催化学报

催化学报 ›› 2012, Vol. 33 ›› Issue (2): 348-353.DOI: 10.3724/SP.J.1088.2012.10919

• 研究论文 • 上一篇    下一篇

还原温度对 Ir/ZrO2 催化剂上巴豆醛选择性加氢的影响

朱琳, 鲁继青, 谢冠群, 陈萍, 罗孟飞   

  1. 浙江师范大学物理化学研究所, 浙江省固体表面反应化学重点实验室, 浙江金华 321004
  • 收稿日期:2011-09-13 修回日期:2011-10-20 出版日期:2012-02-20 发布日期:2015-07-27

Effects of Reduction Temperature on Selective Hydrogenation of Crotonaldehyde over Ir/ZrO2 Catalyst

ZHU Lin, LU Jiqing, XIE Guanqun, CHEN Ping, LUO Mengfei*   

  1. Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang, China
  • Received:2011-09-13 Revised:2011-10-20 Online:2012-02-20 Published:2015-07-27

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摘要： 采用浸渍法制备了负载型 Ir/ZrO2 催化剂, 详细考察了 H2 还原温度对 Ir/ZrO2 催化剂上气相巴豆醛选择性加氢反应性能的影响. 结果表明, 随着还原温度的升高, Ir/ZrO2 催化剂上巴豆醛转化率和巴豆醇选择性均先升后降. 400 °C 下还原时, Ir/ZrO2 催化剂性能最佳, 巴豆醛转化率和巴豆醇选择性分别达 32.2% 和 74.3%. X 射线光电子能谱结果表明, 催化剂表面系 Ir0 和 Ir3+ 共存, 且随着还原温度的升高, Ir0 的比例逐渐增加, 至 600 oC 时, 表面 Ir 物种大部分以 Ir0 存在. NH3 程序升温脱附结果表明, 随着还原温度的升高, 催化剂表面 Lewis 酸中心的数目减少, 强度下降. 这是由于催化剂中 Cl 含量下降所致. Ir0 和 Ir3+ 共存和中等强度的表面 Lewis 酸中心有利于提高巴豆醇选择性.

关键词: 铱, 氧化锆, 负载型催化剂, 巴豆醛, 选择性加氢, 巴豆醇, Lewis 酸

Abstract: The Ir/ZrO2 catalyst was prepared by impregnation, and the effect of reduction temperature on its catalytic performance for hydrogenation of crotonaldehyde in gas phase was measured. With increasing reduction temperature, the crotonaldehyde conversion and selectivity for crotyl alcohol over the Ir/ZrO2 catalyst first increase and then decrease. The catalyst reduced at 400 oC exhibits the highest crotonaldehyde conversion, reaching a value as high as 32.2%, and the selectivity for ctotyl alcohol is 74.3%. The results of X-ray photoelectron spectroscopy indicated that both Ir0 and Ir3+ species coexist on the catalyst surface after reduction at 400 oC. With increasing reduction temperature, the ratio of Ir0/Ir3+ increases, and the surface Ir species exists mainly as Ir0 when the reduction temperature is 600 oC. Additionally, NH3 temperature-programmed desorption indicated that the amount and intensity of Lewis acid sites show a downward trend with increasing reduction temperature, which is attributed to the decline of Cl element in the catalyst. Therefore, it is concluded that the coexistence of Ir0 and Ir3+ and moderate-intensity of surface Lewis acid help improve the yield and selectivity of crotyl alcohol.

Key words: iridium, zirconium dioxide, supported catalyst, crotonaldehyde, selective hydrogenation, crotyl alcohol, Lewis acid