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B18-Core EXAFS	Direct conversion of methane to ethylene and acetylene over an iron-based metal–organic framework Yujie Ma , Xue Han , Shaojun Xu , Zhe Li , Wanpeng Lu , Bing An , Daniel Lee , Sarayute Chansai , Alena M. Sheveleva , Zi Wang , Yinlin Chen , Jiangnan Li , Weiyao Li , Rongsheng Cai , Ivan Da Silva , Yongqiang Cheng , Luke L. Daemen , Floriana Tuna , Eric J. L. Mcinnes , Lewis Hughes , Pascal Manuel , Anibal J. Ramirez-Cuesta , Sarah J. Haigh , Christopher Hardacre , Martin Schroeder , Sihai Yang Journal Of The American Chemical Society DOI: 10.1021/jacs.3c03935 Diamond Proposal Number(s): [19850] Open Access Show Abstract ▼ Abstract: Conversion of methane (CH4) to ethylene (C2H4) and/or acetylene (C2H2) enables routes to a wide range of products directly from natural gas. However, high reaction temperatures and pressures are often required to activate and convert CH4 controllably, and separating C2+ products from unreacted CH4 can be challenging. Here, we report the direct conversion of CH4 to C2H4 and C2H2 driven by non-thermal plasma under ambient (25 °C and 1 atm) and flow conditions over a metal–organic framework material, MFM-300(Fe). The selectivity for the formation of C2H4 and C2H2 reaches 96% with a high time yield of 334 μmol gcat–1 h–1. At a conversion of 10%, the selectivity to C2+ hydrocarbons and time yield exceed 98% and 2056 μmol gcat–1 h–1, respectively, representing a new benchmark for conversion of CH4. In situ neutron powder diffraction, inelastic neutron scattering and solid-state nuclear magnetic resonance, electron paramagnetic resonance (EPR), and diffuse reflectance infrared Fourier transform spectroscopies, coupled with modeling studies, reveal the crucial role of Fe–O(H)–Fe sites in activating CH4 and stabilizing reaction intermediates via the formation of an Fe–O(CH3)–Fe adduct. In addition, a cascade fixed-bed system has been developed to achieve online separation of C2H4 and C2H2 from unreacted CH4 for direct use. Integrating the processes of CH4 activation, conversion, and product separation within one system opens a new avenue for natural gas utility, bridging the gap between fundamental studies and practical applications in this area.	Sep 2023

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B18-Core EXAFS

Direct conversion of methane to ethylene and acetylene over an iron-based metal–organic framework