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Instruments / Technical Area	Publication Details	Published	Actions
B22-Multimode InfraRed imaging And Microspectroscopy	Direct photo-oxidation of methane to methanol over a mono-iron hydroxyl site Bing An , Zhe Li , Zi Wang , Xiangdi Zeng , Xue Han , Yongqiang Chen , Alena M. Sheveleva , Zhongyue Zhang , Floriana Tuna , Eric J. L. Mcinnes , Mark D. Frogley , Anibal J. Ramirez-Cuesta , Louise S. Natrajan , Cheng Wang , Wenbin Li , Sihai Yang , Martin Schroeder Nature Materials 338 DOI: 10.1038/s41563-022-01279-1 Diamond Proposal Number(s): [23782] Show Abstract ▼ Abstract: Natural gas, consisting mainly of methane (CH4), has a relatively low energy density at ambient conditions (~36 kJ l−1). Partial oxidation of CH4 to methanol (CH3OH) lifts the energy density to ~17 MJ l−1 and drives the production of numerous chemicals. In nature, this is achieved by methane monooxygenase with di-iron sites, which is extremely challenging to mimic in artificial systems due to the high dissociation energy of the C–H bond in CH4 (439 kJ mol−1) and facile over-oxidation of CH3OH to CO and CO2. Here we report the direct photo-oxidation of CH4 over mono-iron hydroxyl sites immobilized within a metal–organic framework, PMOF-RuFe(OH). Under ambient and flow conditions in the presence of H2O and O2, CH4 is converted to CH3OH with 100% selectivity and a time yield of 8.81 ± 0.34 mmol gcat−1 h−1 (versus 5.05 mmol gcat−1 h−1 for methane monooxygenase). By using operando spectroscopic and modelling techniques, we find that confined mono-iron hydroxyl sites bind CH4 by forming an [Fe–OH···CH4] intermediate, thus lowering the barrier for C–H bond activation. The confinement of mono-iron hydroxyl sites in a porous matrix demonstrates a strategy for C–H bond activation in CH4 to drive the direct photosynthesis of CH3OH.	Jun 2022

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B22-Multimode InfraRed imaging And Microspectroscopy

Direct photo-oxidation of methane to methanol over a mono-iron hydroxyl site