关键词: 甲醇, 甲酸甲酯, 多相羰化, 负载液膜催化剂

Abstract: By using zeolite-supported alkali methoxide liquid-film catalysts, such as KOCH₃-PEG/NaZSM-5(or NaY), the heterogeneous catalytic carbonylation of methanol to methyl formate was realized in a fixed-bed continuous flow reactor. Under the reaction conditions of 353 K,1.0 MPa, feedgas composition of CO/CH₃OH=6.48(molar ratio) and GHSV=11160h^-1, the STYof MFreached up to 1900mg/(h·gcat.), with selectivity to MFat 100%.The experimental results indicated that methoxide anion CH₃O- was crucial catalyti-cally active species. The role of the additive polyethylene glycol(PEG) in generating a liquid-film environment, in which the carbonylation reaction would take place, is important,espe-cially in the case of supports with large pore-diameter as SiO₂. However, in the case of some support materials with abundant micropore structure such as ZSM-5 or Y-type zeolite, it is probable to design and select appropriate reaction conditions(mainly, temperature and partial pressure of methanol in feedstream) to generate directly liquid-film of methanol by means of the "capillary condensation effect", as a consequence, addition of PEGmay be cut down, or even, avoided.

Key words: Methanol, Methyl formate, Heterogeneous carbonylation, Supported liquid-film catalyst