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Structural Evolution of Iron-Loaded Metal-Organic Framework Catalysts for Continuous Gas-Phase Oxidation of Methane to Methanol
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Document Title
Structural Evolution of Iron-Loaded Metal-Organic Framework Catalysts for Continuous Gas-Phase Oxidation of Methane to Methanol
Author
Rungtaweevoranit B., Abdel-Mageed A.M., Khemthong P., Eaimsumang S., Chakarawet K., Butburee T., Kunkel B., Wohlrab S., Chainok K., Phanthasri J., Wannapaiboon S., Youngjan S., Seehamongkol T., Impeng S., Faungnawakij K.
Affiliations
National Nanotechnology Center (NANOTEC), National Science and Technology Development Agency (NSTDA), Pathum Thani, 12120, Thailand; Leibniz-Institut f?r Katalyse e.V. (LIKAT Rostock), Albert-Einstein-Stra?e 29a, Rostock, 18059, Germany; Department of Chemistry, Faculty of Science, Cairo University, Giza, 12613, Egypt; Institute of Surface Chemistry and Catalysis, Ulm University, Ulm, D-89069, Germany; Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, United States; Department of Chemistry, Faculty of Science, Mahidol University, Bangkok, 10400, Thailand; Thammasat University Research Unit in Multifunctional Crystalline Materials and Applications (TU-MCMA), Faculty of Science and Technology, Thammasat University, Pathum Thani, 12121, Thailand; Synchrotron Light Research Institute (Public Organization), 111 University Avenue, Nakhon Ratchasima, 30000, Thailand
Type
Article
Source Title
ACS Applied Materials and Interfaces
ISSN
19448244
Year
2023
Volume
15
Issue
22
Page
26700-26709
Open Access
All Open Access, Hybrid Gold, Green
Publisher
American Chemical Society
DOI
10.1021/acsami.3c03310
Format
Abstract
Catalytic partial oxidation of methane presents a promising route to convert the abundant but environmentally undesired methane gas to liquid methanol with applications as an energy carrier and a platform chemical. However, an outstanding challenge for this process remains in developing a catalyst that can oxidize methane selectively to methanol with good activity under continuous flow conditions in the gas phase using O2 as an oxidant. Here, we report a Fe catalyst supported by a metal-organic framework (MOF), Fe/UiO-66, for the selective and on-stream partial oxidation of methane to methanol. Kinetic studies indicate the continuous production of methanol at a superior reaction rate of 5.9 ? 10-2 ?molMeOH gFe-1 s-1 at 180 ?C and high selectivity toward methanol, with the catalytic turnover verified by transient methane isotopic measurements. Through an array of spectroscopic characterizations, electron-deficient Fe species rendered by the MOF support is identified as the probable active site for the reaction. ? 2023 The Authors. Published by American Chemical Society.
License
CC-BY-NC-ND
Rights
Authors
Publication Source
WOS