Base-Free Hydrogenation of Carbon Dioxide to Methyl Formate with a Molecular Ruthenium-Phosphine Catalyst

被引:32
|
作者
Westhues, Niklas [1 ]
Belleflamme, Maurice [1 ]
Klankermayer, Juergen [1 ]
机构
[1] Rhein Westfal TH Aachen, Inst Tech & Makromol Chem, Worringerweg 2, D-52074 Aachen, Germany
关键词
homogeneous catalysis; hydrogenation; methyl formate; ruthenium; N-triphos; formic acid; CO2; carbon dioxide; FORMIC-ACID; CO2; HYDROGENATION; ACTIVE-SITES; METHANOL; COMPLEXES; TRIPHOS; DISPROPORTIONATION; COORDINATION; REACTIVITY; LIGANDS;
D O I
10.1002/cctc.201900627
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Herein, a molecular ruthenium-phosphine catalyst system for the effective base-free methyl formate production from carbon dioxide is described. In detail, the novel [Ru(N-triphos(Cy))(tmm)] complex, bearing sterically demanding cyclohexyl groups in the triphos-ligand structure, enabled in combination with the Lewis acid Al(OTf)(3) the selective transformation of carbon dioxide to methyl formate with unprecedented activity. From a mechanistic perspective, in the initial step formic acid is formed, undergoing a consecutive Lewis acid promoted esterification with methanol to methyl formate. This selective transformation with carbon dioxide paves the way to versatile processes for important C-1 building blocks.
引用
收藏
页码:5269 / 5274
页数:6
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