Carbonylation of Methanol Over Nickel-Copper Based Supported Catalysts

摘要

The results are reported concerning the production of methyl acetate in the halide-free vapor-phase methanol carbonylation (MC) over NiCl2-CuCl2 based catalysts on activated carbons and honeycomb cordierite supports. The formation of the MeOAc with the yield of 18% over nickel-copper chlorides on the BAC-A grade carbon support is shown to be facilitated by the optimal combination of the characteristics of the porous structure (mesopores with an average diameter of similar to 7 nm) and the surface acidity of the catalyst. 15% of MeOAc yield over NiCl2-CuCl2/cordierite, commensurate with the Y-MeOAc for NiCl2-CuCl2/AC, is achieved due to advantages of structured systems in comparison with the highly porous granular ones, including more efficient mass transfer and heat removal as well as the increased outputs per active components loadings. Using CuO-ZnO-NiO/Al2O3/cordierite (to generate CO as a carbonylation agent by MeOH decomposition) and NiCl2-CuCl2/AC(or cordierite) catalysts placed in series-connected flow-type reactors or in a single reactor with two different temperature zones provides producing methyl acetate in a carbon monoxide free gas feedstock with the MeOAc yields of 13-16.5% in "self-carbonylation" tandem process.