{"title":"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","authors":"Ying Zhang, Liyang Liu, Ziyue Wang, Xingcong Zhang, Xiaohui He, Hongbing Ji","doi":"10.1007/s11426-024-2135-y","DOIUrl":null,"url":null,"abstract":"<div><p>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/Al<sub>2</sub>O<sub>3</sub>-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/Al<sub>2</sub>O<sub>3</sub>, Co/Al<sub>2</sub>O<sub>3</sub>, and their physically mixed counterparts. <i>In situ</i> 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.\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3706 - 3711"},"PeriodicalIF":10.4000,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Tandem hydroformylation/hydrogenation of olefins to alcohols using atomically dispersed bifunctional catalysts\",\"authors\":\"Ying Zhang, Liyang Liu, Ziyue Wang, Xingcong Zhang, Xiaohui He, Hongbing Ji\",\"doi\":\"10.1007/s11426-024-2135-y\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>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/Al<sub>2</sub>O<sub>3</sub>-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/Al<sub>2</sub>O<sub>3</sub>, Co/Al<sub>2</sub>O<sub>3</sub>, and their physically mixed counterparts. <i>In situ</i> 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.\\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":772,\"journal\":{\"name\":\"Science China Chemistry\",\"volume\":\"67 11\",\"pages\":\"3706 - 3711\"},\"PeriodicalIF\":10.4000,\"publicationDate\":\"2024-08-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science China Chemistry\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11426-024-2135-y\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science China Chemistry","FirstCategoryId":"1","ListUrlMain":"https://link.springer.com/article/10.1007/s11426-024-2135-y","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
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。
Tandem hydroformylation/hydrogenation of olefins to alcohols using atomically dispersed bifunctional catalysts
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.
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.
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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.
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