Journal of the American Chemical Society · 2007 · 137 citations · 12 references
Natural SciencesChemical EngineeringChemistryCatalysisNanomaterialsSurface ScienceCatalyst DesignCatalyst PreparationCatalytic MaterialsCatalytic Reactor DesignNanocatalysisSurface CatalysisCarbon DioxideCatalytic Process OptimizationCo-precipitationMetal Oxide NanocatalystsMild Reaction ConditionsNanostructured CatalystsSelectivitySurface Coverage
Chemical fixation of CO 2 has recently attracted attention as a possible way to manufacture useful chemicals. Here, we demonstrate a one-step catalytic fixation of CO 2 to methyl formate (MF) in liquid phase under mild industrial applicable conditions by using a new concept of coupling surface formate species formed from CO 2 on solid catalyst with excess methanol in hydrogen to form the MF, and the quantity of the product is found to greatly exceed the surface coverage of the catalyst by >45-fold. As a result, we report, for the first time, that the optimum Pd/Cu/ZnO/alumina nanocatalyst prepared from simple co-precipitation is capable of activating gaseous CO 2 to condensable MF at high yields (>20%) with excellent selectivity (>96%). The present study also offers directions to rationally design and optimize the required catalyst, reactor, and experimental conditions for this new reaction.
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