Higher alcohols are key intermediates used in chemical industries for the manufacture of fuels, fuel additives, plasticizers, detergents, and lubricants etc. Modified Fischer�Tropsch Cu-Fe based catalyst is one type of catalyst active for higher alcohols synthesis (HAS) from synthesis gas (syngas). A fundamental understanding of HAS from syngas on this type of catalyst is important for the development of catalysts with high activity and selectivity for this process. Three-dimensionally ordered macroporous (3DOM) Cu-Fe catalysts were prepared by using a facile glyoxylate route poly(methyl methacrylate) (PMMA) colloidal crystal template method. The catalytic activity and selectivity in the production of higher alcohols on these 3DOM Cu-Fe catalysts as well as their surface chemistries during catalysis were investigated. In situ studies of their surface chemistries during catalysis, using ambient-pressure X-ray photoelectron spectroscopy (AP�XPS), revealed the active sites of the 3DOM Cu-Fe catalysts for HAS. Combined with the techniques of ex situ XRD, HRTEM, M�ssbauer spectroscopy, we concluded that the high intrinsic activity of the 3DOM Cu-Fe catalysts was ascribed to three factors. First, the unique ordered structure has a large pore size and interconnected macroporous tunnels of the catalyst with a large accessible surface area improves the catalytic activity. Second, a high density of uniformly distributed defective Cu0 and H�gg carbide ?-Fe5C2 nanoparticles derived from the glyoxylate route helps to provide abundant, active, stable dual sites. Third, atomic steps on the Cu surface, induced by planar defects and lattice strain, serve as high-activity oxygenation sites; and active ?-Fe5C2 chain-growth sites surrounds the defective and strained form of Cu surface intimately, which results in a synergetic effect between the active and stable Cu�FexCy dual sites for higher alcohols synthesis.

In situ AP-XPS and catalytic performances of 3D ordered macroporous Cu-Fe catalysts for higher alcohols synthesis from syngas

248th National Meeting (2014)

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