Edge-Functionalized Graphene Nanoribbon Frameworks for the Capture and Separation of Greenhouse Gases

We demonstrate a bottom-up synthetic approach for the synthesis of graphene nanoribbon frameworks (GNFs) incorporating edge-functionalized graphene nanoribbons via the Diels–Alder cycloaddition polymerization and a subsequent FeCl 3 -catalyzed cyclo-dehydrogenation reactions. This approach not only allowed us to precisely position substituents, namely, −OMe (GNF-0), −H (GNF-1), −CF 3 (GNF-2), and −F (GNF-3), but also enabled to tune textural properties and gas affinity of resulting frameworks. GNFs exhibited promising physical properties such as high surface areas (up to 755 m 2 g –1 ) and excellent physicochemical and thermal stabilities (up to 400 °C). Narrow pore size distribution and the presence of large aromatic units led to high affinity toward gases such as CO 2 (27.4–30.9 kJ mol –1 at 1 bar), CH 4 (21.3–26.0 kJ mol –1 at 1 bar), and H 2 (6.5–8.2 kJ mol –1 at 1 bar). Notably, GNF…