| 赖群萍,万惠霖,伊晓东,华卫琦,翁维正.Mn对异丁烯选择氧化制甲基丙烯醛Mo-Bi-Fe-Co-Cs-K复合氧化物催化剂的促进作用及其机理[J].分子催化,2012,(1):10-18 |
| Mn对异丁烯选择氧化制甲基丙烯醛Mo-Bi-Fe-Co-Cs-K复合氧化物催化剂的促进作用及其机理 |
| Promotion Effect of Mn on the Mo-Bi-Fe-Co-Cs-K Composite Oxide Catalysts for Selective Oxidation of Isobutene to Methacrolein |
| 投稿时间：2012-01-19 修订日期：2012-02-26 |
| DOI： |
| 中文关键词: 异丁烯 选择氧化 甲基丙烯醛 锰 铋钼系氧化物催化剂 |
| 英文关键词:isobutene selective oxidation methacrolein (MAL) manganese Mo-Bi based catalyst |
| 基金项目:国家重点基础研究发展计划 (973 计划, 2010CB732303); 教育部创新团队 (No. IRT1036)；国家自然科学基金 (21033006, 20923004)和烟台万华聚氨酯股份有限公司资助项目 |
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| 中文摘要: |
| 采共沉淀法制备了系列异丁烯选择氧化制甲基丙烯醛（MAL）Mo-Bi基复合氧化物催化剂，在常压固定床流动反应体系上考察了Mn助剂及其添加方式对催化剂性能的影响，并结合对相关催化剂物相结构的表征，探讨了Mn的作用机理。研究表明，以Mn(NO3)2为前驱体将Mn引入Mo-Bi-Fe-Co-Cs-K复合氧化物可显著提高催化剂的异丁烯转化率，催化剂活性的改善源于Mn加入后有助于生成更多Bi3FeMo2O12物相，但该物相的增多对催化剂MAL选择性的影响不大。以MnMoO4为前驱体引入Mn可以进一步改善催化剂的性能，在400 ?C，空气：异丁烯 = 10:1 (体积比) 和GHSV = 2000 mL?g-1?h-1的反应条件下，异丁烯的转化率可达92.8 %，甲基丙烯醛的选择性最高可达93.5 %，催化剂经72 h反应后性能稳定。XRD测试结果表明，以MnMoO4为前驱体引入Mn有助于促进催化剂上生成衍射峰位于25.6和28.5 ?新物相，该物相的生成可大幅改善催化剂的选择性，进而显著提高催化剂在较高异丁烯转化率下的MAL得率。 |
| 英文摘要: |
| Mn promoted Mo based mixed oxide catalysts were prepared by coprecipitation method and were tested for selective oxidation of isobutene to methacrolein (MAL). Catalytic reaction were carried out in a fixed-bed micro-reactor at atmospheric pressure, while the properties of the catalysts were studied by BET and XRD. It was found that, with the generation of Bi3FeMo2O12, Mn(NO3)2 as precursor to introduce Mn to Mo-Bi-Fe-Co-Cs-K based catalyst can improve the conversion of the catalyst effectively, even though the Bi3FeMo2O12 phase certainly do not play much role in improving the selectivity of MAL. However, catalyst shows superior catalytic performance when using MnMoO4 as precursor instead of Mn(NO3)2, under suitable condition, the conversion of isobutene and the selectivity of MAL reach 92.8% and 93.5%, respectively. The performance is stable after the reaction for 72 h, XRD test shows that the excellent performance is closely related with the new phase called MX which would generate when Mn added with MnMoO4 as precursor. |
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