合成和合成后改性沸石 Y 以改善甲醇吸附性和抗焦炭形成性

IF 2.8 3区 材料科学 Q3 CHEMISTRY, PHYSICAL
Silicon Pub Date : 2024-07-24 DOI:10.1007/s12633-024-03089-3
Boumediéne Bensafi, Nadjat Chouat, Abdelkarim Maziz, Fatiha Djafri
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引用次数: 0

摘要

合成沸石 Faujasite Y,用 NH4+ 进行离子交换,然后煅烧,得到质子化的 H-Y 形式。随后的合成后改变包括用草酸进行不同持续时间(1 和 2 小时)的煅烧,得到的样品标记为 H-Y/1h 和 H-Y/2h。表征技术表明,尽管结晶度略有下降,但沸石 Y 结构依然存在,尤其是在 H-Y/2h 中。质子化和脱胶后,质地有所改善。NH3-TPD 分析表明,酸处理使沸石结构中的铝大量脱落,增加了处理样品中强酸位点的浓度。由于甲醇的动力学直径小、极性低,有利于其在微孔和分层孔中的扩散,因此在 25 ℃ 时,甲醇的吸附动力学表现为假二阶行为。在 35 ℃ 时,Na-Y、H-Y 和 H-Y/1h 样品表现出二阶动力学,表明沸石孔隙内的甲醇吸附动力学良好。对甲醇吸附的 DTG 研究表明,分层孔隙率的产生有效地抑制了焦炭的形成,从而保持了催化活性,这一点在高温下的 H-Y/2h 中可以看到。这些发现凸显了合成后处理在提高沸石-Y 催化剂的甲醇吸附性和抗焦性方面的重要作用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Synthesis and Post-synthesis Modification of Zeolite Y for Improved Methanol Adsorption and Coke Formation Resistance

Zeolite Faujasite Y was synthesized, ion-exchanged with NH4+, and calcined to provide the protonated H-Y form. Subsequent post-synthesis alterations included dealumination with oxalic acid for varied durations (1 and 2 h), resulting in samples labeled as H-Y/1h and H-Y/2h. Characterization techniques demonstrated the persistence of the zeolite Y structure despite minor crystallinity loss, particularly in H-Y/2h. Textural improvements were seen following protonation and dealumination. NH3-TPD analysis revealed that acid treatment resulted in considerable aluminum removal from the zeolite structure, increasing the concentration of strong acid sites in the treated samples. Methanol adsorption kinetics at 25 °C exhibited pseudo-second-order behavior due to its small kinetic diameter and low polarity, which facilitated diffusivity in micro- and hierarchical pores. At 35 °C, Na-Y, H-Y, and H-Y/1h samples exhibited second-order kinetics, indicating favorable methanol adsorption dynamics within zeolite pores. DTG study of methanol adsorption showed that hierarchical porosity creation efficiently suppressed coke formation, hence conserving catalytic activity, as seen in H-Y/2h at high temperatures. These findings highlight the crucial significance of post-synthesis treatments in increasing methanol adsorption and imparting coke resistance to zeolite-Y catalysts.

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来源期刊
Silicon
Silicon CHEMISTRY, PHYSICAL-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
5.90
自引率
20.60%
发文量
685
审稿时长
>12 weeks
期刊介绍: The journal Silicon is intended to serve all those involved in studying the role of silicon as an enabling element in materials science. There are no restrictions on disciplinary boundaries provided the focus is on silicon-based materials or adds significantly to the understanding of such materials. Accordingly, such contributions are welcome in the areas of inorganic and organic chemistry, physics, biology, engineering, nanoscience, environmental science, electronics and optoelectronics, and modeling and theory. Relevant silicon-based materials include, but are not limited to, semiconductors, polymers, composites, ceramics, glasses, coatings, resins, composites, small molecules, and thin films.
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