TE module consisting of seven p-n couples, 1.74 μW of power is generated.