期刊
CATALYSIS LETTERS
卷 145, 期 6, 页码 1217-1223出版社
SPRINGER
DOI: 10.1007/s10562-015-1525-4
关键词
Nanoporous gold; Selective oxidation; Ethanol; 1-Butanol; Ester formation; Aerobic oxidation; Catalysis
资金
- U.S. Department of Energy, Basic Energy Sciences, Catalysis Science Program [DE-FG-02-84ER13289]
- U.S. Department of Energy by LLNL [DE-AC52-07NA27344]
A dilute Ag alloy of nanoporous Au (npAu) has been shown to self-couple methanol with 100 % selectivity and high conversion under catalytic flow conditions. However, because prior studies in flow reactors showed difficulty in self-coupling ethanol and 1-butanol over npAu in flow reactors, the inherent capability on npAu for self-coupling of ethanol and 1-butanol was examined under ultrahigh vacuum conditions on identical npAu catalysts. This study shows that the oxygen-covered Ag-modified npAu does efficiently effect the self-coupling of ethanol and 1-butanol under UHV conditions. The coupling is initiated by adsorbed atomic oxygen formed from O-2 dissociation via a chemisorbed molecular state. The amount of ester formed increases with the degree of oxygen precoverage at the expense of aldehyde production. Repeated annealing of the catalyst above 550 K for temperature programmed reaction changes the ligament and pore sizes, affecting the product distribution, but high reactivity is sustained over many heating cycles. [GRAPHICS] .
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