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

页码：1276 / 1283

页数：8

共 50 条

[21] Hydrogen production by aqueous phase reforming of phenol over Ni/ZSM-5 catalysts
Yan, Beibei
Li, Wanqing
Tao, Junyu
Xu, Ningge
Li, Xiangping
Chen, Guanyi
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2017, 42 (10) : 6674 - 6682
[22] Syngas production with dry reforming of methane over Ni/ZSM-5 catalysts
Moradi, Gholamreza
Khezeli, Foroogh
Hemmati, Hamed
JOURNAL OF NATURAL GAS SCIENCE AND ENGINEERING, 2016, 33 : 657 - 665
[23] Identifying the crucial role of water and chloride for efficient mild oxidation of methane to methanol over a [Cu2(μ-O)]2+-ZSM-5 catalyst
Fang, Zhihao
Huang, Mengyuan
Liu, Bing
Jiang, Feng
Xu, Yuebing
Liu, Xiaohao
JOURNAL OF CATALYSIS, 2022, 405 : 1 - 14
[24] Furfural Oxidation with Hydrogen Peroxide Over ZSM-5 Based Micro-Mesoporous Aluminosilicates
Nataliya D. Shcherban
Roman Yu. Barakov
Sergii A. Sergiienko
Kari Eränen
Johan Wärnå
Dmitry Yu. Murzin
Catalysis Letters, 2022, 152 : 2920 - 2932
[25] Frustrated Lewis pairs promote selective methane oxidation over ZSM-5 supported Au-WO3 photocatalyst
Wu, Tong
Zhang, Mengyao
Gong, Xiaoxiao
Ni, Caihong
Zou, Yupeng
Gao, Panpan
Sun, Songmei
MOLECULAR CATALYSIS, 2025, 581
[26] Partial oxidation of methane to formaldehyde and methanol using molecular oxygen over Fe-ZSM-5
Michalkiewicz, B
APPLIED CATALYSIS A-GENERAL, 2004, 277 (1-2) : 147 - 153
[27] Oxidation of Methane to Methanol with Hydrogen Peroxide Using Supported Gold-Palladium Alloy Nanoparticles
Ab Rahim, Mohd Hasbi
Forde, Michael M.
Jenkins, Robert L.
Hammond, Ceri
He, Qian
Dimitratos, Nikolaos
Lopez-Sanchez, Jose Antonio
Carley, Albert F.
Taylor, Stuart H.
Willock, David J.
Murphy, Damien M.
Kiely, Christopher J.
Hutchings, Graham J.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (04) : 1280 - 1284
[28] Deactivation Aspects of Methane Oxidation Catalysts Based on Palladium and ZSM-5
Andrey W. Petrov
Davide Ferri
Mohamed Tarik
Oliver Kröcher
Jeroen A. van Bokhoven
Topics in Catalysis, 2017, 60 : 123 - 130
[29] Solid Catalysts for the Selective Low-Temperature Oxidation of Methane to Methanol
Palkovits, Regina
Antonietti, Markus
Kuhn, Pierre
Thomas, Arne
Schueth, Ferdi
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (37) : 6909 - 6912
[30] Structure and reactivity of copper iron pyrophosphate catalysts for selective oxidation of methane to formaldehyde and methanol
Polniser, Robert
Stolcova, Magdalena
Hronec, Milan
Mikula, Milan
APPLIED CATALYSIS A-GENERAL, 2011, 400 (1-2) : 122 - 130

← 1 2 3 4 5 →