Rational and wide-range tuning of CNT aerogel conductors with multifunctionalities

Different from conventional conductors, elastic 3D nanoarchitectured conductors have shown promise in developing various flexible devices. However, rational design and control of their microstructures to achieve desired physicochemical properties is challenging and lacks comprehensive and profound investigation. In this study, we report an interesting quantitative correlation between density and physical properties when highly porous CNT aerogels are densified, enabling a wide-range tuning of CNT 3D networked structures with different functions. Upon densification by compressing the original thickness of a CNT aerogel by 100 fold, a linear double-logarithmic structure-property relationship in terms of both thickness and density is witnessed, with the resultant density increased by a factor of 100 from 3 to 286 mg cm-3, Young's modulus by 20 times (5.0-105 kPa), electrical conductivity by 400 times (0.4-163 s cm-1), and thermal conductivity by 140 times (0.048-6.7 W m-1 K-1). It can be thus inferred that the CNT aerogel can be regulated with desired mechanical, electrical and thermal properties in a quantitative manner over a wide range, making it promising as a multifunctional aerogel conductor. As a proof, two pieces of CNT aerogel conductors tailored with high conductivity and low thermal conductivity are employed to fabricate a flexible TE device using a simple all-carbon design, which yields a typical power density of 27.5 μW cm-2 and stable outputs under various deformations, demonstrating a potential strategy for design and fabrication of low-cost, flexible and portable power-generation devices.