Tandem hydroformylation/hydrogenation of olefins to alcohols using atomically dispersed bifunctional catalysts

IF 10.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Science China Chemistry Pub Date : 2024-08-16 DOI:10.1007/s11426-024-2135-y

Ying Zhang, Liyang Liu, Ziyue Wang, Xingcong Zhang, Xiaohui He, Hongbing Ji

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引用次数: 0

Abstract

Tandem hydroformylation/hydrogenation of olefins to alcohols is an appealing and challenging route that has received continuous interest. Herein, we report a bifunctional atomically dispersed Rh and Co catalyst (RhCo/Al₂O₃-10) prepared by a simple ball milling method that displays superior synergistic catalytic performance (>95% olefins conversion and >80% alcohols selectivity) and broad substrate scope for tandem hydroformylation/hydrogenation reaction, outperforming Rh/Al₂O₃, Co/Al₂O₃, and their physically mixed counterparts. In situ CO-DRIFTS, XPS, and kinetic experiments demonstrate that the electron interaction between Rh and Co atoms effectively lowers the apparent activation energy, thus promoting the tandem hydroformylation/hydrogenation reaction. This work not only presents a novel tandem hydroformylation/hydrogenation reaction system for converting olefins to alcohol but also throws light on the rational design of versatile bifunctional catalysts for on-demand synergistic catalysis.

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使用原子分散双官能催化剂串联加氢甲酰化/加氢将烯烃转化为醇

烯烃与醇的串联加氢甲酰化/加氢反应是一条极具吸引力和挑战性的路线，一直受到人们的关注。在此，我们报告了一种通过简单球磨法制备的双功能原子分散 Rh 和 Co 催化剂（RhCo/Al2O3-10），该催化剂在串联加氢甲酰化/加氢反应中表现出卓越的协同催化性能（95% 的烯烃转化率和 80% 的醇选择性）和广泛的底物范围，优于 Rh/Al2O3、Co/Al2O3 及其物理混合催化剂。原位 CO-DRIFTS、XPS 和动力学实验证明，Rh 原子和 Co 原子间的电子相互作用有效降低了表观活化能，从而促进了串联加氢甲酰化/加氢反应。这项研究不仅提出了一种将烯烃转化为酒精的新型串联加氢甲酰化/加氢反应体系，还为按需协同催化的多功能双功能催化剂的合理设计提供了启示。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

14.40

自引率

7.30%

发文量

3787

审稿时长

2.2 months

期刊介绍： Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.