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

来源：

CHEMCATCHEM | 2019年 / 11卷 / 21期

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

页码：5269 / 5274

页数：6

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