Citation: YANG Dong-Hua, ZHAO Jun-Fu, ZHANG Jun-Liang, DOU Tao, WU Zhong-Hua, CHEN Zhong-Jun. Designed Synthesis and Crystallization of Fe-Al-EU-1 Zeolites Containing Framework-Iron[J]. Acta Physico-Chimica Sinica, ;2012, 28(03): 720-728. doi: 10.3866/PKU.WHXB201201031 shu

Designed Synthesis and Crystallization of Fe-Al-EU-1 Zeolites Containing Framework-Iron

1.
1. College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, P. R. China;
2. College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, P. R. China;
3. Key Laboratory of Catalysis, College of Chemical Engineering, China University of Petroleum-Beijing, Beijing 102249, P. R. China;
4. Research Institute of Special Chemicals, Taiyuan University of Technology, Taiyuan 030024, P. R. China;
5. Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100039, P. R. China

Received Date: 22 September 2011
Available Online: 3 January 2012
Fund Project: 国家重点基础研究发展规划项目(973) (2012CB215002) (973) (2012CB215002) 国家自然科学基金(20973123) (20973123)煤转化国家重点实验室开放基金(11-12-603)资助 (11-12-603)

Highly crystalline Fe-Al-EU-1 zeolites were hydrothermally synthesized in a HMBr₂-Na₂OAl₂O₃- SiO₂-Fe₂O₃-H₂O system by using hexamethonium bromide (HMBr₂) as a template. The physical and chemical properties, and the bonding state of Fe in the zeolite framework for the prepared Fe-Al-EU-1 samples were characterized by a series of techniques including X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetric-derivative thermogravimetric (TG-DTG) analysis, N₂ adsorption-desorption, solid-state nuclear magnetic resonance (NMR), UV-visible diffuse reflectance spectroscopy (UV-Vis DRS), and X-ray absorption fine structure (XAFS). The results show that with increasing the mass fraction of Fe in the original sol-gel, the unit cell volume of Fe-Al-EU-1 zeolite inflates; the zeolite doped with Fe causes an increase in its surface area (BET) from 272 to 365 m²·g^-1 and a reduced amount of template removal, as well as a decrease in decomposition temperature. Adding Fe ions into sol-gel also leads to lowered zeta potential, easily gathered colloidal particles, and increased shape of zeolite. The UV-Vis spectrum shows that there is a characteristic peak at about 220-250 nm with a sharply increased intensity due to the p-d transition of the bonding electrons from the 2p-orbital of O atom to the d-orbital of the four-coordinated Fe atom in the framework. Also at around 373 nm, the coordination bonding of fourcoordinated Fe atoms and adjacent Si－O groups leads to a d-d charge transition peak with an energy level splitting and increased peak intensity. The XAFS results show that with the crystallization process ing on, the pre-edge absorption peak for 1s→3d and main absorption peak for 1s→4p change significantly. Four-coordinated structural units of iron species formed from the original sol-gel samples are gradually transformed into a tetrahedral coordinated iron-silicon-oxygen skeleton, in which iron-siliconoxygen ionic structural unit is also transformed into skeleton iron species with a tetrahedral covalent bonding structure.
- Fe-Al-EU-1 zeolite,
- Bonding state,
- Crystallization,
- X-ray absorption fine structure,
- Physical and chemical property,
- Characterization
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