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.