Integrated-Trifunctional Single Catalyst with Fine Spatial Distribution via Stepwise Anchored Strategy for Multistep Autotandem Catalysis
Shan‐Chao Ke, Ganggang Chang, Zhi‐Yi Hu, Ge Tian, Daiwen Yang, Xiaochen Ma, Kexin Huang, Jiaxin Li, Xiaoyu Yang
Abstract
Tandem catalysis that facilitates a series of consecutive catalytic reactions to perform in a concurrent behavior is regarded as one of the most important future directions for enabling sustainable chemical syntheses. However, a general and facile method to finely tailor the spatial distribution of varied catalytic sites in a single catalyst to prevent chemical incompatibility while working synergistically is highly demanded yet with grand challenges. Herein, a stable multifunctional catalyst simultaneous with antagonistic acid, base, and anchored metal sites was successfully integrated in a single system by using a stepwise anchored strategy. Through fine control, the accessible acid, base, and anchored metal sites could be tuned and controlled in a highly ordered arrangement, which ensures a highly efficient communication between the trifunctional catalytic sites while cooperatively contribute to tandem transformation process. As a result, when applied in a one-pot three-step deacetalization-Knoevenagel-hydrogenation (D-K-H) model reaction, the multifunctional single catalyst showed excellent catalytic performance with higher than 99% yield to benzylmalononitrile. More importantly, the catalytic performance and structure stability could be maintained even after successive eight recycle tests benefited from the strong ionic bonds formed between the acid–base pairs and N-metal interaction in the as-prepared single catalyst. This work provides a fresh strategy for the construction of multifunctional single catalyst, especially for the application in challenging autotandem catalysis.