期刊
ACS CATALYSIS
卷 5, 期 7, 页码 4237-4241出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.5b00330
关键词
nanoporous gold; energy-efficient catalysis; selective oxidation; activation; ozone
资金
- Integrated Mesoscale Architectures for Sustainable Catalysis, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0012573]
- National Science Foundation under NSF [ECS-0335765]
- U.S. Department of Energy [DE-AC52-07NA27344]
We report a new method for facile and reproducible activation of nanoporous gold (npAu) materials of different forms for the catalytic selective partial oxidation of alcohols under ambient pressure, steady flow conditions. This method, based on the surface cleaning of npAu ingots with ozone to remove carbon documented in ultrahigh vacuum conditions, produces active npAu catalysts from ingots, foils, and shells by flowing an ozone/dioxygen mixture over the catalyst at 150 degrees C, followed by a temperature ramp from 50 to 150 degrees C in a flowing stream of 10% methanol and 20% oxygen. With this treatment, all three materials (ingots, foils, and shells) can be reproducibly activated, despite potential carbonaceous poisons resulting from their synthesis, and are highly active for the selective oxidation of primary alcohols over prolonged periods of time. The npAu materials activated in this manner exhibit catalytic behavior substantially different from those activated under different conditions previously reported. Once activated in this manner, they can be stored and easily reactivated by flow of reactant gases at 150 degrees C for a few hours. They possess improved selectivity for the coupling of higher alcohols, such as 1-butanol, and are not active for carbon monoxide oxidation. This ozone-treated npAu is a functionally new catalytic material.
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