Zhai Shengliang, Zhang Ling, Sun Jikai, Sun Lei, Jiang Shuchao, Yu Tie, Zhai Dong, Liu Chengcheng, Li Zhen, Ren Guoqing
Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University, Qingdao, China.
Front Chem. 2022 Jul 19;10:957412. doi: 10.3389/fchem.2022.957412. eCollection 2022.
Single-atom catalysts (SACs) as the new frontier in heterogeneous catalysis have attracted increasing attention. However, the rational design of SACs with high catalytic activities for specified reactions still remains challenging. Herein, we report the rational design of a Pd-Pd synergistic structure on -pyridinedicarbonitrile-derived covalent triazine framework () as an efficient active site for CO hydrogenation to formate under ambient conditions. Compared with the catalysts mainly comprising Pd and Pd, this hybrid catalyst presented significantly improved catalytic activity. By regulating the ratio of Pd to Pd, we obtained the optimal catalytic activity with a formate formation rate of 3.66 mol·mol ·h under ambient conditions (30°C, 0.1 MPa). Moreover, as a heterogeneous catalyst, this hybrid catalyst is easily recovered and exhibits about a 20% decrease in the catalytic activity after five cycles. These findings are significant in elucidating new rational design principles for CO hydrogenation catalysts with superior activity and may open up the possibilities of converting CO under ambient conditions.
单原子催化剂（SACs）作为多相催化领域的新前沿已引起越来越多的关注。然而，合理设计对特定反应具有高催化活性的SACs仍然具有挑战性。在此，我们报道了在吡啶二腈衍生的共价三嗪框架（）上合理设计Pd-Pd协同结构，作为在环境条件下将CO加氢生成甲酸盐的高效活性位点。与主要由Pd和Pd组成的催化剂相比，这种混合催化剂的催化活性显著提高。通过调节Pd与Pd的比例，我们在环境条件（30°C，0.1 MPa）下获得了最佳催化活性，甲酸盐生成速率为3.66 mol·mol·h。此外，作为一种多相催化剂，这种混合催化剂易于回收，并且在五个循环后催化活性降低约20%。这些发现对于阐明具有优异活性的CO加氢催化剂的新合理设计原则具有重要意义，并可能开辟在环境条件下转化CO的可能性。
