甲醇气相羰基化负载型金属氯化物催化剂研究  

Study on Metal Chloride Supported Catalysts for Vapor Phase Carbonylation of Methanol

作　　者：彭峰[1] 傅小波[1] 郭慧[1] 顾星[1] 

机构地区：[1]华南理工大学化学工程系,广州510640

出　　处：《天然气化工—C1化学与化工》2003年第3期9-12,共4页Natural Gas Chemical Industry

基　　金：国家自然科学基金资助(2 990 3 0 0 3 )

摘　　要：以活性炭为载体,制备了FeCl3、CoCl2、NiCl2、CuCl2、ZnCl2一系列负载的金属氯化物催化剂,并对甲醇常压下直接气相羰基化反应进行了研究,实验发现以氯化镍的活性最高,氯化铜的选择性最好。通过对一系列双组分金属氯化物催化剂的研究发现,NiCl2 CuCl2/C与NiCl2/C催化剂相比甲醇转化率、羰化选择性都明显提高,羰化产物的收率提高了25%,其催化剂的最佳负载量分别是5%NiCl2和15%CuCl2。在新研制的NiCl2 CuCl2/C催化剂上,对甲醇直接气相羰化反应工艺条件进行了研究,结果表明此新催化剂活性高,稳定性好。优化的工艺条件为:反应温度300℃,甲醇进料浓度22 5%,CO空速3000L/kg cat/h,此时甲醇转化率达34 5%,醋酸甲酯选择性达94 7%(mol),产物时空收率为3 2mol/kg cat/h。A series of metallic chloride catalysts supported on activated carbon are prepared and tested for vaporphase carbonylation of methanol The results show that NiCl2/C has a high conversion of methanol, and CuCl2/C has a high selectivity to methyl acetate without addition of any promoter in the feed The order of activity of catalytic carbonylation is as follows: NiCl2/C >CuCl2/C> FeCl3/C >>CoCl2/C >ZnCl2/C A series of bimetallic chlorides supported catalysts are also prepared and tested for the same reaction The results show that NiCl2-CuCl2/C has a higher activity and selectivity than NiCl2/C, and the yield of methyl acetate increase by 25% The optimum component of composite catalyst is 5wt%NiCl2 and 15wt%CuCl2 This novel NiCl2-CuCl2/C catalyst has high activity and good stability for methanol vaporphase carbonylation The reaction conditions are optimized as follows: reaction temperature of 300℃, methanol concentration of 225mol% and carbon monoxide space velocity of 3000 L/kgcath Under the optimum conditions, methanol conversion of 345%, selectivity of 947mol% to methyl acetate, and spacetime yield of 32 mol AcOMe/kgcath are obtained 

关 键 词：甲醇 气相羰基化 催化剂 金属氯化物 醋酸甲酯 

分 类 号：O643[理学—物理化学] TQ426[理学—化学]