Methanol oxidation on Au(332): methyl formate selectivity and surface deactivation under isothermal conditions

被引：7
作者：
Feldt, Christoph D. [1 ]
Kirschbaum, Thorren [1 ,2 ]
Low, Jian Liang [1 ]
Riedel, Wiebke [1 ]
Risse, Thomas [1 ]
机构：
[1] Free Univ Berlin, Inst Chem & Biochem, Arnimallee 22, D-14195 Berlin, Germany
[2] Helmholtz Zentrum Berlin Mat & Energie, Hahn Meitner Pl 1, D-14109 Berlin, Germany
来源：
CATALYSIS SCIENCE & TECHNOLOGY | 2022年 / 12卷 / 05期
关键词：
TEMPERATURE CO OXIDATION; NANOPOROUS GOLD CATALYSTS; ATOMIC OXYGEN; AU(110) SURFACE; CHEMISTRY; ADSORPTION; EVOLUTION; PT(111); SITES; AU;
D O I：
10.1039/d1cy02034j
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
Methanol oxidation on the stepped Au(332) surface was investigated by pulsed isothermal molecular beam (MB) experiments. The effect of the surface temperature as well as the influence of changes in the methanol and atomic oxygen flux on the partial oxidation to methyl formate was studied. A maximum in methyl formate formation is observed at 250 K under the applied single collision conditions. Increasing the methanol to oxygen ratio was found to increase the selectivity to methyl formate and decrease unwanted overoxidation to surface deactivating formate detected by in situ infrared reflection absorption spectroscopy (IRAS). The results show evidence for the importance of an additional deactivation mechanism for methyl formate formation connected to methanol which is active under oxygen-deficient conditions at low temperatures. Moreover, the measurements suggest a small number of sites to be highly reactive for methyl formate formation which are preferentially blocked under oxygen-deficient conditions.
引用
收藏
页码：1418 / 1428
页数：11
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