| 罗策琪,章轩语,洪笑,喻琴,鲁继青,王月娟,罗孟飞.助剂Fe对Ir/SiO2催化剂的巴豆醛选择性加氢性能的影响[J].分子催化,2014,(3):218-226 |
| 助剂Fe对Ir/SiO2催化剂的巴豆醛选择性加氢性能的影响 |
| Effect of Fe promotion on the performance of Ir/SiO2 catalysts for seletive hydrogenation of crotonaldehyde |
| 投稿时间：2014-02-24 修订日期：2014-04-04 |
| DOI： |
| 中文关键词: 铱 铁 巴豆醛 选择性加氢 巴豆醇 |
| 英文关键词:Iridium Iron crotonaldehyde selective hydrogenation crotyl alcohol |
| 基金项目:国家自然科学基金项目（面上项目，重点项目，重大项目） |
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| 中文摘要: |
| 摘要：以SiO2为载体采用分步浸渍法制备了Fe/Ir/SiO2催化剂, 考察了助剂Fe对Ir/SiO2催化剂气相巴豆醛选择性加氢性能的影响. 采用X射线粉末衍射(XRD)、CO化学吸附、H2-程序升温还原(H2-TPR)和拉曼光谱(Raman)等技术对催化剂进行了表征. 结果表明, 助剂Fe能有效提高Ir/SiO2催化剂的巴豆醛转化率和巴豆醇选择性. Fe含量为0.087 wt.%的0.087Fe/Ir/SiO2催化剂的反应性能最佳, 反应进行9 h的巴豆醛转化率36.9 %, 巴豆醇选择性83 %. 随着催化剂CO吸附量的下降(Fe覆盖的增加), 催化剂的转换频率（turn over frequency, TOF）明显增加, 这表明Fe促进Ir/SiO2催化剂表面活性位的加氢活性. 然而, Fe的掺杂使得Ir/SiO2催化剂存在明显的活性下降现象, 归因于Fe导致Ir/SiO2催化剂表面积炭和CO中毒. |
| 英文摘要: |
| Abstract： Fe/Ir/SiO2 catalysts were prepared by a two-step impregnation method, and the effect of Fe promotion on the performance on Ir/SiO2 catalysts for gas phase selective hydrogenation of crotonaldehyde was investigated. The catalysts were characterized by X-ray powder diffraction, H2 temperture-programmed reduction, and Raman spectroscopy. The results showed that Fe promotion was helpful to improve the conversion of crotonaldehyede and the selectivity to crotyl alcohol of Ir/SiO2 catalysts for selective hydrogenation of crotonaldehyde. The 0.087Fe/Ir/SiO2 catalyst containing 0.087 wt.% Fe had the best catalytic performance, with the crotonaldehyde conversion of 36.9 % and the selectivity to crotyl alcohol of 83 % obtained at steady state (9 h). Calculated turnover frequencies increased significantly with the decline in the adsorption amount of CO (increasing Fe coverage) on the catalyst, indicating that Fe promoted the activity of hydrogenation on surface active sites of Ir/SiO2 catalysts. However, the addition of Fe resulted in obvious decrease catalyst activity, which was attributed to the Fe promotion accelerated carbon deposition and CO poisoning on the Ir/SiO2 catalysts surface. |
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