摘要
The direct carbonylation of methanol, without any halide in the feed as apromoter, is presented. A series of Mo catalysts supported on activated carbon, γ-Al_2O_3 and SiO_2were prepared. The results show that the support greatly affects the Mo catalyst in the directvapor-phase carbonylation of methanol, and activated carbon is the best supports of the investigatedsupports. In addition, the relationships between adsorptions of NH_3 and CO and carbonylation ofmethanol were investigated. A novel sulfided Mo/C catalyst had high activity and selectivity for thevapor phase carbonylation of methanol to methyl acetate without the addition of a CH_3I promoter tothe feed. The reaction conditions were optimized at a reaction temperature of 573 K, a methanolconcentration of 23 mol% and a carbon monoxide space velocity of 3,000 L/(kg·h). Under theseoptimal conditions a methanol conversion of 50%, carbonylation selectivity of 80 rnol%, andspace-time yield of 8.0 mol/(kg·h) were obtained. The active phase of this novel sulfided Mo/Ccatalyst is the non-crystalline phase, and the active component is present as MoS_(2.5) on thesurface of the activated carbon.
The direct carbonylation of methanol, without any halide in the feed as apromoter, is presented. A series of Mo catalysts supported on activated carbon, γ-Al_2O_3 and SiO_2were prepared. The results show that the support greatly affects the Mo catalyst in the directvapor-phase carbonylation of methanol, and activated carbon is the best supports of the investigatedsupports. In addition, the relationships between adsorptions of NH_3 and CO and carbonylation ofmethanol were investigated. A novel sulfided Mo/C catalyst had high activity and selectivity for thevapor phase carbonylation of methanol to methyl acetate without the addition of a CH_3I promoter tothe feed. The reaction conditions were optimized at a reaction temperature of 573 K, a methanolconcentration of 23 mol% and a carbon monoxide space velocity of 3,000 L/(kg·h). Under theseoptimal conditions a methanol conversion of 50%, carbonylation selectivity of 80 rnol%, andspace-time yield of 8.0 mol/(kg·h) were obtained. The active phase of this novel sulfided Mo/Ccatalyst is the non-crystalline phase, and the active component is present as MoS_(2.5) on thesurface of the activated carbon.
基金
This work was supported by the National Nature Science Foundation of China (No.29903003).
