A comprehensive study of a less harmful functionalization of multiwalled carbon nanotubes (MWCNT) was performed. The influence of ultrasonic cavitation and solid/liquid interface was indirectly evaluated by statistical characterization of MWCNT aspect ratio and degree of functionalization. MWCNT aspect ratio was determined through hundreds of electron microscopy images. Degree of functionalization of MWCNT was characterized by elemental analysis and thermogravimetry. Distribution of different oxygen-containing functional groups was assessed by potentiometric titration. MWCNT aqueous dispersions were evaluated by electrophoretic mobility and dynamic light scattering. An acid volume over 90% lower than usually reported in literature guaranteed MWCNTs with significantly larger aspect ratio, higher proportion of carboxylic groups and a more negative zeta potential in aqueous suspension. These results can be related to a more localized ultrasonic cavitation in MWCNTs/acid interface for reduced liquid volumes. This distinguished influence of ultrasonic cavitation may be a valuable contribution to more eco-friendly processes with nanomaterials.

The introduction of oxygen groups in carbon nanotubes is considered crucial for many applications. However, there is a lack of controlled functionalization methods which ensure nanotubes with specific property values according to each interest. In this work, acid treatments of multiwalled carbon nanotubes (MWCNTs) employing an optimized ultrasound process with moderate heating and stirring were studied by means of a factorial design. The functionalized nanotubes were characterized by thermogravimetry, elemental analysis, Raman spectroscopy, electron microscopy and water stability tests. Statistic models were fitted for the degree of functionalization and length reduction of MWCNTs. Temperature was identified as a key parameter to produce more functionalized MWCNTs with less structural damage. The properties of the functionalized MWCNTs can be tailored by the choice of parameters exploited in the statistical models developed to enable different end-use requests, such as for polymeric composites or bio-related applications, which is the original contribution of this work.

Multi-walled carbon nanotubes (MWCNTs) functionalized with amine and carboxyl groups were used to prepare polyurethane/MWCNT nanocomposites in two distinct concentrations: a lower value of 1 mass% (spray coating) and a higher one of ~50 mass% (buckypaper based). The MWCNT-NH2 sample contained only 0.5 mass% of amine groups, whereas MWCNT-COOH contained 5 mass% of carboxyl groups. The MWCNT functionalized with low amine group content showed improved thermal properties when compared to neat thermoplastic polyurethane (TPU) and MWCNT-COOH based nanocomposites. The electrical conductivity of the polyurethane elastomer was greatly increased from 10-12 to ~10-5 S cm-1in the 1 mass% nanotube composite and to 7 S cm-1for the MWCNT-NH2 buckypaper-based nanocomposite. Furthermore, the relative high content of functional groups in the MWCNT-COOH sample, which disrupt the sp²structure in the nanotube walls, led to inferior properties; for instance the conductivity of the buckypaper based composite is one order of magnitude lower when using MWCNT-COOH in comparison with the MWCNT-NH2. These results show the range of property design possibilities available with the elastomeric polyurethane nanocomposite by tailoring the functional group content and the carbon nanotube load.