天然气化工2016,Vol.41Issue(6):37-43,7.
还原温度和Cu负载量对乙二醇还原法制备的Cu/AC催化剂甲醇氧化羰基化反应性能的影响
Effect of reduction temperature and copper loading on the catalytic activity of Cu/AC catalysts prepared by polyol process for oxidative carbonylation of methanol
摘要
Abstract
The Cu/AC catalysts were prepared by the polyol process using activated carbon (AC) as support and ethylene glycol (EG) as reductant at different reduction temperature, and characterized by XRD, XPS, AAS, H2-TPR and TEM. The effect of reduction temperature and copper loading on the catalytic performance of Cu/AC catalysts for liquid-phase oxidative carbonylation of methanol to dimethyl carbonate was investigated. The results showed that Cu2+ were gradually reduced to Cu2O and Cu0 with the elevated reduction temperature. When the reduction temperature was 160℃, the content of Cu2O attained the highest with small crystalline size, and the corresponding catalyst exhibited the best catalytic activity. When copper loading was below 2.8% by mass, the Cu species could be highly dispersed on AC surface, resulting in catalytic activity improving with increasing Cu loading, and increasing copper loading to above 2.8% caused the agglomeration of Cu species and thus the catalytic activity decreased. Over the optimal catalyst, DMC space-time yield, selectivity and methanol conversion were 670mg·g-1·h-1, 91.7%and 6.0%, respectively.关键词
碳酸二甲酯/Cu/AC催化剂/乙二醇还原法/还原温度/负载量Key words
dimethyl carbonate/Cu/AC catalyst/polyol reduction method/reduction temperature/copper loading分类
化学工程引用本文复制引用
闫俊芬,张国强,郑华艳,李忠..还原温度和Cu负载量对乙二醇还原法制备的Cu/AC催化剂甲醇氧化羰基化反应性能的影响[J].天然气化工,2016,41(6):37-43,7.基金项目
国家自然科学基金(21276169,U1510203)。 (21276169,U1510203)