Facile and Nondestructive Transformation of Intrinsic Hydrophobic Behavior of a Carbon Nanotubes Sheet to Hydrophilic

It is imperative to induce hydrophilicity in intrinsically hydrophobic carbon nanotubes (CNTs) without losing their superior properties for applications that specifically deal with aqueous media. A method for transforming a CNTs sheet from hydrophobic to hydrophilic by treatment with N-methyl-2-pyrrolidone (NMP) is explored. The NMP-treated CNT sheets are assessed based on complementing characterization, and it is concluded that the binding of NMP to a CNTs surface is through noncovalent interaction without the incorporation of defects in CNTs. The induced hydrophilicity in the CNTs sheet is stable for water exposure over a longer duration while it displays a semireversible nature upon heat treatment. The mechanical and electrical properties of the NMP-treated CNTs sheet revealed enhancement in the tensile strength from 221 to 421 MPa while maintaining a good electrical conductivity of ∼1.22 × 104 S/m because of the improved interfacial properties. The hydrophilic CNTs exhibited excellent adsorption capacity for methylene blue dye. The NMP-treated CNTs sheets demonstrated their suitability in flexible hybrid supercapacitor (FHSC) devices with improved electrochemical performance with enhancement in the capacitance from 5.4 to 7.6 F/g and a decrease in the equivalent series resistance from 53 to 34 Ω compared to pristine CNTs-based devices. These solid-state FHSC devices displayed excellent cyclic charge–discharge performance along with robust behavior over thousands of bending cycles without significant performance degradation. The excellent dye removal capability and superior electrochemical performance of the NMP-treated CNTs sheet is a consequence of their improved interface with aqueous media, which is governed by the hydrophilic nature of the CNTs sheet.