Research investigations involving pristine carbon nanotubes (CNTs) and their applications in diversified fields have been gathering enormous impetus in recent times. One such emerging domain deals with the hybridization of CNTs within hydrogels to form soft nanocomposites with superior properties. However, till now, reports on the inclusion of pristine CNTs within low-molecular-weight hydrogels are very scarce due to their intrinsic feature of remaining in the bundled state and strong repulsive behavior to the aqueous milieu. Herein, the synthesis of a series of amino acid/dipeptide-based amphiphilic hydrogelators having a quaternary ammonium/imidazolium moiety at the polar head and a C16 hydrocarbon chain as the hydrophobic segment is reported. The synthesized amphiphiles exhibited excellent hydrogelation (minimum gelation concentration (MGC) ≈0.7–5 % w/v) as well as single-walled carbon nanotube (SWNT) dispersion ability in aqueous medium. Interestingly, the dispersed SWNTs were incorporated into the supramolecular hydrogel formed by amphiphiles with an imidazolium moiety at the polar end through complementary cation–π and π–π interactions. More importantly, the newly synthesized hydrogelators were able to accommodate a significantly high amount of pristine SWNTs (2–3.5 % w/v) at their MGCs without affecting the gelating properties. This is the first time that such a huge amount of SWNTs has been successfully incorporated within hydrogels. The efficient inclusion of SWNTs to develop soft nanocomposites was thoroughly investigated by spectroscopic and microscopic methods. Remarkably, the developed nanocomposites showed manifold enhancement (≈85-fold) in their mechanical strength compared with native hydrogel without SWNTs. The viscoelastic properties of these nanocomposites were readily tuned by varying the amount of incorporated CNTs.
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