Qian Qingli, Cui Meng, He Zhenhong, Wu Congyi, Zhu Qinggong, Zhang Zhaofu, Ma Jun, Yang Guanying, Zhang Jingjing, Han Buxing
Beijing National Laboratory for Molecular Sciences , CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics , Institute of Chemistry , Chinese Academy of Sciences , Beijing 100190 , China . Email:
Chem Sci. 2015 Oct 1;6(10):5685-5689. doi: 10.1039/c5sc02000j. Epub 2015 Jul 10.
The hydrogenation of CO to produce alcohols with two or more carbons (C alcohols) is of great importance, but is challenging. In this work, we found that a Ru(CO)/Rh(CO)Cl-LiI system could catalyze the reaction effectively in 1,3-dimethyl-2-imidazolidinone (DMI) under mild conditions. Methanol, ethanol, propanol, 2-methyl propanol, butanol, and 2-methyl butanol were produced in the homogeneous catalytic reaction. The C alcohols could be generated at 160 °C, which is the lowest temperature reported so far for producing C alcohols CO hydrogenation. The selectivity for the C alcohols could be as high as 96.4% at the optimized conditions, which is higher than those reported in the literature. In addition, the catalytic system could be easily recycled. The route of the reaction for forming the C alcohols was discussed on the basis of control experiments.
将一氧化碳加氢生成含两个或更多碳原子的醇类（C醇）具有重要意义，但颇具挑战性。在本工作中，我们发现Ru(CO)/Rh(CO)Cl-LiI体系在温和条件下于1,3-二甲基-2-咪唑啉酮（DMI）中能有效催化该反应。在均相催化反应中生成了甲醇、乙醇、丙醇、2-甲基丙醇、丁醇和2-甲基丁醇。C醇可在160℃生成，这是迄今为止报道的一氧化碳加氢生成C醇的最低温度。在优化条件下，C醇的选择性可达96.4%，高于文献报道的值。此外，该催化体系易于循环使用。基于对照实验讨论了形成C醇的反应途径。
