Formylation with supercritical carbon dioxide over Ru/Al2O3 modified by phosphines:: heterogeneous or homogeneous catalysis?

被引：18
|
作者：
Rohr, M [1 ]
Grunwaldt, JD [1 ]
Baiker, A [1 ]
机构：
[1] Swiss Fed Inst Technol, ETH Honggerberg, Dept Chem & Appl Biosci, CH-8093 Zurich, Switzerland
来源：
JOURNAL OF CATALYSIS | 2005年 / 229卷 / 01期
关键词：
formylation of amines; 3-methoxypropylamine; supercritical carbon dioxide; Ru/Al2O3; phosphines; X-ray absorption spectroscopy; EXAFS; in situ spectroscopy;
D O I：
10.1016/j.jcat.2004.09.026
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：
The formylation of 3-methoxypropylamine with hydrogen and "supercritical" carbon dioxide over Ru-based catalysts was studied. In this solventless process, carbon dioxide acts as both reactant and solvent. Interestingly, Ru/Al2O3 modified by the phosphine 1,2-bis(diphenylphosphino)ethane (dppe) showed a high formylation activity at 100% selectivity, comparable to those of the homogeneous catalysts RuCl2(dppe)(2) and RuCl2(PPh3)(3). Analysis of the reaction mixture by ICP-OES and structural studies by in situ X-ray absorption spectroscopy discovered that the presence of the phosphine modifier led to the formation of a homogeneous ruthenium catalyst. (C) 2004 Elsevier Inc. All rights reserved.
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页码：144 / 153
页数：10
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