Structural Evolution of Iron-Loaded Metal–Organic Framework Catalysts for Continuous Gas-Phase Oxidation of Methane to Methanol
Bunyarat Rungtaweevoranit, Ali M. Abdel‐Mageed, Pongtanawat Khemthong, Srisin Eaimsumang, Khetpakorn Chakarawet, Teera Butburee, Benny Kunkel, Sebastian Wohlrab, Kittipong Chainok, Jakkapop Phanthasri, Suttipong Wannapaiboon, Saran Youngjan, Theerada Seehamongkol, Sarawoot Impeng, Kajornsak Faungnawakij
Abstract
High Resolution Image Download MS PowerPoint Slide 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 O 2 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 μmol MeOH g Fe –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.