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The development of high thermally conductive polymer composites with low filler content remains challenging in the field of thermal interface materials (TIMs). Herein, we fabricated a series of flexible fiber membranes (TMMFM) with high thermally conductive based on thermoplastic polyurethane (TPU) and acidified multiwalled carbon nanotubes (a-MWCNTs) via electrospinning and ultrasonic anchoring method. The SEM and TEM results demonstrated that the a-MWCNTs aligned along the fiber orientation in the membrane and anchored on the membrane surface strongly, which can establish the heat conduction path both in the horizontal and vertical directions. With the incorporation of 10 wt% a-MWCNTs, the horizontal direction (λ ∥ ) and vertical direction (λ ⊥ ) thermal conductivity value of TMMFM-5 was 3.60 W/mK and 1.79 W/mK, respectively, being 18 times and 10 times higher compared to pure TPU fiber membranes. Furthermore, the TMMFM maintained favorable flexibility of the TPU matrix because the small amount of a-MWCNTs only slightly hinders the mobility of the TPU molecular chain. The performance of the obtained TMMFM unveils their potential as a promising choice of flexible TIMs.

Flexible Fiber Membrane Based on Carbon Nanotube and Polyurethane with High Thermal Conductivity