Tahta M. Karim, Hiroto Toyoda, Masato Sawada, Liang Zhao, Yong Wang, Peipei Xiao, Lizhuo Wang, Jun Huang and Toshiyuki Yokoi*,
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Furthermore, the influence of the hydrothermal synthesis time on the formation of the hierarchical structure and the arrangement of aluminum within the framework was also investigated. The prolongation of the hydrothermal synthesis time to 144 h was found to be an optimal period for the formation of a well-hierarchical structure, as demonstrated by the observed increase in the hierarchy factor. Moreover, this process resulted in an increase in the strength of the acid sites and a change in the crystal morphology of the hierarchical ZSM-5 from a coffin-like morphology to a coral reef-like or a flower-like morphology. Additionally, the influence of the alteration in the aluminum distribution on the catalytic performance was also investigated. In the case of the <i>n</i>-hexane cracking and methanol conversion reactions, hierarchical ZSM-5 with Na was observed to produce bulkier molecules (≥C5s) than that without Na. 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引用次数: 0
摘要
在我们之前的研究中,我们对添加和不添加钠(Na)的微孔 ZSM-5 上的铝分布进行了控制。在当前的研究中,我们对使用表面活性剂作为介孔剂合成的分层 ZSM-5 上的铝分布进行了调整。铝分布的研究基于 27Al MAS NMR、约束指数 (CI) 值和 Co(II) 离子吸附紫外可见光。上述表征结果表明,与不含 Na 的分层 ZSM-5 相比,含 Na 的分层 ZSM-5 在通道交叉处的铝分布更为集中。而微孔 ZSM-5 则呈现出相反的趋势。此外,还研究了水热合成时间对分层结构的形成和铝在框架内排列的影响。研究发现,将水热合成时间延长至 144 小时是形成良好分层结构的最佳时间段,这一点可以从观察到的分层系数增加中得到证明。此外,这一过程还增加了酸性位点的强度,并改变了分层 ZSM-5 的晶体形态,从棺材状形态变为珊瑚礁状或花朵状形态。此外,还研究了铝分布的变化对催化性能的影响。在正己烷裂解和甲醇转化反应中,观察到与不含 Na 的分层 ZSM-5 相比,含 Na 的分层 ZSM-5 产生的分子体积更大(≥C5s)。另一方面,与微孔 ZSM-5 相比,分层结构 ZSM-5 在生产低级烯烃(尤其是丙烯)方面表现出更高的性能。
Aluminum Distribution on the Microporous and Hierarchical ZSM-5 Intracrystalline and Its Impact on the Catalytic Performance
In our previous work, the control of aluminum distribution on microporous ZSM-5 with and without the addition of sodium (Na) was conducted. In the current research, adjustment of the aluminum distribution on hierarchical ZSM-5 synthesized using a surfactant as a mesoporogen has been carried out. The investigation of aluminum distribution was based on 27Al MAS NMR, constraint index (CI) value, and Co(II) ion-adsorbed UV–vis. The aforementioned characterizations revealed that the hierarchical ZSM-5 with Na exhibited a more concentrated aluminum distribution in the channel intersections than the hierarchical ZSM-5 without Na did. The opposite trend was observed with microporous ZSM-5. Furthermore, the influence of the hydrothermal synthesis time on the formation of the hierarchical structure and the arrangement of aluminum within the framework was also investigated. The prolongation of the hydrothermal synthesis time to 144 h was found to be an optimal period for the formation of a well-hierarchical structure, as demonstrated by the observed increase in the hierarchy factor. Moreover, this process resulted in an increase in the strength of the acid sites and a change in the crystal morphology of the hierarchical ZSM-5 from a coffin-like morphology to a coral reef-like or a flower-like morphology. Additionally, the influence of the alteration in the aluminum distribution on the catalytic performance was also investigated. In the case of the n-hexane cracking and methanol conversion reactions, hierarchical ZSM-5 with Na was observed to produce bulkier molecules (≥C5s) than that without Na. On the other hand, it was observed that the hierarchically structured ZSM-5 exhibited enhanced performance in the production of lower olefins, particularly propene, in comparison to the microporous ZSM-5.