Scalable Fabrication of Multifunctional Freestanding Carbon Nanotube/Polymer Composite Thin Films for Energy Conversion

Translating the unique properties of individual single-walled carbon nanotubes (SWNTs) to the macroscale while simultaneously incorporating additional functionalities into composites has been stymied by inadequate assembly methods. Here we describe a technique for developing multifunctional SWNT/polymer composite thin films that provides a fundamental engineering basis to bridge the gap between their nano- and macroscale properties. Selected polymers are infiltrated into a Mayer rod coated conductive SWNT network to fabricate solar cell transparent conductive electrodes (TCEs), fuel cell membrane electrode assemblies (MEAs), and lithium ion battery electrodes. Our TCEs have an outstanding optoelectronic figure of merit σ_dc/σ_ac of 19.4 and roughness of 3.8 nm yet are also mechanically robust enough to withstand delamination, a step toward scratch resistance necessary for flexible electronics. Our MEAs show platinum utilization as high as 1550 mW/mg_Pt, demonstrating our technique’s ability to integrate ionic conductivity of the polymer with electrical conductivity of the SWNTs at the Pt surface. Our battery anodes, which show reversible capacity of ∼850 mAh/g after 15 cycles, demonstrate the integration of electrode and separator to simplify device architecture and decrease overall weight. Each of these applications demonstrates our technique’s ability to maintain the conductivity of SWNT networks and their dispersion within a polymer matrix while concurrently optimizing key complementary properties of the composite. Here, we lay the foundation for the assembly of nanotubes and nanostructured components (rods, wires, particles, <i>etc</i>.) into macroscopic multifunctional materials using a low-cost and scalable solution-based processing technique