甲醇气相羰基化非铑非卤素新催化体系研究Ⅲ.硫化的单组分Mo/C催化剂制备及羰化性能

Study on the halide and rhodium free catalytic system for vapor phase carbonylation of methanol Ⅲ. preparation of a novel sulfided Mo/C catalyst and its carbonylation behavior

采用硫化铵溶液硫化法制备的Mo/C催化剂经还原活化后具有很高的甲醇气相羰化活性与选择性。最佳的催化剂制备条件为 :Mo/S摩比为 1 /4、氢气还原温度为 450℃。最佳的羰化反应工艺条件为 :反应温度 2 80℃ ,CH3OH/CO进料摩比为 1 /2 ,CO的GHSV为 450 0L/(kgcat·h) ,此时甲醇转化率达 45 2 % ,醋酸甲酯选择性为77 8% ,产物时空收率高达 1 9 2 3mol/(kgcat·h)。

A novel Mo/C catalyst,which are reduced in H 2 after sulfidization with (NH 4) 2S in an aqueous solution,has a sighificantly higher activity and selectivity for vapor phase carbonylation of methanol The optimal conditions of catalyst preparation have been found:Mo/S molar ratio is 1/?4 ;temperature of catalyst reduction is 450℃ The optimal reaction conditions are also examined:reaction temperature is 280℃;CH 3OH/CO molar ratio is 1/?2; CO GHSV is 4500L/(kg·h) Under these conditions,the conversion of methanol is 45 2%;the selectivity of methyl acetate is 77 8mol% and the space time yield is 19 2mol/(kg·h)