Isotope-selective pore opening in a flexible metal-organic framework

Linda Bondorf; Jhonatan Luiz Fiorio; Volodymyr Bon; Linda Zhang; Mariia Maliuta; Sebastian Ehrling; Irena Senkovska; Jack D. Evans; Jan Ole Joswig; Stefan Kaskel; Thomas Heine; Michael Hirscher

doi:10.1126/sciadv.abn7035

Isotope-selective pore opening in a flexible metal-organic framework

Linda Bondorf, Jhonatan Luiz Fiorio, Volodymyr Bon, Linda Zhang, Mariia Maliuta, Sebastian Ehrling, Irena Senkovska, Jack D. Evans, Jan Ole Joswig, Stefan Kaskel, Thomas Heine, Michael Hirscher

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

2 Citations (Scopus)

Abstract

Flexible metal-organic frameworks that show reversible guest-induced phase transitions between closed and open pore phases have enormous potential for highly selective, energy-efficient gas separations. Here, we present the gate-opening process of DUT-8(Ni) that selectively responds to D₂, whereas no response is observed for H₂ and HD. In situ neutron diffraction directly reveals this pressure-dependent phase transition. Low-temperature thermal desorption spectroscopy measurements indicate an outstanding D₂-over-H₂ selectivity of 11.6 at 23.3 K, with high D₂ uptake. First-principles calculations coupled with statistical thermodynamics predict the isotope-selective gate opening, rationalized by pronounced nuclear quantum effects. Simulations suggest DUT-8(Ni) to remain closed in the presence of HT, while it also opens for DT and T₂, demonstrating gate opening as a highly effective approach for isotopolog separation.

Original language	English
Article number	eabn7035
Journal	Science Advances
Volume	8
Issue number	15
DOIs	https://doi.org/10.1126/sciadv.abn7035
Publication status	Published - 2022 Apr

Bibliographical note

Funding Information:
The current study was funded by DFG within FOR2433 research unit “MOF-switches.” V.B. thanks BMBF (project no. 05K19OD2) for financial support. J.D.E. is supported by a Ramsay Fellowship from the University of Adelaide. T.H. thanks DFG RTG2721 “Hydrogen Isotopes.” ZIH Dresden and Phoenix HPC service at the University of Adelaide are thanked for providing high-performance computing resources.

Publisher Copyright:
Copyright © 2022 The Authors, some rights reserved.

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title = "Isotope-selective pore opening in a flexible metal-organic framework",

abstract = "Flexible metal-organic frameworks that show reversible guest-induced phase transitions between closed and open pore phases have enormous potential for highly selective, energy-efficient gas separations. Here, we present the gate-opening process of DUT-8(Ni) that selectively responds to D2, whereas no response is observed for H2 and HD. In situ neutron diffraction directly reveals this pressure-dependent phase transition. Low-temperature thermal desorption spectroscopy measurements indicate an outstanding D2-over-H2 selectivity of 11.6 at 23.3 K, with high D2 uptake. First-principles calculations coupled with statistical thermodynamics predict the isotope-selective gate opening, rationalized by pronounced nuclear quantum effects. Simulations suggest DUT-8(Ni) to remain closed in the presence of HT, while it also opens for DT and T2, demonstrating gate opening as a highly effective approach for isotopolog separation.",

author = "Linda Bondorf and Fiorio, {Jhonatan Luiz} and Volodymyr Bon and Linda Zhang and Mariia Maliuta and Sebastian Ehrling and Irena Senkovska and Evans, {Jack D.} and Joswig, {Jan Ole} and Stefan Kaskel and Thomas Heine and Michael Hirscher",

note = "Funding Information: The current study was funded by DFG within FOR2433 research unit “MOF-switches.” V.B. thanks BMBF (project no. 05K19OD2) for financial support. J.D.E. is supported by a Ramsay Fellowship from the University of Adelaide. T.H. thanks DFG RTG2721 “Hydrogen Isotopes.” ZIH Dresden and Phoenix HPC service at the University of Adelaide are thanked for providing high-performance computing resources. Publisher Copyright: Copyright {\textcopyright} 2022 The Authors, some rights reserved.",

year = "2022",

month = apr,

doi = "10.1126/sciadv.abn7035",

language = "English",

volume = "8",

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AU - Bondorf, Linda

AU - Fiorio, Jhonatan Luiz

AU - Bon, Volodymyr

AU - Zhang, Linda

AU - Maliuta, Mariia

AU - Ehrling, Sebastian

AU - Senkovska, Irena

AU - Evans, Jack D.

AU - Joswig, Jan Ole

AU - Kaskel, Stefan

AU - Heine, Thomas

AU - Hirscher, Michael

N1 - Funding Information: The current study was funded by DFG within FOR2433 research unit “MOF-switches.” V.B. thanks BMBF (project no. 05K19OD2) for financial support. J.D.E. is supported by a Ramsay Fellowship from the University of Adelaide. T.H. thanks DFG RTG2721 “Hydrogen Isotopes.” ZIH Dresden and Phoenix HPC service at the University of Adelaide are thanked for providing high-performance computing resources. Publisher Copyright: Copyright © 2022 The Authors, some rights reserved.

PY - 2022/4

Y1 - 2022/4

N2 - Flexible metal-organic frameworks that show reversible guest-induced phase transitions between closed and open pore phases have enormous potential for highly selective, energy-efficient gas separations. Here, we present the gate-opening process of DUT-8(Ni) that selectively responds to D2, whereas no response is observed for H2 and HD. In situ neutron diffraction directly reveals this pressure-dependent phase transition. Low-temperature thermal desorption spectroscopy measurements indicate an outstanding D2-over-H2 selectivity of 11.6 at 23.3 K, with high D2 uptake. First-principles calculations coupled with statistical thermodynamics predict the isotope-selective gate opening, rationalized by pronounced nuclear quantum effects. Simulations suggest DUT-8(Ni) to remain closed in the presence of HT, while it also opens for DT and T2, demonstrating gate opening as a highly effective approach for isotopolog separation.

AB - Flexible metal-organic frameworks that show reversible guest-induced phase transitions between closed and open pore phases have enormous potential for highly selective, energy-efficient gas separations. Here, we present the gate-opening process of DUT-8(Ni) that selectively responds to D2, whereas no response is observed for H2 and HD. In situ neutron diffraction directly reveals this pressure-dependent phase transition. Low-temperature thermal desorption spectroscopy measurements indicate an outstanding D2-over-H2 selectivity of 11.6 at 23.3 K, with high D2 uptake. First-principles calculations coupled with statistical thermodynamics predict the isotope-selective gate opening, rationalized by pronounced nuclear quantum effects. Simulations suggest DUT-8(Ni) to remain closed in the presence of HT, while it also opens for DT and T2, demonstrating gate opening as a highly effective approach for isotopolog separation.

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Isotope-selective pore opening in a flexible metal-organic framework

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