H- [Al] -BEA，H- [Fe] -BEA，H- [Ga] -BEA和H- [B] -BEA沸石中呋喃的脱水芳构化为芳烃的常规酸型催化,The Journal of Physical Chemistry C

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H- [Al] -BEA，H- [Fe] -BEA，H- [Ga] -BEA和H- [B] -BEA沸石中呋喃的脱水芳构化为芳烃的常规酸型催化
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2017-06-20 00:00:00 , DOI: 10.1021/acs.jpcc.7b02344
Ryan E. Patet ₁ , Maura Koehle ₁ , Raul F. Lobo ₁ , Stavros Caratzoulas ₁ , Dionisios G. Vlachos ₁

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已经检验了Al，Ga，Fe和B金属取代基改变呋喃，2-甲基呋喃和2,5-二甲基呋喃的芳烃生产中BEA沸石的布朗斯台德酸强度和抑制不希望的水解的能力。我们使用电子结构计算来检查H- [Al]-，H- [Fe]-，H- [Ga]-和H- [B] -BEA沸石中的这一系列呋喃。这些计算用于参数化微动力学模型，以便与呋喃和DMF分别在最弱和最强酸性沸石H- [B] -BEA和H- [Al] -BEA中进行的实验进行直接比较。电子结构计算表明，狄尔斯-阿尔德反应不受沸石布朗斯台德酸强度变化的影响，而脱水和水解反应则以普通酸催化的方式受到影响。分别来自呋喃和2,5-二甲基呋喃的对二甲苯。用微动力学模型分析表明，即使具有较弱的异质酸位点，脱水反应也能得到充分催化，从而激活了芳烃的生产途径。但是，使用较弱的非均质布朗斯台德酸性沸石对产物的选择性没有明显影响，这表明两种催化剂均具有相同的反应路径。

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General Acid-Type Catalysis in the Dehydrative Aromatization of Furans to Aromatics in H-[Al]-BEA, H-[Fe]-BEA, H-[Ga]-BEA, and H-[B]-BEA Zeolites

Al, Ga, Fe, and B metal substituents have been examined for their ability to change the Brønsted acid strength of BEA zeolite and inhibit undesired hydrolysis in the production of aromatics from furan, 2-methylfuran, and 2,5-dimethylfuran. We employed electronic structure calculations to examine this series of furans in H-[Al]-, H-[Fe]-, H-[Ga]-, and H-[B]-BEA zeolites. These calculations were used to parametrize a microkinetic model to make direct comparisons to experiments run with furan and DMF in the weakest and strongest acid zeolites, H-[B]-BEA and H-[Al]-BEA, respectively. Electronic structure calculations revealed that the Diels–Alder reaction remains unaffected by changes to the Brønsted acid strength of the zeolite, whereas the dehydration and hydrolysis reactions are affected in a fashion reminiscent of general acid catalysis. Interestingly, despite its significantly lower acid strength, H-[B]-BEA was experimentally shown to have an activity similar to that of H-[Al]-BEA for the production of both benzene and p-xylene from furan and 2,5-dimethylfuran, respectively. Analysis with the microkinetic model revealed that, even with this weaker heterogeneous acid site, the dehydration reaction is sufficiently catalyzed, activating the aromatic production pathway. The use of a weaker, heterogeneous Brønsted-acidic zeolite did not have a significant effect on the product selectivity, however, indicating that the same reaction pathways are active with both catalysts.

更新日期：2017-06-28

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