期刊
CHEMCATCHEM
卷 6, 期 1, 页码 142-151出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201300635
关键词
alkenes; cobalt; Fischer-Tropsch synthesis; mesoporous materials; zeolites
资金
- CatchBio program [053.70.005]
- Smart Mix Program of the Netherlands Ministry of Economic Affairs
- Netherlands Ministry of Education, Culture and Science
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]
Mesoporous H-ZSM-5 (mesoH-ZSM-5) was used as a carrier for a series of bifunctional Co-based catalysts for Fischer-Tropsch synthesis with ZrO2 and/or Ru added as promoters. The reducibility of the catalysts was studied in detail by using temperature-programmed reduction and X-ray absorption spectroscopy. A comparison of the catalytic performance of Co/mesoH-ZSM-5 and Co/SiO2 (a conventional catalyst), after 140h on stream, reveals that the former is two times more active and three times more selective to the C5-C11 fraction with a large content of unsaturated hydrocarbons, which is next to -olefins. The acid-catalyzed conversion of n-hexane and 1-hexene, as model reactions, demonstrates that the improvement in the selectivity toward gasoline range hydrocarbons is due to the acid-catalyzed reactions of the Fischer-Tropsch -olefins over the acidic zeolite. The formation of methane over the zeolite-supported Co catalysts originates from direct CO hydrogenation and hydrocarbon hydrogenolysis on coordinatively unsaturated Co sites, which are stabilized as a consequence of a strong metal-zeolite interaction. Although the addition of either ZrO2 or Ru increases the catalyst reducibility considerably, it does not affect the product selectivity significantly.
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