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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
B22-Multimode InfraRed imaging And Microspectroscopy	Efficient capture and storage of ammonia in robust aluminium-based metal-organic frameworks Lixia Guo , Joseph Hurd , Meng He , Wanpeng Lu , Jiangnan Li , Danielle Crawshaw , Mengtian Fan , Sergey A. Sapchenko , Yinlin Chen , Xiangdi Zeng , Meredydd Kippax-Jones , Wenyuan Huang , Zhaodong Zhu , Pascal Manuel , Mark D. Frogley , Daniel Lee , Martin Schroeder , Sihai Yang Communications Chemistry 6 DOI: 10.1038/s42004-023-00850-4 Diamond Proposal Number(s): [30398] Open Access Show Abstract ▼ Abstract: The development of stable sorbent materials to deliver reversible adsorption of ammonia (NH3) is a challenging task. Here, we report the efficient capture and storage of NH3 in a series of robust microporous aluminium-based metal-organic framework materials, namely MIL-160, CAU-10-H, Al-fum, and MIL-53(Al). In particular, MIL-160 shows high uptakes of NH3 of 4.8 and 12.8 mmol g−1 at both low and high pressure (0.001 and 1.0 bar, respectively) at 298 K. The combination of in situ neutron powder diffraction, synchrotron infrared micro-spectroscopy and solid-state nuclear magnetic resonance spectroscopy reveals the preferred adsorption domains of NH3 molecules in MIL-160, with H/D site-exchange between the host and guest and an unusual distortion of the local structure of [AlO6] moieties being observed. Dynamic breakthrough experiments confirm the excellent ability of MIL-160 to capture of NH3 with a dynamic uptake of 4.2 mmol g−1 at 1000 ppm. The combination of high porosity, pore aperture size and multiple binding sites promotes the significant binding affinity and capacity for NH3, which makes it a promising candidate for practical applications.	Mar 2023

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