期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 6, 期 21, 页码 7841-7851出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6cy01763k
关键词
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资金
- Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE) [DE-EE0006878]
- Canadian Light Source
- U.S. DOE [DE-AC02-06CH11357]
- NSF [DMR-1121288]
- University of Wisconsin-Madison Nanoscale Science and Engineering Center [DMR-0832760]
- University of Wisconsin Materials Science Center
- China Scholarship Council (CSC)
Tetrahydropyran-2-methanol undergoes selective C-O-C hydrogenolysis to produce 1,6-hexanediol using a bifunctional RhRe (reducible metal with an oxophilic promoter) catalyst supported on Vulcan XC-72 carbon (VXC) with >90% selectivity. This RhRe/VXC catalyst is stable over 40 h of reaction in a continuous flow fixed bed reactor. The hydrogenolysis activity of RhRe/VXC is two orders-of-magnitude higher than that of RhRe supported on Norit Darco 12X40 activated carbon (NDC). STEM-EDS analysis reveals that, compared to the RhRe/VXC catalyst, the Re and Rh component metals are segregated on the surface of the low activity RhRe/NDC catalyst, suggesting that Rh and Re in close proximity (bimetallic particles) are required for an active hydrogenolysis catalyst. Differences in metal distribution on the carbon surfaces are, in turn, linked to the properties of the carbons: NDC has both a higher surface area and surface oxygen content. The low areal density of Rh and Re precursors on the high area NDC and/or interactions of the precursors with its O functional groups may interfere with the formation of the bimetallic species required for an active catalyst.
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