期刊
SURFACE SCIENCE
卷 652, 期 -, 页码 58-66出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.susc.2016.03.017
关键词
Aldehyde esterification; Oxidative cross-coupling; Methyl acrylate production; Nanoporous gold; Gold; Au(110); Selective oxidation
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]
- U.S. Department of Energy by LLNL [DE-AC52-07NA27344]
Modern methods of esterification, one of the most important reactions in organic synthesis, are reaching their limits, as far as waste and expense are concerned. Novel chemical approaches to ester formation are therefore of importance. Here we report a simple procedure free of caustic reagents or byproducts for the facile direct oxidative methyl esterification of aldehydes over nanoporous Au catalysts. Complementary model studies on single crystal gold surfaces establish the fundamental reactions involved. We find that methanol more readily reacts with adsorbed active oxygen than do the aldehydes, but that once the aldehydes do react, they form strongly bound acrylates that block reactive sites and decrease the yields of acrylic esters under steady flow conditions at 420 K. Significant improvements in yield can be achieved by operating at higher temperatures, which render the site-blocking acrylates unstable. (C) 2016 Elsevier B.V. All rights reserved.
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