ReOx/ZrO2催化甲醇一步合成二甲氧基甲烷的研究

利用负载型ReOxZrO2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。

One-step synthesis of dimethoxymethane from methanol over ReOx/ZrO2

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.