催化学报 ›› 2010, Vol. 31 ›› Issue (6): 705-710.

• 研究论文 • 上一篇    下一篇

双杂原子 Fe-V-β 沸石的合成、表征及催化性能

肖质文, 何红运   

  1. 湖南师范大学化学生物学及中药分析教育部重点实验室, 湖南长沙 410081
  • 收稿日期:2010-06-25 出版日期:2010-06-25 发布日期:2013-12-05

Synthesis, Characterization, and Catalytic Behavior of Biheteroatomic Fe-V-β Zeolite

XIAO Zhiwen, HE Hongyun*   

  1. Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research of Ministry of Education, Hunan Normal University, Changsha 410081, Hunan, China
  • Received:2010-06-25 Online:2010-06-25 Published:2013-12-05

摘要: 采用水热合成法在 SiO2-Fe2O3-V2O5-(TEA)2O-H2O-NH4F 体系中合成了 Fe-V-β 沸石, 并用 X 射线衍射、红外光谱、固体漫反射光谱、热重-差热分析、扫描电镜-能量色散谱仪和等离子体发射光谱等技术对沸石样品进行了表征, 探讨了影响 Fe-V-β 沸石合成的因素. 结果表明, 按摩尔比组成SiO2:Fe2O3:V2O5:(TEA)2O:H2O:NH4F = 60:(0.1~0.75):(0.1~0.75):(17~18):(550~ 650):(30~50) 配制初始反应混合物, 可以制备出结晶良好的 Fe-V-β 沸石, 且 Fe 和 V 原子进入到沸石骨架. 所得 Fe-V-β (Si/(Fe+V) = 30) 沸石在 H2O2 氧化苯乙烯反应中表现出最高的催化活性, 苯乙烯转化率为 25.4%, 苯甲醛、苯乙醛和苯乙酮的选择性分别为 69.1%, 22.5% 和 4.1%.

关键词: 铁, 钒, β沸石, 水热合成, 苯乙烯, 氧化, 苯甲醛, 苯乙醛

Abstract: The Fe-V-β zeolite was hydrothermally synthesized in a SiO2-Fe2O3-V2O5-(TEA)2O-H2O-NH4F system. The structure and chemical composition of the zeolite samples were characterized by X-ray diffraction, infrared spectroscopy, thermogravimetry-differential thermal analysis, inductively coupled plasma-atomic emission spetrometry, scanning electron microscopy-energy dispersive spectrometry, and ultra-violet-visual diffuse reflection spectroscopy. The factors that affected the synthesis of Fe-V-β zeolite were investigated. The results indicated that the well-crystallized Fe-V-β zeolite could be synthesized from the precursor with SiO2:Fe2O3:V2O5:(TEA)2O:H2O:NH4F molar ratio of 60:(0.1–0.75):(0.1–0.75):(17–18):(550–650):(30–50), and the Fe and V atoms entered the framework of the zeolite. The as-synthesized Fe-V-β zeolite with Si/(Fe+V) = 30 showed higher catalytic activity in the oxidation of styrene using H2O2 as the oxidant. The styrene con-version was 25.4%, and the selectivity was 69.1% for PhCHO, 22.5% for PhCH2CHO, and 4.1% for PhCOMe, respectively.

Key words: iron, vanadium, β zeolite, hydrothermal synthesis, styrene, oxidation, benzaldehyde, benzeneacetaldehyde