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Room-Temperature Tandem Condensation-Hydrogenation Catalyzed by Porous C₃N₄ Nanosheet-Supported Pd Nanoparticles
- Renfeng Nie, Minda Chen, Yuchen Pei, Biying Zhang, Long Qi, Jingwen Chen, Tian Wei Goh, Zhiyuan Qi, Zhiguo Zhang, Wenyu Huang
- ACS sustainable chemistry & engineering 2018 v.7 no.3 pp. 3356-3363
- ambient temperature, carbon nitride, catalysts, catalytic activity, cyclohexanones, hydrogen, hydrogenation, nanoparticles, nanosheets, nitriles, palladium, surface area
- Tandem catalysis, often inspired by biological systems, offers many advantages in the synthesis of highly functionalized small molecules. NH₂-grafted porous C₃N₄ nanosheet with rich N species and surface area of 138 m²/g was fabricated via a NH₃-exfoliation method. After supporting Pd nanoparticles, the resulting bifunctional catalyst (Pd/C₃N₄–NH₂) could catalyze a one-step tandem condensation-hydrogenation reaction between ketones and nitriles to form α-alkylated nitriles at room temperature. Under 2 MPa H₂ for 8 h, Pd/C₃N₄–NH₂ could afford 99.7% cyclohexanone conversion and 99.8% selectivity without other side reactions, which is much higher than that of bulk C₃N₄-supported Pd. Compared with commonly used two-step processes, this one-step tandem reaction could largely shorten reaction time and allow condensation-hydrogenation to take place at room temperature. We also found that the hydrogenation step accelerated the condensation step, which increased the overall efficiency of the tandem transformation. This catalytic system demonstrates the design of a bifunctional catalyst with cooperative sites that allow the tandem reaction to take place in one step under mild conditions.