Carbon nanomaterials (fullerenes, carbon nanotubes, graphene, etc) are subjects of intense research due to their excellent electronic and optical properties. Our research aims at synthesizing carbon-rich nanotubes and two-dimensional polymers whose physical properties can be modulated through modification of their chemical nature. To achieve this goal, we use a “hybrid” strategy that relies on the transformation of well-organized carbon-rich precursors in the solid state using physical stimuli (light or heat). This strategy allows a good control over the structural parameters of the resulting nanomaterials. As precursors, we use small molecules possessing alkyne moieties that we further transform into a polydiacetylene (PDA) intermediates. These PDAs are further graphitized to yield various carbon nanomaterials:
To obtain nanotubes, we synthesize and self-assemble phenylacetylene macrocycles (PAM) that we irradiate to provide covalently-linked stable assemblies.
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In addition to nanotubes, we use this approach to prepare other nanoarchitectures such as nanoparticles (ChemComm 2012, 48, 10144), nanorods (Langmuir 2013, 29, 3446) and 2D layered materials (Chem. Sci. 2014, 5, 831).
Graphene nanoribbons (GNRs)
Recently, we have also been interested in the total synthesis of carbon nanomaterials. In this approach, we prepare the bottom-up, solution-phase synthesis of polychlorinated polyphenylenes that undergo a photochemical cyclodehydrochlorination (CDHC) reaction to provide well-defined graphene nanoribbons (GNRs). The CDHC reaction takes place in metal-free, mild reaction conditions and proceeds selectively without the formation of side-products. Moreover, the CDHC reaction is compatible with different heterocycles and provides better control over the edge configuration of nanographenes than the Scholl reaction. Using this approach, we have been able to prepare nanographenes (Angew. Chem. Int. Ed. 2016, 55, 2042), helical GNRs (Angew. Chem. Int. Ed. 2017, 56, 6213) and thiophene-edged GNRs (Angew. Chem. Int. Ed. 2018, in press.)