Influence of framework Al distribution in HZSM-5 channels on catalytic performance in the methanol to propylene reaction

Influence of framework Al distribution in HZSM-5 channels on catalytic performance in the methanol to propylene reaction
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HZSM-5通道中骨架Al分布对甲醇制丙烯反应催化性能的影响

DOI:
10.1016/j.apcata.2021.118422
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发表时间:
2021-11
期刊:
Applied Catalysis A, General
影响因子:
--
通讯作者:
Zifeng Yan
Zifeng Yan
中科院分区:
其他
文献类型:
--
作者:
Rui Feng;Bao Liu;Peng Zhou;Xinlong Yan;Xiaoyan Hu;Min Zhou;Zifeng Yan

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在葡萄糖存在下,使用两阶段结晶法制备纳米尺寸和微米尺寸的ZSM-5样品,并通过酸浸、四丙基氢氧化铵或氟硅酸铵进行额外的后处理。表征结果表明,在合成ZSM-5分子筛时,葡萄糖抑制了Al原子在孔道交叉处的位置,从而形成了更多的单Al原子,使更多的Al对分布在直孔道和正弦孔道上,而不是孔道交叉处。在甲醇转化反应中的催化性能表明,纳米ZSM-5催化剂在通道交叉点处富含Al对,并通过基于芳烃的循环表现出较高的乙烯和芳烃选择性,而微米ZSM-5催化剂在通道交叉点处具有多个单Al中心和低Al对,并通过基于烯烃的循环表现出较高的丙烯选择性但较低的芳烃选择性。该方法为制备具有较好催化性能的ZSM-5分子筛提供了一种简便的方法。
Nanosized and microsized ZSM-5 samples were prepared using a two-stage crystallization method in the presence of glucose and additional post-treated by acid leaching, tetrapropylammonium hydroxide, or ammonium fluorosilicate. The characterization results show that for synthesizing ZSM-5 zeolites, glucose inhibits the position of Al atoms in the channel intersections, thus forming additional single Al atoms and making more Al pairs at the straight and sinusoidal channels rather than channel intersections. The catalytic performance in the methanol conversion reaction shows that nanosized ZSM-5 catalysts are enriched in Al pairs in the channel intersections and exhibit higher ethylene and aromatics selectivity via the aromatic-based cycle, whereas microsized ZSM-5 catalysts have multiple single Al sites and low Al pairs in the channel intersections and exhibit higher propylene selectivity but lower aromatics selectivity via olefinic-based cycle. It provides a facile method to prepare the ZSM-5 zeolite with improved catalytic performance in the MTP reaction.
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