Exceptional capture of methane at low pressure by an iron-based metal-organic framework

Yujie Ma; Cheng Li; Lixia Guo; Wanpeng Lu; Yongqiang Cheng; Xue Han; Jiangnan Li; Danielle Crawshaw; Meng He; Lutong Shan; Daniel Lee; Ivan da Silva; Pascal Manuel; Anibal J. Ramirez-Cuesta; Martin Schröder; Sihai Yang

doi:10.1002/chem.202303934

Exceptional capture of methane at low pressure by an iron-based metal-organic framework

Yujie Ma, Cheng Li, Lixia Guo, Wanpeng Lu, Yongqiang Cheng, Xue Han, Jiangnan Li, Danielle Crawshaw, Meng He, Lutong Shan, Daniel Lee, Ivan da Silva, Pascal Manuel, Anibal J. Ramirez-Cuesta, Martin Schröder, Sihai Yang

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Abstract

The selective capture of methane (CH₄) at low concentrations and its separation from N₂ are extremely challenging owing to the weak host-guest interactions between CH₄ molecules and any sorbent material. Here, we report the exceptional adsorption of CH₄ at low pressure and the efficient separation of CH₄/N₂ by MFM-300(Fe). MFM-300(Fe) shows a very high uptake for CH₄ of 0.85 mmol g⁻¹ at 1 mbar and 298 K and a record CH₄/N₂ selectivity of 45 for porous solids, representing a new benchmark for CH₄ capture and CH₄/N₂ separation. The excellent separation of CH₄/N₂ by MFM-300(Fe) has been confirmed by dynamic breakthrough experiments. In situ neutron powder diffraction, and solid-state nuclear magnetic resonance and diffuse reflectance infrared Fourier transform spectroscopies, coupled with modelling, reveal a unique and strong binding of CH₄ molecules involving Fe−OH⋯CH₄ and C⋯phenyl ring interactions within the pores of MFM-300(Fe), thus promoting the exceptional adsorption of CH₄ at low pressure.

Original language	English
Article number	e202303934
Journal	Chemistry - A European Journal
Volume	30
Issue number	20
DOIs	https://doi.org/10.1002/chem.202303934
State	Published - Apr 5 2024

Funding

We thank the EPSRC (EP/I011870, EP/V056409), the UK Catalysis Hub, the Royal Society and the University of Manchester for funding. This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement No 742401, NANOCHEM). We are grateful to the STFC/ISIS Facility for access to Beamline WISH. This research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Computing resources for neutron data analysis were made available through the VirtuES and the ICE‐MAN projects, funded by Laboratory Directed Research and Development program and Compute and Data Environment for Science (CADES) at ORNL. Y.M., L.G., M.H. and L.S. thank the China Scholarship Council (CSC) for funding.

Funders	Funder number
Compute and Data Environment for Science
Laboratory Directed Research and Development
Engineering and Physical Sciences Research Council	EP/V056409, EP/I011870
Royal Society
University of Manchester
European Research Council
China Scholarship Council
Horizon 2020	742401
UK Catalysis Hub

Keywords

binding sites
metal-organic framework
methane capture
methane/nitrogen separation

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10.1002/chem.202303934

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Ma, Y., Li, C., Guo, L., Lu, W., Cheng, Y., Han, X., Li, J., Crawshaw, D., He, M., Shan, L., Lee, D., da Silva, I., Manuel, P., Ramirez-Cuesta, A. J., Schröder, M., & Yang, S. (2024). Exceptional capture of methane at low pressure by an iron-based metal-organic framework. Chemistry - A European Journal, 30(20), Article e202303934. https://doi.org/10.1002/chem.202303934

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abstract = "The selective capture of methane (CH4) at low concentrations and its separation from N2 are extremely challenging owing to the weak host-guest interactions between CH4 molecules and any sorbent material. Here, we report the exceptional adsorption of CH4 at low pressure and the efficient separation of CH4/N2 by MFM-300(Fe). MFM-300(Fe) shows a very high uptake for CH4 of 0.85 mmol g−1 at 1 mbar and 298 K and a record CH4/N2 selectivity of 45 for porous solids, representing a new benchmark for CH4 capture and CH4/N2 separation. The excellent separation of CH4/N2 by MFM-300(Fe) has been confirmed by dynamic breakthrough experiments. In situ neutron powder diffraction, and solid-state nuclear magnetic resonance and diffuse reflectance infrared Fourier transform spectroscopies, coupled with modelling, reveal a unique and strong binding of CH4 molecules involving Fe−OH⋯CH4 and C⋯phenyl ring interactions within the pores of MFM-300(Fe), thus promoting the exceptional adsorption of CH4 at low pressure.",

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author = "Yujie Ma and Cheng Li and Lixia Guo and Wanpeng Lu and Yongqiang Cheng and Xue Han and Jiangnan Li and Danielle Crawshaw and Meng He and Lutong Shan and Daniel Lee and {da Silva}, Ivan and Pascal Manuel and Ramirez-Cuesta, {Anibal J.} and Martin Schr{\"o}der and Sihai Yang",

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AU - Li, Cheng

AU - Guo, Lixia

AU - Lu, Wanpeng

AU - Cheng, Yongqiang

AU - Han, Xue

AU - Li, Jiangnan

AU - Crawshaw, Danielle

AU - He, Meng

AU - Shan, Lutong

AU - Lee, Daniel

AU - da Silva, Ivan

AU - Manuel, Pascal

AU - Ramirez-Cuesta, Anibal J.

AU - Schröder, Martin

AU - Yang, Sihai

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N2 - The selective capture of methane (CH4) at low concentrations and its separation from N2 are extremely challenging owing to the weak host-guest interactions between CH4 molecules and any sorbent material. Here, we report the exceptional adsorption of CH4 at low pressure and the efficient separation of CH4/N2 by MFM-300(Fe). MFM-300(Fe) shows a very high uptake for CH4 of 0.85 mmol g−1 at 1 mbar and 298 K and a record CH4/N2 selectivity of 45 for porous solids, representing a new benchmark for CH4 capture and CH4/N2 separation. The excellent separation of CH4/N2 by MFM-300(Fe) has been confirmed by dynamic breakthrough experiments. In situ neutron powder diffraction, and solid-state nuclear magnetic resonance and diffuse reflectance infrared Fourier transform spectroscopies, coupled with modelling, reveal a unique and strong binding of CH4 molecules involving Fe−OH⋯CH4 and C⋯phenyl ring interactions within the pores of MFM-300(Fe), thus promoting the exceptional adsorption of CH4 at low pressure.

AB - The selective capture of methane (CH4) at low concentrations and its separation from N2 are extremely challenging owing to the weak host-guest interactions between CH4 molecules and any sorbent material. Here, we report the exceptional adsorption of CH4 at low pressure and the efficient separation of CH4/N2 by MFM-300(Fe). MFM-300(Fe) shows a very high uptake for CH4 of 0.85 mmol g−1 at 1 mbar and 298 K and a record CH4/N2 selectivity of 45 for porous solids, representing a new benchmark for CH4 capture and CH4/N2 separation. The excellent separation of CH4/N2 by MFM-300(Fe) has been confirmed by dynamic breakthrough experiments. In situ neutron powder diffraction, and solid-state nuclear magnetic resonance and diffuse reflectance infrared Fourier transform spectroscopies, coupled with modelling, reveal a unique and strong binding of CH4 molecules involving Fe−OH⋯CH4 and C⋯phenyl ring interactions within the pores of MFM-300(Fe), thus promoting the exceptional adsorption of CH4 at low pressure.

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Exceptional capture of methane at low pressure by an iron-based metal-organic framework

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