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摘要: 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。Abstract: The synthesis of dimethoxymethane (DMM) by selective oxidization of methanol over the catalyst rhenium supported on ZrO2 in a fixedbed 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.
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Key words:
- dimethoxymethane /
- selective oxidation /
- methanol /
- rhenium oxide
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