铑/亚磷酰胺催化剂与 ZSM-35(10)协同催化烯烃的串联加氢甲酰化-缩醛化反应。
Co-catalysis of rhodium/phosphoramidite catalyst and ZSM-35(10) for the tandem hydroformylation-acetalization of olefins.
机构信息
Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, MOE, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, P. R. China.
Shandong Provincial Key Laboratory of Molecular Engineering, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, P. R. China.
出版信息
Chem Commun (Camb). 2023 Apr 27;59(35):5237-5240. doi: 10.1039/d3cc00488k.
The Rh/BINAPa and ZSM-35(10) co-catalyzed tandem hydroformylation-acetalization of olefins has been developed. A series of olefins with various alcohols performed well in the process, affording the corresponding acetals with high regioselectivities (l/b ≥ 30.5) and excellent catalytic activities (TON of the Rh catalyst up to 4.3 × 10). Control experiments and DFT calculations indicated that the Rh/L11-catalyzed hydroformylation occurred in the solvent outside the molecular sieve, while the acetalization of intermediate aldehydes with alcohols takes place mainly in the interior of the molecular sieve.
开发了 Rh/BINAPa 和 ZSM-35(10)共催化的串联烯烃氢甲酰化-缩醛化反应。一系列具有不同醇的烯烃在该过程中表现良好，以高区域选择性（l/b≥30.5）和优异的催化活性（Rh 催化剂的 TON 高达 4.3×10）得到相应的缩醛。控制实验和 DFT 计算表明，Rh/L11 催化的氢甲酰化反应发生在分子筛外的溶剂中，而中间醛与醇的缩醛化反应主要发生在分子筛内部。
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