USY zeolites with tunable mesoporosity designed by controlling framework Fe content and their catalytic cracking properties

USY zeolites with tunable mesoporosity designed by controlling framework Fe content and their catalytic cracking properties
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通过控制骨架Fe含量设计介孔可调的USY沸石及其催化裂化性能

DOI:
10.1016/j.micromeso.2015.02.004
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发表时间:
2015-07
影响因子:
5.2
通讯作者:
Honghai Liu
Honghai Liu
中科院分区:
材料科学2区
文献类型:
--
作者:
Xinmei Pang;Baojie Wang;Hongjuan Zhao;Honghai Liu

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通过在NaY骨架中引入Fe阳离子作为起始点,然后通过铵离子交换和蒸汽脱铁-脱铝处理,成功地制备了可调介孔材料。因此,介孔的孔径和体积取决于骨架铁的含量。采用X射线衍射(XRD)、N2物理吸附、TEM、DSC、Py-IR和27 Al MAS NMR等手段对沸石产物进行了表征。结果表明,采用水蒸汽连续脱铁-脱铝法制备的铁诱导介孔超稳Y(USYFe)分子筛的介孔体积均大于0.21 cm 3 g − 1,并具有较好的热稳定性。最高可达0.23 cm 3 g −1,比USY(0.15 cm 3 g −1)提高了53%以上,而酸度没有下降。此外,最可能的中孔分布可以被精细调节,通常在9-17 nm的范围内。此外,发现大的中孔(8-50 nm)令人惊讶地随着用于制备USYFe样品的Fe含量的增加而增加。在1,3,5-三异丙苯吸附质分子的催化裂化反应中,富中孔分子筛比USY具有更高的活性和更低的失活倾向。结果表明,通过预先设定的Fe位对沸石进行改性而形成的介孔材料有助于通过介孔向微孔中扩散,从而对催化性能产生积极影响。
Tunable mesoporosity was successfully generated by introducing Fe cations into the framework of NaY as starting points, and then by sequential ammonium ion exchange and steaming deferrization–dealumination treatment. Accordingly, the pore diameter and volume of mesopores depended on the content of framework Fe. The zeolite products were characterized by a complementary combination of X-ray diffraction (XRD), N2physisorption, TEM, DSC, Py-IR, and27Al MAS NMR. The results show that the mesopore volumes of the Fe-induced mesoporous ultra-stable Y (USYFe) zeolites, which prepared via sequential deferrization-dealumination by steaming, are all higher than 0.21 cm3g−1with an additional thermal stability. The highest one reaches 0.23 cm3g−1, over 53% of enhancement compared to USY (0.15 cm3g−1) without deteriorating acidity. Furthermore, the most probable mesopore distributions can be finely tuned, typically in the range of 9–17 nm. In addition, it is found that large mesopores (8–50 nm) are surprisingly boosted with the increase in the Fe content used for the preparation of USYFesamples. In the catalytic cracking of adsorbate molecule of 1,3,5-triisopropylbenzene, the mesopores-enriched zeolites exhibit higher activity and lower deactivation tendency than USY with time on stream. The results demonstrated that the mesoporous material originating from the modification of zeolite with the pre-set Fe sites aided the diffusion into and out of the micropores via mesopores, and thus produced a positive influence on the catalytic performance.
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