NNN-Ru complexes catalyzed β-methylation of alcohols using methanol via borrowing hydrogen approach

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2025-02-15 DOI:10.1016/j.jcat.2025.116026
Mengxuan Bai, Ziying Zhong, Zhiqiang Hao, Xiaoyan Li, Jin Lin
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Abstract

The methyl groups-containing alcohols are important and valuable chemicals and pharmaceuticals. The development of efficient and sustainable methylation methods is highly desirable. Herein, the β-methylation of primary alcohols using methanol as a green and cost-effective methylating reagent has been successfully achieved with NNN-Ru complexes (Ru1-Ru5) as efficient catalysts. It was found that ligand electronics play a crucial role in catalyst activity. Overall, the complex Ru3 bearing bis-OMe substituents displayed the highest catalytic reactivity. The present catalytic system proceeded via borrowing hydrogen (BH) approach and exhibited broad substrate scope. A variety of alcohols such as 2-arylethanols, 3-arylpropanols and aliphatic chain alcohols were selectively methylated, affording the corresponding products in good to excellent yields.

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借氢法催化 NNN-Ru 复合物与甲醇的β-甲基化反应
含甲基的醇类是重要而有价值的化学品和药品。开发高效、可持续的甲基化方法非常必要。在此,以 NNN-Ru 复合物(Ru1-Ru5)为高效催化剂,以甲醇为绿色、经济的甲基化试剂,成功实现了伯醇的 β-甲基化。研究发现,配体电子元件在催化剂活性中起着至关重要的作用。总体而言,带有双-OMe 取代基的配合物 Ru3 显示出最高的催化反应活性。本催化体系通过借氢(BH)方法进行,具有广泛的底物范围。2-arylethanols 、3-arylpropanols 和脂肪族链醇等多种醇类都能被选择性地甲基化,并以良好到极佳的收率得到相应的产物。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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