Aqueous phase carbon dioxide and bicarbonate hydrogenation catalyzed by cyclopentadienyl ruthenium complexes

被引:25
作者
Bosquain, Sylvain S. [1 ]
Dorcier, Antoine [2 ]
Dyson, Paul J. [2 ]
Erlandsson, Mikael [1 ]
Gonsalvi, Luca [1 ]
Laurenczy, Gabor [2 ]
Peruzzini, Maurizio [1 ]
机构
[1] CNR, ICCOM, I-50019 Florence, Italy
[2] Ecole Polytech Fed Lausanne, Inst Sci & Ingn Chim, CH-1015 Lausanne, Switzerland
关键词
catalysis; hydrogenation; carbon dioxide hydrogenation; ruthenium; water-soluble phosphines; cyclopentadienyl complexes;
D O I
10.1002/aoc.1317
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The water-soluble ruthenium(II) complexes [Cp'RuX(PTA)(2)]Y and [CpRuCl(PPh3)(mPTA)]OTf (Cp'= Cp, Cp*, X = Cl and Y = nil; or X = MeCN and Y = PF6; PTA = 1,3,5-triaza-7-phosphaadamantane; mPTA = 1-methyl-1,3,5-triaza-7-phosphaadamantane) were used as catalyst precursors for the hydrogenation Of CO2 and bicarbonate in aqueous solutions, in the absence of amines or other additives, under relatively mild conditions (100 bar H-2, 30-80 degrees C), with moderate activities. Kinetic studies showed that the hydrogenation of HCO3- proceeds without an induction period, and that the rate strongly depends on the pH of the reaction medium. High-pressure multinuclear NMR spectroscopy revealed that the ruthenium(II) chloride precursors are quantitatively converted into the corresponding hydrides under H-2 pressure. Copyright (c) 2007 John Wiley & Sons, Ltd.
引用
收藏
页码:947 / 951
页数:5
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