金属对钛硅分子筛TS-1催化丁二烯环氧化性能的影响

doi:10.1016/S1872-2067(11)60498-1

催化学报 ›› 2013, Vol. 34 ›› Issue (4): 789-797.DOI: 10.1016/S1872-2067(11)60498-1

金属对钛硅分子筛TS-1催化丁二烯环氧化性能的影响

吴妹^a,b, 丑凌军^a, 宋焕玲^a

a 中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室甘肃兰州730000;
b 中国科学院大学, 北京10049

收稿日期:2012-10-29 修回日期:2012-11-21 出版日期:2013-04-23 发布日期:2013-04-24
通讯作者: 宋焕玲
基金资助:
国家自然科学基金(21133011).

Effect of metals on titanium silicalite TS-1 for butadiene epoxidation

WU Mei^a,b, CHOU Lingjun^a, SONG Huanling^a

a State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, Gansu, China;
b University of Chinese Academy of Sciences, Beijing 100049, China

Received:2012-10-29 Revised:2012-11-21 Online:2013-04-23 Published:2013-04-24
Supported by:
This work was supported by the National Natural Science Foundation of China (21133011).

摘要/Abstract

摘要：

制备了不同金属改性的钛硅分子筛样品M-TS-1 (M = V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Cd, La, 负载量为1%), 并研究了其催化丁二烯环氧化反应的性能. 结果表明, V, Cr, Mn的加入导致H₂O₂无效分解, 因而在丁二烯环氧化反应中表现出较高的H₂O₂转化率和较低有效利用率; Fe, Co, Ni以及稀土金属La均在一定程度上促进了TS-1对H₂O₂的有效利用; Cu, Zn抑制了H₂O₂的转化, 使得H₂O₂转化率和有效利用率都较低; Cd有效提高了TS-1的催化活性, H₂O₂转化率和有效利用率均接近100%. 采用X射线衍射、N₂吸附-脱附、X射线光电子能谱、傅里叶变换红外光谱等手段表征了上述各金属的改性对TS-1骨架结构以及Ti活性中心周围电子环境的影响. 结果表明, 各M-TS-1样品的骨架结构都仍保持原有的MFI构型, 但是TS-1中Ti活性中心周围的电子环境受到来自各种金属的不同程度影响, 关联催化活性时没有特定的规律性.

关键词: 丁二烯, 环氧化, 乙烯基环氧乙烷, 金属, 钛硅分子筛

Abstract:

The titanium silicalite-1 (TS-1) modified by various metals (M-TS-1; M = V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Cd, La, 1% metals loading) catalysts were employed to catalyze butadiene epoxidation. The metals influenced the TS-1 activity in various ways. V, Cr, and Mn caused H₂O₂ decomposition. Although the H₂O₂ conversion was high, its utilization was relatively low. The introduction of Fe, Co, Ni, and La into TS-1 promoted the vinyloxirane (VO) yield and H₂O₂ utilization to some extent. Cu and Zn modification inhibited the H₂O₂conversion to VO, resulting in both low H₂O₂ utilization and conversion. We studied the influence of Cd on TS-1 and found that H₂O₂was almost totally converted to VO over the Cd-TS-1 catalyst, and the turnover number of VO reached 1197. Powder X-ray diffraction, N₂ adsorption and desorption, X-ray photoelectron spectroscopy, and Fourier transformed infrared spectra were employed to characterize the specific metal role at the Ti site in the M-TS-1 catalysts. The TS-1 remained as MFI structure with doped metals. The added metals effectively changed the electron environment of the Ti active site. However, no universal trend in behavior was observed for these metals.

Key words: Butadiene, Epoxidation, Vinyloxirane, Metal, Titanium silicalite-1

吴妹, 丑凌军, 宋焕玲. 金属对钛硅分子筛TS-1催化丁二烯环氧化性能的影响[J]. 催化学报, 2013, 34(4): 789-797.

WU Mei, CHOU Lingjun, SONG Huanling. Effect of metals on titanium silicalite TS-1 for butadiene epoxidation[J]. Chinese Journal of Catalysis, 2013, 34(4): 789-797.

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金属对钛硅分子筛TS-1催化丁二烯环氧化性能的影响

Effect of metals on titanium silicalite TS-1 for butadiene epoxidation

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