期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 51, 页码 26500-26505出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202110910
关键词
carbon dioxide; carbon monoxide; decarbonylation; dehydrogenation; hydrogen; methanol
资金
- Max-Planck Society
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [90919832]
- Projekt DEAL
The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen using homogeneous molecular complexes, particularly those containing ruthenium and manganese with the MACHO ligand framework, showed promising catalytic activities. The metal complex was found to mediate the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation, resulting in gas mixtures with varying CO/H2 ratios.
The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and manganese comprising the MACHO ligand framework showed promising activities for this reaction. The molecular ruthenium complex [RuH(CO)(BH4)(HN(C2H4PPh2)(2))] (Ru-MACHO-BH) achieved up to 3150 turnovers for carbon monoxide and 9230 turnovers for hydrogen formation at 150 degrees C reaching pressures up to 12 bar when the decomposition was carried out in a closed vessel. Control experiments affirmed that the metal complex mediates the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation. Depending on the catalyst and reaction conditions, the CO/H-2 ratio in the gas mixture thus varies over a broad range from almost pure hydrogen to the stoichiometric limit of 1:2.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据