关键词: 乙醇, 气相羰基化, 负载型催化剂, 丙酸乙酯, 羰基化

Abstract: A novel Mo/Ccatalyst, which are reduced in H₂ after sulfidizaing ammonium heptamolybdate with (NH₄)₂Saqueous solution, has a high activity and selectivity for ethanol vapor phase carbonylation to ethyl propionate without addition of any promoter in the feed. Ethanol carbonylation is carried out in a fixed bed reactor with a continuous flow system at atmospheric pressure. This catalyst has a higher initial activity and selectivity; the catalytic activity reaches steady state after carbonylation reaction for 30 min. Higher temperatures led to a sharp decrease of the carbonylation activity and to an increase of the selectivities of ethene and ether. The optimal reaction conditions are as follows: reaction temperature is 553 K; n(C₂H₅OH)/n(CO)=4/1; GHSV=4.0 L/(g cat·h). Under these conditions, the conversion of ethanol is 80%, the selectivity of ethyl propionate is 80.6% and the space-time yield is 1.157×10^-2 mol/(g cat·h). This result is surprisingly better than that of ethanol vapor phase carbonylation over Ni-Zn/Ccatalyst with addition of ethyl iodide promoter to the feed [n(C₂H₅OH)/n(C₂H₅I)=10/1], especially, this novel Mo/Ccatalyst has a significantly higher selectivity. No carbonylation product is found over Ni base catalyst without addition of the promoter. This research demonstrates that novel Mo/Ccatalyst may be promising for ethyl propionate production from the carbonylation of ethanol at atmospheric pressure, without requiring ethyl iodide as promoter. This novel catalyst is found to be a non-crystalline by X-ray diffraction. The Mo content in the catalyst is 10%.

Key words: Ethanol, Vapor phase carbonylation, Supported catalyst, Ethyl propionate, Carbonylation