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Seed-fused ZSM-5 nanosheet as a superior MTP catalyst: Synergy of micro/mesopore and inter/external acidity
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2018-10-02 , DOI: 10.1016/j.micromeso.2018.09.038
Yunshan Shang , Wugang Wang , Yanliang Zhai , Yu Song , Xiaomeng Zhao , Tong Ma , Jianhui Wei , Yanjun Gong

ZSM-5 nanosheet (NS) has an optimal diffusivity due to b-axis oriented two-dimensional structure, but the extra large external acidity results in the deactivation of the catalyst in methanol to propylene (MTP) reaction. The seed-fused ZSM-5 nanosheets (CNS-x) were synthesized by a seed induced method, the performance of samples was compared with one without seed. Further, the B-incorporation sample (B-CNS-5) was prepared with 5 wt% seed and boron acid. Revealing the importance of fusion effect of ZSM-5 seed on the nanosheet, especially the change in microstructure properties and its structure-effect relationship, which is not explicitly documented in previous work. With the seed amount increasing from 5 to 30 wt % in the gel, the crystallization time is largely shortened, along with the change in the resulting nanosheet, such as reduction of particle size and acid strength/external surface acidity, an increase of over 50% micropore volume. The CNS-x samples perform longer catalytic lifetime (168–226 h) compared to NS (103 h). CNS-5 displays an extremely high selectivity to propylene (C = 3) ∼54% and total light olefins (C = 2-C = 4) of∼84%. A super sample B-CNS-5 exhibits longest lifetime (302 h), achieving highest C = 3 yield due to change in the acid sites distribution and increase of extra weak acid sites. For the converted methanol (g/gcatalyst), the result is B-CNS-5 (966) > CNS-5 (525)> NS (324). In converse, the average coke selectivity (Sav, C) is B-CNS-5 (0.18‰) < the CNS-5 (0.29‰)< NS (0.47‰). This result offers new insight for MTP catalyst about the synergy of acidity and diffusion in the ZSM-5 nanosheet.



中文翻译:

种子融合的ZSM-5纳米片材是优异的MTP催化剂:微孔/中孔和内部/外部酸度的协同作用

ZSM-5纳米片(NS)由于b轴定向的二维结构而具有最佳的扩散率,但是过大的外部酸度会导致甲醇中的催化剂失活成丙烯(MTP)反应。通过种子诱导法合成了种子融合的ZSM-5纳米片(CNS-x),将样品的性能与没有种子的样品进行了比较。此外,用5重量%的种子和硼酸制备B掺入样品(B-CNS-5)。揭示了ZSM-5种子在纳米片上的融合作用的重要性,特别是微观结构性质及其结构效应关系的变化,这在先前的工作中并未明确记录。随着凝胶中晶种数量从5 wt%增加到30 wt%,结晶时间以及所得纳米片的变化大大缩短了,例如减小粒径和酸强度/外部表面酸度,增加超过50%的微孔体积。与NS(103 h)相比,CNS-x样品具有更长的催化寿命(168–226 h)。CNS-5对丙烯(C = 3)〜54%的选择性极高,总轻烯烃(C = 2-C = 4)的选择性为〜84%。超级样品B-CNS-5表现出最长的寿命(302小时),由于酸性位点分布的变化和额外弱酸性位点的增加,实现了最高的C = 3产量。对于转化的甲醇(g / g 超级样品B-CNS-5表现出最长的寿命(302小时),由于酸性位点分布的变化和额外弱酸性位点的增加,实现了最高的C = 3产量。对于转化的甲醇(g / g 超级样品B-CNS-5表现出最长的寿命(302小时),由于酸性位点分布的变化和额外弱酸性位点的增加,实现了最高的C = 3产量。对于转化的甲醇(g / g催化剂),结果为B-CNS-5(966)> CNS-5(525)> NS(324)。相反,平均焦炭选择性(S av,C)为B-CNS-5(0.18‰)<CNS-5(0.29‰)<NS(0.47‰)。这一结果为MTP催化剂提供了有关ZSM-5纳米片中酸度和扩散协同作用的新见解。

更新日期:2018-10-02
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