The interfacial issue is a critical
factor affecting the thermoelectric
performance in the organic–inorganic composite system. However,
in the traditionally adopted solution casting method for organic–inorganic
composites, it is difficult to tune the interface effectively. Herein,
as a proof-of-concept, high-performance polyaniline (PANI)/carbon
nanotube (CNT) thermoelectric (TE) composite films have been fabricated
by a green vacuum-assisted method through the interfacial morphology
control via a different solvent treatment. Morphological characterization
indicates that the PANI is successfully uniformly wrapped around the
surface of CNTs, and the interfaces are improved by proper treatment
with N,N-dimethylformamide (DMF)
solvent. Combining cold-pressure treatment for the vacuum-assisted
thin films further achieves higher electrical conductivity and a relatively
higher Seebeck coefficient through the enhancement of interfacial
adhesion. Ultimately, the composite films prepared with 90 wt % CNTs
show the highest TE properties, while the room-temperature electrical
conductivity and power factor reach 1965 S cm–1 and
114.4 μW·m–1·K–2 with DMF solvent treatment, respectively. Furthermore, the Seebeck
coefficient value increases with increase in temperature from room
temperature to 410 K, leading to a maximum power factor of 203 and
402 μW·m–1·K–2 for the 70 and 90 wt % CNT composite films, respectively. Our approach
using vacuum-assisted assembly method combining solvent and cold-pressure
treatment provides a good paradigm for developing high-performance
thermoelectric materials that benefit from interface engineering.