摘要
利用负载型ReOx/ZrO2催化剂,将甲醇选择性氧化并一步合成二甲氧基甲烷。考察了反应时间、反应温度以及铼负载量对反应的影响。并利用N2吸附/脱附、X射线光电子能谱、氨程序升温脱附(NH3-TPD)和氢程序升温还原(H2-TPR)等手段对催化剂进行了表征。结果表明,较高的反应温度有利于提高甲醇的转化率,但对二甲氧基甲烷的选择性不利;催化剂上所负载铼的质量分数对甲醇转化率影响较大,在铼的质量分数为1.64%时转化率达到最大值25.1%;负载于ZrO2上的ReOx具有双功能催化性质:它既可作为氧化中心氧化甲醇,在还原后又可作为酸中心催化醇醛缩合。
The synthesis of dimethoxymethane(DMM) by selective oxidization of methanol over the catalyst rhenium supported on ZrO2 in a fixed-bed reactor was investigated.It was found that higher temperature may promote the conversion of methanol but reduce the selectivity of DMM.The loading of rhenium on the catalyst exhibits a significant influence on methanol conversion and a maximum methanol conversion is obtained at a rhenium loading of 1.64%.XPS,H2-TPR and NH3-TPD suggested that ReOx/ZrO2 acts as a bifunctional catalyst in the reaction: the ReOx supported on ZrO2 is able to oxidize methanol,and then the reduced active sites contribute to the condensation of HCHO and methanol to form DMM.
出处
《燃料化学学报》
EI
CAS
CSCD
北大核心
2007年第3期334-338,共5页
Journal of Fuel Chemistry and Technology
关键词
二甲氧基甲烷
选择性氧化
铼氧化物
氧化锆
dimethoxymethane
selective oxidation
methanol
rhenium oxide
zirconia