Multiwalled carbon nanotubes (MWCNTs) were incorporated into highly concentrated water-in-oil emulsions with the ultimate aim of achieving a uniform and effective dispersion of MWCNTs within the emulsion matrix. The emulsion was formulated in such a way, wherein the internal phase consists of higher than 90 wt %. By keeping the same aqueous-to-oil phase ratio, the amount of MWCNTs in the oil phase was systematically adjusted to investigate their effects on the microstructure development and rheological behavior of the emulsion. The addition of MWCNTs led to a reduced droplet size and also resulted in a narrower distribution of the droplet size. The rheological behavior of nanotube-incorporated emulsions was characterized with varying MWCNT concentrations and also as a function of the emulsification time. The rheological characteristics of the nanotube-incorporated emulsions were identical to those of the neat emulsion and were primarily governed by the variation in the droplet size and droplet-size distribution. However, the yield strain and cross-over strain were independent of the mean droplet size and polydispersity of the emulsion. Emulsions that have smaller droplets exhibited higher storage modulus (G'), yield stress (τY), and apparent viscosity (η). For all refining times investigated, nanotube-incorporated emulsions have higher G', τY, and η values when compared to the neat emulsion, and these values further increased with the MWCNT concentration. This was primarily due to the decrease in the droplet size with MWCNT addition. Furthermore, our findings suggest that the incorporated MWCNTs did not induce any significant change in the rheological behavior of emulsions with identical droplet sizes, and it remained essentially unchanged with the concentration of MWCNTs. However, the nanotube-incorporated emulsions possessed solidlike behavior up to a higher applied stress when compared to a neat emulsion of identical droplet size.

Highly concentrated water-in-oil emulsions incorporating multiwalled carbon nanotubes (MWCNTs) are prepared. Homogeneous and selective dispersions of MWCNTs throughout the oil phase of the emulsions are investigated. The practical insolubility of carbon nanotubes (CNTs) in aqueous and organic media necessitates the disentanglement of CNT "agglomerates" through the utilization of functionalized CNTs. The design and synthesis of two tetra-alkylated pyrene derivatives, namely, 1,3,6,8-tetra(oct-1-yn-1-yl)pyrene (TOPy) and 1,3,6,8-tetra(dodec-1-yn-1-yl)pyrene (TDPy), for the noncovalent organic modification of MWCNTs are reported. The modifier molecules are designed in such a manner that they facilitate an improved dispersion of individualized MWCNTs in the continuous-oil phase of the highly concentrated emulsion (HCE). Transmission electron microscopic analyses suggest that the alkylated pyrene molecules are adsorbed on the MWCNT surface, and their adsorption eventually results in the debundling of MWCNT agglomerates. Fourier transform infrared, Raman, and fluorescence spectroscopic analyses confirm the π-π interaction between the alkylated pyrene molecules and MWCNTs. The noncovalent modification significantly improves the effective debundling and selective dispersion of MWCNTs in HCEs.