Verifying the dominant catalytic cycle of the methanol-to-hydrocarbon conversion over SAPO-41
Verifying the dominant catalytic cycle of the methanol-to-hydrocarbon conversion over SAPO-41
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验证 SAPO-41 上甲醇转化为碳氢化合物的主要催化循环
DOI：
10.1039/c3cy00740e
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发表时间：
2014-02
影响因子：
5
通讯作者：
Michael Hunger
中科院分区：
文献类型：
--
作者：
Wu Guangjun;Li L;ong;Guan Naijia;Michael Hunger
本文研究了具有一维10环孔的硅铝磷酸酯SAPO-41上甲醇制烃的机理。为此，我们进行了共投料催化实验，对装载氨的催化剂进行了原位FTIR和UV/Vis光谱分析，以及1H MAS NMR谱分析。使用这些方法，在SAPO-41催化剂上只能观察到低含量的芳烃。这些发现和共投料实验中乙烯选择性的特征变化表明，烷基芳体化合物可以作为活性烃池化合物在SAPO-41上用作MTH催化剂。另一方面，用FTIR和UV/Vis光谱检测二烯和烯基碳离子，用1h MAS NMR谱检测烯烃与氨反应生成胺。实验结果表明，部分以正碳态存在的大烯烃主导了SAPO-41的催化活性烃池。由于这种以烯烃为主的反应机理和有限的芳烃生成，SAPO-41是C3+C4烯烃和汽油生产的合适催化剂。
In the present work, the mechanism of the methanol-to-hydrocarbon (MTH) conversion over the silicoaluminophosphate SAPO-41 with one-dimensional 10-ring pores has been investigated. For this purpose, catalytic experiments with co-feeding of reactants, in situ FTIR and UV/Vis spectroscopy, and 1H MAS NMR spectroscopy of used catalysts upon loading of ammonia were performed. Using these methods, only a low content of aromatics could be observed on the working SAPO-41 catalyst. These findings and the characteristic changes in the ethene selectivity during the co-feeding experiments indicate that alkylaromatics can be excluded as active hydrocarbon pool compounds on SAPO-41 applied as MTH catalysts. On the other hand, dienes and enylic carbenium ions were detected using FTIR and UV/Vis spectroscopy and the formation of amines by reaction of alkenes with ammonia was detected via1H MAS NMR spectroscopy. These results are experimental evidence that large olefins partially existing in their carbenium state dominate the catalytically active hydrocarbon pool on the working SAPO-41. Due to this dominant alkene-based reaction mechanism and the limited formation of aromatics, SAPO-41 is a suitable catalyst for the C3+C4 olefin as well as gasoline production.
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