天然气化工Issue(3)：10-15,6.
助剂Ce对合成DMC的无氯Cu/AC催化剂结构和性能的影响
Effect of additive Ce on structure and catalytic performance of the Cl-free Cu/AC catalyst for synthesis of dimethyl carbonate
摘要
Abstract
The rare earth Ce was introduced to the Cu/AC catalyst by impregnating the activated carbon (AC) with a Ce (NO3)3 solution firstly and with a Cu (CH3COO)2 solution subsequently, and the effects of Ce loading on the structure of catalyst and the catalytic performance in synthesis of dimethyl carbonate (DMC) via gas phase oxidative carbonylation of methanol were investigated. The surface properties of catalyst were characterized by XRD, XPS and H2-TPR. The results showed that the Ce of 1%to 2% by mass pre-introduced in AC could interact with the post-impregnated Cu, which resulted in that the Cu (II) species were easily reduced to the dispersed Cu2O and Cu (0) species during thermal decomposition and thus improving the catalytic activity. The space time yield and selectivity of dimethyl carbonate could be up to 155.1mg·g-1·h-1 and 88.9%, respectively, under the reaction conditions of 130℃, CO/O2 volume ratio of 11 and GHSV of 3092h-1. However, when Ce was over loaded the Cu(0) became the main species of Cu in the catalyst and Cu2O species were fewer, which resulted in the reduction of catalytic activity.关键词
Cu/AC催化剂/助剂Ce/无氯催化剂/碳酸二甲酯/合成/氧化羰基化/甲醇Key words
Cu/AC catalyst/additive Ce/Cl-free catalyst/dimethyl carbonate/synthesis/oxidative carbonylation/methanol分类
化学化工引用本文复制引用
齐君,郭天玉,郑华艳,李忠..助剂Ce对合成DMC的无氯Cu/AC催化剂结构和性能的影响[J].天然气化工,2014,(3):10-15,6.基金项目
国家自然科学基金(批准号21276169)、山西省科技攻关项目(批准号20120321003-03) （批准号21276169）
