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机构地区:[1]辽宁石油化工大学化学化工与环境学部,辽宁抚顺113001 [2]中国石油化工股份有限公司抚顺石油化工研究院,辽宁抚顺113001
出 处:《工业催化》2015年第5期366-371,共6页Industrial Catalysis
基 金:中国石油化工股份有限公司资助项目(061202)
摘 要:采用浸渍法制备了不同载体和金属组分的系列负载型催化剂,考察对溴甲烷制二甲醚的催化活性,并采用XRD、TPR和BET进行表征。结果表明,铜基催化剂催化性能较好,且以Al2O3-1#为载体制备的催化剂催化性能更优。Cu O负载量较低时,具有较高的分散度;高温焙烧使催化剂的活性中心由分散态Cu O转变为晶相Cu O,导致Cu O利用率下降;添加助剂K可显著提高Cu O利用率。优选的催化剂制备条件为:以Al2O3-1#为载体,活性组分Cu O负载质量分数为5%,助剂K负载质量分数为0.8%,焙烧温度为350℃,此条件下制备的催化剂,CH3Br转化率和二甲醚选择性均为100%,催化剂的Cu O利用率达到88.04%;再生10次后,催化剂性能保持稳定,没有明显下降。The supported catalysts with different carriers and metal components were prepared by impreg- nation method and their catalytic activities for methyl bromide to dimethyl ether were investigated. The as-prepared catalysts were characterized by means of XRD, TPR and BET techniques. The results showed that copper based catalysts exhibited good catalytic performance, and the catalysts prepared with A1203-1# as the carrier possessed better properties than the catalysts with other carriers. CuO on the surface of the catalyst with low CuO loading had high dispersion. After the catalyst was calcined at high temperature, its active centre dispersion state of CuO was change into crystalline phase of CuO, which resulted in the decline of CuO utilization rate. The addition of K assistant could significantly improve the utilization rate of CuO. The optimal condition of catalyst preparation was as follows: Al2O3-1# as the carrier, active component CuO mass fraction 5% ,K assistant mass fraction 0.8% ,and calcination temperature 350℃. On the catalyst prepared under the optimal condition,both the conversion of CH3Br and the selectivity to dimethyl ether were 100% ,while the utilization rate of CuO reached 88.04%. After ten times regeneration, the performance of the catalyst was stable and had no obvious decline.
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