期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 121, 期 25, 页码 13666-13679出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.7b02344
关键词
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资金
- Catalysis Center for Energy Innovation, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001004]
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
Al, Ga, Fe, and B metal substituents have been examined for their ability to change the Bronsted 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-[A1]-,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-[13]-BEA and H-[Al]-BEA, respectively. Electronic structure calculations revealed that the Diels-Alder reaction remains unaffected by changes to the Bronsted 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 Bronsted-acidic zeolite did not have a significant effect on the product selectivity, however, indicating that the same reaction pathways are active with both catalysts.
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