A Microwave-Assisted, Solvent-Free Approach for the Versatile Functionalization of Carbon Nanotubes

While the functionalization of carbon nanotubes (CNTs) has attracted extensive interest for a wide range of applications, a facial and versatile strategy remains in demand. Here, we report a microwave-assisted, solvent-free approach to directly functionalize CNTs both in raw form and in arbitrary macroscopic assemblies. Rapid microwave irradiation was applied to generate active sites on the CNTs while not inducing excessive damage to the graphitic network, and a gas-phase deposition afforded controllable grafting for thorough or regioselective functionalization. Using methyl methacrylate (MMA) as a model functional group and a CNT sponge as a model assembly, homogeneous grafting was exhibited by the increased robust hydrophobicity (contact angle increase from 30 to 140°) and improved structural stability (compressive modulus increased by 135%). Therefore, when our MMA-functionalized CNTs served as a solar absorber for saline distillation, high operating stability with a superior water evaporation rate of ∼2.6 kg m^-2 h^-1 was observed. Finally, to highlight the efficacy and versatility of this functionalization approach, we fabricated asymmetrically hydrophobic CNT sponges by regioselective functionalization to serve as a moisture-driven generator, which demonstrated a stable open-circuit voltage of 0.6 mV. This versatile, solvent-free approach can complement conventional solution-based techniques in the design and fabrication of multifunctional nanocarbon-based materials. © 2023 American Chemical Society.