Selective Oxidation of Methane to Methanol over ZSM-5 Catalysts in Aqueous Hydrogen Peroxide: Role of Formaldehyde

被引：25
|
作者：
Al-Shihri, Saeed [1 ]
Richard, Christian J. [1 ]
Chadwick, David [1 ]
机构：
[1] Imperial Coll London, Dept Chem Engn, London SW7 2AZ, England
来源：
CHEMCATCHEM | 2017年 / 9卷 / 07期
关键词：
hydrogen peroxide; methane; methanol; oxidation; ZSM-5; METHYL HYDROPEROXIDE; LOW-TEMPERATURE; POLYACETAL COPOLYMERS; PROMOTED FE-ZSM-5; DIRECT CONVERSION; FEZSM-5; ZEOLITE; FORMIC-ACID; ACTIVATION; CHEMISTRY; CHEMICALS;
D O I：
10.1002/cctc.201601563
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：
The selective oxidation of methane in aqueous hydrogen peroxide over ZSM-5 catalysts with different Si/Al ratios has been investigated. Methyl hydroperoxide was confirmed as the initial product of methane oxidation by a study of product distribution versus reaction time in agreement with previous work. Formaldehyde was identified as an intermediate in the oxidation reaction pathway from MeOOH to formic acid and ultimately CO2. Hydrogen evolution during the oxidation of methane is reported for the first time. Oxidation of the HCHO intermediate to formic acid was demonstrated to be the source of the evolved hydrogen. HCHO appeared to be the source of low levels of soluble polyoxomethylene. Higher productivity of liquid oxygenated products is reported compared to previous work.
引用
收藏
页码：1276 / 1283
页数：8
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