Composites of Graphene and Other Nanocarbons with Organogelators Assembled through Supramolecular Interactions

Carbon nanomaterials (CNMs), such as exfoliated graphene (EG), long‐chain functionalized EG, single‐walled carbon nanotubes (SWNTs), and fullerene (C60), have been investigated for their interaction with two structurally different gelators based on all‐trans tri‐p‐phenylenevinylene bis‐aldoxime (1) and n‐lauroyl‐L‐alanine (2) both in solution and in supramolecular organogels. Gelation occurs in toluene through hydrogen bonding and van der Waals interactions for 1 and 2 in addition to π–π stacking specifically in the case of 1. These nanocomposites provide a thorough understanding in terms of molecular‐level interactions of dimensionally different CNMs with structurally different gelators. The presence of densely wrapped CNMs encapsulated fibrous network in the resulting composites is evident from various spectroscopic and microscopic studies, indicating the presence of supramolecular interactions. Concentration‐ and temperature‐dependent UV/Vis and fluorescence spectra show that CNMs promote aggregation of the gelator molecules, leading to hypochromism and quenching of the fluorescence intensity. Thermotropic mesophases of 1 are altered by the inclusion of a small amount of CNMs. The gel–CNM composites show increased electrical conductivity compared with that of the native organogel. Rheological studies of the composites demonstrate the formation of rigid and viscoelastic solidlike assembly due to reinforced aggregation of the gelators on CNMs. Synergistic behavior is observed in case of the composite gel of 1, containing a mixture of EG and SWNT, when compared with other mixtures of CNMs in all combinations with EG. This affords new nanocomposites with interesting optical, thermal, electrical, and mechanical properties. Gelled together: Graphene and other nanocarbons were doped with two structurally different organogelators based on π‐stacking and van der Waals interactions, which determined their self‐assembly behavior (see figure) and brought about changes in the macroscopic behavior.