以硝酸铜和可溶性淀粉为原料,经过溶胶-凝胶化过程、高温炭化和KOH活化得到炭负载铜催化剂(Cu/C),采用扫描电镜、透射电镜、X射线衍射、热重-差热分析仪、N2吸附和CO程序升温脱附对催化剂结构进行了表征,并考察了它在甲醇氧化羰基化合成碳酸二甲酯(DMC)反应中的催化活性.结果表明,活化温度和KOH用量对催化剂的表面结构及金属铜粒子尺寸影响显著,当活化温度为850℃,KOH:C=1(质量比)时,Cu/C催化剂的比表面积达到1690m2/g,铜纳米粒子平均晶粒尺寸为30.4nm,催化活性最高,DMC时空收率达到235.7mg·g-1·h-1,甲醇转化率和DMC选择性分别为1.6%和76.5%.
Carbon-supported Cu (Cu/C) catalyst was prepared from Cu(NO3)2 and starch, by the sol-gel method, subsequent high temperature carbonization and KOH activation. Catalyst samples were characterized by scanning and transmission electron microscopies, X-ray diffraction, thermogravimetric analysis, N2 adsorption-desorption and CO temperature-programmed desorption. Their catalytic performance in the oxidative carbonylation of methanol to dimethyl carbonate (DMC) in a fixed-bed reactor was investigated. The activation temperature and KOH content greatly influenced the catalyst microstructure and catalytic performance. The Cu/C catalyst prepared at activation temperature of 850℃ and KOH/C mass ratio of 1 exhibited the best catalytic activity. Its specific surface area and mean Cu particle size were 1690 m2/g and 30.4 nm, respectively. The space time yield was 235.7 mg·g-1·h-1, and the methanol conversion and selectivity for DMC were 1.6% and 76.5%, respectively.