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
相关论文
共 50 条
  • [41] Alkylation of benzene with formaldehyde over ZSM-5
    Wu, XC
    Anthony, RG
    JOURNAL OF CATALYSIS, 1999, 184 (01) : 294 - 297
  • [42] Formic Acid Production Via Methane Peroxide Oxidation Over Oxalic Acid Activated Fe-MFI Catalysts
    Taran, Oxana P.
    Yashnik, Svetlana A.
    Boltenkov, Vadim V.
    Parkhomchuk, Ekaterina V.
    Sashkina, Kseniya A.
    Ayusheev, Artemiy B.
    Babushkin, Dmitrii E.
    Parmon, Valentin N.
    TOPICS IN CATALYSIS, 2019, 62 (5-6) : 491 - 507
  • [43] Methanol selective oxidation to formaldehyde over iron-molybdate catalysts
    Soares, APV
    Portela, MF
    CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2005, 47 (01): : 125 - 174
  • [44] Alkylation of benzene with aqueous solution of ethanol over ZSM-5 catalysts
    Yuan, Jun-Jun
    Gevert, Borge S.
    INDIAN JOURNAL OF CHEMICAL TECHNOLOGY, 2006, 13 (04) : 334 - 340
  • [45] Catalytic and Mechanistic Insights of the Low-Temperature Selective Oxidation of Methane over Cu-Promoted Fe-ZSM-5
    Hammond, Ceri
    Jenkins, Robert L.
    Dimitratos, Nikolaos
    Lopez-Sanchez, Jose Antonio
    ab Rahim, Mohd Hasbi
    Forde, Michael M.
    Thetford, Adam
    Murphy, Damien M.
    Hagen, Henk
    Stangland, Eric E.
    Moulijn, Jacob M.
    Taylor, Stuart H.
    Willock, David J.
    Hutchings, Graham J.
    CHEMISTRY-A EUROPEAN JOURNAL, 2012, 18 (49) : 15735 - 15745
  • [46] Selective Oxidation of Methanol to Formaldehyde Over Active Molybdenum Oxide Supported on Hydroxyapatite Catalysts
    Abd El-Aziz A. Said
    Mohamed M. M. Abd El-Wahab
    Alian M. Alian
    Catalysis Letters, 2016, 146 : 82 - 90
  • [47] Selective Oxidation of Methanol to Formaldehyde Over Active Molybdenum Oxide Supported on Hydroxyapatite Catalysts
    Said, Abd El-Aziz A.
    Abd El-Wahab, Mohamed M. M.
    Alian, Alian M.
    CATALYSIS LETTERS, 2016, 146 (01) : 82 - 90
  • [48] Mechanistic Insights into the Desorption of Methanol and Dimethyl Ether Over ZSM-5 Catalysts
    Omojola, Toyin
    Cherkasov, Nikolay
    McNab, Andrew I.
    Lukyanov, Dmitry B.
    Anderson, James A.
    Rebrov, Evgeny V.
    van Veen, Andre C.
    CATALYSIS LETTERS, 2018, 148 (01) : 474 - 488
  • [49] Mechanistic Insights into the Desorption of Methanol and Dimethyl Ether Over ZSM-5 Catalysts
    Toyin Omojola
    Nikolay Cherkasov
    Andrew I. McNab
    Dmitry B. Lukyanov
    James A. Anderson
    Evgeny V. Rebrov
    André C. van Veen
    Catalysis Letters, 2018, 148 : 474 - 488
  • [50] Partial oxidation of CH4 over ZSM-5 catalysts
    Kudo, H
    Ono, T
    APPLIED SURFACE SCIENCE, 1997, 121 : 413 - 416
12345