Ionic copolymer-modified hexagonal carbon nitride tube as a high-performance catalyst for regioselective synthesis of hexahydroquinoline frameworks

Abstract

The conventional structure of carbon nitride materials presents limitations, especially in the catalysis field, attributed to a restricted number of active sites and a low surface area. To address these challenges, we developed a unique design for a mesoporous carbon nitride tube (CNT), which was constructed by incorporating the ionic imidazole-epichlorohydrin copolymer ([IMEP][Cl]) as a template in the fabrication process. The self-assembly behavior of [IMEP][Cl] influences the formation of the melamine-cyanuric acid aggregate (as precursors) through electrostatic forces and polarity, potentially resulting in the creation of a thin-wall CNT with unique pore morphology. Synthesized three-dimensional hollow CNT demonstrated key factors of a high-performance catalyst in terms of high thermal stability (up to 550 °C), good specific surface area (108 m²/g), and significant recoverability (seven runs without a significant decrease in reaction yield). The CNT architecture was employed as a heterogeneous catalyst, and its catalytic efficiency was investigated in the regioselective synthesis of hexahydroquinoline ring systems. Based on the obtained results, CNT shows super-fast synthesis (5 min) of different pharmaceutical quinoline frameworks with exceptional yields (94–98 %) under ultrasound agitations. For the first time, an effective synthesis method is introduced for constructing hollow carbon nitride tubes, utilizing an ionic polymer (produced via chemical crosslinking rather than radical chain polymerization) as a template. This work offers a new viewpoint on improving the catalytic capability of traditional graphitic carbon nitrides through the utilization of ionic copolymers, presenting potential advancements for various technological applications.