Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
School of Chemical Engineering, Beijing Institute of Petrochemical Technology, Beijing, 102617, China.
Angew Chem Int Ed Engl. 2016 Aug 16;55(34):9902-7. doi: 10.1002/anie.201603556. Epub 2016 Jul 22.
Zn- and Na-modulated Fe catalysts were fabricated by a simple coprecipitation/washing method. Zn greatly changed the size of iron species, serving as the structural promoter, while the existence of Na on the surface of the Fe catalyst alters the electronic structure, making the catalyst very active for CO activation. Most importantly, the electronic structure of the catalyst surface suppresses the hydrogenation of double bonds and promotes desorption of products, which renders the catalyst unexpectedly reactive toward alkenes-especially C5+ alkenes (with more than 50% selectivity in hydrocarbons)-while lowering the selectivity for undesired products. This study enriches C1 chemistry and the design of highly selective new catalysts for high-value chemicals.
采用简单的共沉淀/洗涤法制备了 Zn 和 Na 调制的 Fe 催化剂。Zn 极大地改变了铁物种的尺寸,起到了结构促进剂的作用,而 Na 存在于 Fe 催化剂的表面改变了电子结构,使催化剂对 CO 活化非常活跃。最重要的是,催化剂表面的电子结构抑制了双键的加氢,并促进了产物的脱附,这使得催化剂对烯烃具有出乎意料的反应活性——尤其是 C5+烯烃(在烃类中具有超过 50%的选择性)——同时降低了对不需要的产物的选择性。这项研究丰富了 C1 化学,并为高价值化学品设计了高选择性的新型催化剂。