A novel hydrogenation of carbon dioxide proceeds in the presence of a RU~(CO),~-KJ homogeneous catalytic system with successive formation of carbon monoxide, methanol and methane.
A series
of mononuclear Ru halogen carbonyl complexes, [PPN][Ru
X3 (CO)3] (X = Cl, Br, and I), were found to
catalyze the reverse water-gas shift reaction (RWGSR: H2 + CO2 → CO + H2O). The Ru species in
the reaction solution were investigated in situ using a high-pressure
IR spectroscopy apparatus, which showed that [RuCl3(CO)3]− was the exclusive Ru species when [PPN][RuCl3(CO)3] was used as a catalyst. On the basis of
the IR spectra of stepwise reaction experiments, a plausible reaction
mechanism for the mononuclear species is proposed.
Methanol, together with methane, is formed for the first time by homogeneous hydrogenation of CO2 using a catalytic system consisting of Ru3(CO)12 and alkaline iodides in N-methylpyrrolidone (NMP) solution at 240 °C. The time course of the reaction indicates the successive formation of CO, methanol, and then methane. The FT-IR analysis of the resulting reaction solutions reveals the formation of several species of ruthenium carbonyl anion and their mutual interchanges during the reaction. A mechanism for the overall reaction is proposed, based on these results.
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