Refinement of pore size at sub-angstrom precision in robust metal–organic frameworks for separation of xylenes

Xiaolin Li; Juehua Wang; Nannan Bai; Xinran Zhang; Xue Han; Ivan da Silva; Christopher G. Morris; Shaojun Xu; Damian M. Wilary; Yinyong Sun; Yongqiang Cheng; Claire A. Murray; Chiu C. Tang; Mark D. Frogley; Gianfelice Cinque; Tristan Lowe; Haifei Zhang; Anibal J. Ramirez-Cuesta; K. Mark Thomas; Leslie W. Bolton; Sihai Yang; Martin Schröder

doi:10.1038/s41467-020-17640-4

Refinement of pore size at sub-angstrom precision in robust metal–organic frameworks for separation of xylenes

Xiaolin Li, Juehua Wang, Nannan Bai, Xinran Zhang, Xue Han, Ivan da Silva, Christopher G. Morris, Shaojun Xu, Damian M. Wilary, Yinyong Sun, Yongqiang Cheng, Claire A. Murray, Chiu C. Tang, Mark D. Frogley, Gianfelice Cinque, Tristan Lowe, Haifei Zhang, Anibal J. Ramirez-Cuesta, K. Mark Thomas, Leslie W. BoltonSihai Yang, Martin Schröder

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Abstract

The demand for xylenes is projected to increase over the coming decades. The separation of xylene isomers, particularly p- and m-xylenes, is vital for the production of numerous polymers and materials. However, current state-of-the-art separation is based upon fractional crystallisation at 220 K which is highly energy intensive. Here, we report the discrimination of xylene isomers via refinement of the pore size in a series of porous metal–organic frameworks, MFM-300, at sub-angstrom precision leading to the optimal kinetic separation of all three xylene isomers at room temperature. The exceptional performance of MFM-300 for xylene separation is confirmed by dynamic ternary breakthrough experiments. In-depth structural and vibrational investigations using synchrotron X-ray diffraction and terahertz spectroscopy define the underlying host–guest interactions that give rise to the observed selectivity (p-xylene < o-xylene < m-xylene) and separation factors of 4.6–18 for p- and m-xylenes.

Original language	English
Article number	4280
Journal	Nature Communications
Volume	11
Issue number	1
DOIs	https://doi.org/10.1038/s41467-020-17640-4
State	Published - Dec 1 2020

Funding

We thank EPSRC (EP/I011870), 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 especially grateful to Diamond Light Source for access to Beamlines I11 and B22. The computing resources were made available through the VirtuES and the ICE-MAN projects funded by Laboratory Directed Research and Development programme and by Compute and Data Environment for Science (CADES) at ORNL. XL, JW, NB and XZ acknowledge the financial support from Chinese Scholarship Council and the Newton Fund.

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Li, X., Wang, J., Bai, N., Zhang, X., Han, X., da Silva, I., Morris, C. G., Xu, S., Wilary, D. M., Sun, Y., Cheng, Y., Murray, C. A., Tang, C. C., Frogley, M. D., Cinque, G., Lowe, T., Zhang, H., Ramirez-Cuesta, A. J., Thomas, K. M., ... Schröder, M. (2020). Refinement of pore size at sub-angstrom precision in robust metal–organic frameworks for separation of xylenes. Nature Communications, 11(1), Article 4280. https://doi.org/10.1038/s41467-020-17640-4

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title = "Refinement of pore size at sub-angstrom precision in robust metal–organic frameworks for separation of xylenes",

abstract = "The demand for xylenes is projected to increase over the coming decades. The separation of xylene isomers, particularly p- and m-xylenes, is vital for the production of numerous polymers and materials. However, current state-of-the-art separation is based upon fractional crystallisation at 220 K which is highly energy intensive. Here, we report the discrimination of xylene isomers via refinement of the pore size in a series of porous metal–organic frameworks, MFM-300, at sub-angstrom precision leading to the optimal kinetic separation of all three xylene isomers at room temperature. The exceptional performance of MFM-300 for xylene separation is confirmed by dynamic ternary breakthrough experiments. In-depth structural and vibrational investigations using synchrotron X-ray diffraction and terahertz spectroscopy define the underlying host–guest interactions that give rise to the observed selectivity (p-xylene < o-xylene < m-xylene) and separation factors of 4.6–18 for p- and m-xylenes.",

author = "Xiaolin Li and Juehua Wang and Nannan Bai and Xinran Zhang and Xue Han and {da Silva}, Ivan and Morris, {Christopher G.} and Shaojun Xu and Wilary, {Damian M.} and Yinyong Sun and Yongqiang Cheng and Murray, {Claire A.} and Tang, {Chiu C.} and Frogley, {Mark D.} and Gianfelice Cinque and Tristan Lowe and Haifei Zhang and Ramirez-Cuesta, {Anibal J.} and Thomas, {K. Mark} and Bolton, {Leslie W.} and Sihai Yang and Martin Schr{\"o}der",

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Li, X, Wang, J, Bai, N, Zhang, X, Han, X, da Silva, I, Morris, CG, Xu, S, Wilary, DM, Sun, Y, Cheng, Y, Murray, CA, Tang, CC, Frogley, MD, Cinque, G, Lowe, T, Zhang, H, Ramirez-Cuesta, AJ, Thomas, KM, Bolton, LW, Yang, S & Schröder, M 2020, 'Refinement of pore size at sub-angstrom precision in robust metal–organic frameworks for separation of xylenes', Nature Communications, vol. 11, no. 1, 4280. https://doi.org/10.1038/s41467-020-17640-4

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AU - Han, Xue

AU - da Silva, Ivan

AU - Morris, Christopher G.

AU - Xu, Shaojun

AU - Wilary, Damian M.

AU - Sun, Yinyong

AU - Cheng, Yongqiang

AU - Murray, Claire A.

AU - Tang, Chiu C.

AU - Frogley, Mark D.

AU - Cinque, Gianfelice

AU - Lowe, Tristan

AU - Zhang, Haifei

AU - Ramirez-Cuesta, Anibal J.

AU - Thomas, K. Mark

AU - Bolton, Leslie W.

AU - Yang, Sihai

AU - Schröder, Martin

PY - 2020/12/1

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N2 - The demand for xylenes is projected to increase over the coming decades. The separation of xylene isomers, particularly p- and m-xylenes, is vital for the production of numerous polymers and materials. However, current state-of-the-art separation is based upon fractional crystallisation at 220 K which is highly energy intensive. Here, we report the discrimination of xylene isomers via refinement of the pore size in a series of porous metal–organic frameworks, MFM-300, at sub-angstrom precision leading to the optimal kinetic separation of all three xylene isomers at room temperature. The exceptional performance of MFM-300 for xylene separation is confirmed by dynamic ternary breakthrough experiments. In-depth structural and vibrational investigations using synchrotron X-ray diffraction and terahertz spectroscopy define the underlying host–guest interactions that give rise to the observed selectivity (p-xylene < o-xylene < m-xylene) and separation factors of 4.6–18 for p- and m-xylenes.

AB - The demand for xylenes is projected to increase over the coming decades. The separation of xylene isomers, particularly p- and m-xylenes, is vital for the production of numerous polymers and materials. However, current state-of-the-art separation is based upon fractional crystallisation at 220 K which is highly energy intensive. Here, we report the discrimination of xylene isomers via refinement of the pore size in a series of porous metal–organic frameworks, MFM-300, at sub-angstrom precision leading to the optimal kinetic separation of all three xylene isomers at room temperature. The exceptional performance of MFM-300 for xylene separation is confirmed by dynamic ternary breakthrough experiments. In-depth structural and vibrational investigations using synchrotron X-ray diffraction and terahertz spectroscopy define the underlying host–guest interactions that give rise to the observed selectivity (p-xylene < o-xylene < m-xylene) and separation factors of 4.6–18 for p- and m-xylenes.

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Refinement of pore size at sub-angstrom precision in robust metal–organic frameworks for separation of xylenes

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