Isotopologue-induced structural dynamics of a triazolate metal-organic framework for efficient hydrogen isotope separation

Linda Zhang; Richard Röß-Ohlenroth; Vanessa K. Peterson; Samuel G. Duyker; Cheng Li; Jhonatan Luiz Fiorio; Jan Ole Joswig; Robert Dinnebier; Dirk Volkmer; Michael Hirscher

doi:10.1038/s41467-025-61107-3

Isotopologue-induced structural dynamics of a triazolate metal-organic framework for efficient hydrogen isotope separation

Linda Zhang
, Richard Röß-Ohlenroth
, Vanessa K. Peterson
, Samuel G. Duyker
, Cheng Li
, Jhonatan Luiz Fiorio
, Jan Ole Joswig
, Robert Dinnebier
, Dirk Volkmer
, Michael Hirscher

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

2 Scopus citations

Abstract

Efficient hydrogen isotope separation remains the biggest challenge due to the nearly identical physicochemical properties of H₂ and D₂. Through in situ neutron powder diffraction and gas adsorption experiments, we investigate the hydrogen isotopologue-induced structural dynamics of the triazole-based metal-organic framework [Mn(ta)₂]. Gas loading induces a measurable lattice expansion, more pronounced for H₂ than D₂, and two distinct adsorption sites are identified with a subtle but significant difference in the occupancy of H₂ and D₂ at 60 K. Cryogenic thermal desorption spectroscopy after exposure to a 1:1 isotope mixture reveals an exceptionally high D₂/H₂ selectivity of 32.5 at 60 K. When exposed to a D₂/H₂ mixture of 5:95, D₂ enriches to 75% in a single cycle. Given the commercial availability of the ligand and the scalability of the dia-framework topology across divalent transition metals, upscaling for industrial-scale deuterium separation is a realistic prospect. Our results give crucial molecular-level insights into isotopologue-induced structural dynamics in triazolate-based MOFs and provide guidance for improvement of isotope separation materials.

Original language	English
Article number	5941
Journal	Nature Communications
Volume	16
Issue number	1
DOIs	https://doi.org/10.1038/s41467-025-61107-3
State	Published - Dec 2025
Externally published	Yes

Funding

L.Z. is grateful for partial funding by the Japan Society for the Promotion of Science (JSPS) Grants-in-Aid for Scientific Research (KAKENHI) (No. JP24K17650). We gratefully acknowledge the Australian Nuclear Science and Technology Organisation (ANSTO; proposal number P9673) and the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory (ORNL; proposal number IPTS-29081.1) for providing the neutron beamtime essential to this research. J.-O. J. thanks the Zentrum für Informationsdienste und Hochleistungsrechnen (ZIH) at TU Dresden for granted computational time within project TRANSPHEMAT. L. Z. thanks Prof. Hao Li from Tohoku University, for his suggestions, proofreading, and constructive feedback.

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title = "Isotopologue-induced structural dynamics of a triazolate metal-organic framework for efficient hydrogen isotope separation",

abstract = "Efficient hydrogen isotope separation remains the biggest challenge due to the nearly identical physicochemical properties of H2 and D2. Through in situ neutron powder diffraction and gas adsorption experiments, we investigate the hydrogen isotopologue-induced structural dynamics of the triazole-based metal-organic framework [Mn(ta)2]. Gas loading induces a measurable lattice expansion, more pronounced for H2 than D2, and two distinct adsorption sites are identified with a subtle but significant difference in the occupancy of H2 and D2 at 60 K. Cryogenic thermal desorption spectroscopy after exposure to a 1:1 isotope mixture reveals an exceptionally high D2/H2 selectivity of 32.5 at 60 K. When exposed to a D2/H2 mixture of 5:95, D2 enriches to 75\% in a single cycle. Given the commercial availability of the ligand and the scalability of the dia-framework topology across divalent transition metals, upscaling for industrial-scale deuterium separation is a realistic prospect. Our results give crucial molecular-level insights into isotopologue-induced structural dynamics in triazolate-based MOFs and provide guidance for improvement of isotope separation materials.",

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AU - Röß-Ohlenroth, Richard

AU - Peterson, Vanessa K.

AU - Duyker, Samuel G.

AU - Li, Cheng

AU - Fiorio, Jhonatan Luiz

AU - Joswig, Jan Ole

AU - Dinnebier, Robert

AU - Volkmer, Dirk

AU - Hirscher, Michael

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N2 - Efficient hydrogen isotope separation remains the biggest challenge due to the nearly identical physicochemical properties of H2 and D2. Through in situ neutron powder diffraction and gas adsorption experiments, we investigate the hydrogen isotopologue-induced structural dynamics of the triazole-based metal-organic framework [Mn(ta)2]. Gas loading induces a measurable lattice expansion, more pronounced for H2 than D2, and two distinct adsorption sites are identified with a subtle but significant difference in the occupancy of H2 and D2 at 60 K. Cryogenic thermal desorption spectroscopy after exposure to a 1:1 isotope mixture reveals an exceptionally high D2/H2 selectivity of 32.5 at 60 K. When exposed to a D2/H2 mixture of 5:95, D2 enriches to 75% in a single cycle. Given the commercial availability of the ligand and the scalability of the dia-framework topology across divalent transition metals, upscaling for industrial-scale deuterium separation is a realistic prospect. Our results give crucial molecular-level insights into isotopologue-induced structural dynamics in triazolate-based MOFs and provide guidance for improvement of isotope separation materials.

AB - Efficient hydrogen isotope separation remains the biggest challenge due to the nearly identical physicochemical properties of H2 and D2. Through in situ neutron powder diffraction and gas adsorption experiments, we investigate the hydrogen isotopologue-induced structural dynamics of the triazole-based metal-organic framework [Mn(ta)2]. Gas loading induces a measurable lattice expansion, more pronounced for H2 than D2, and two distinct adsorption sites are identified with a subtle but significant difference in the occupancy of H2 and D2 at 60 K. Cryogenic thermal desorption spectroscopy after exposure to a 1:1 isotope mixture reveals an exceptionally high D2/H2 selectivity of 32.5 at 60 K. When exposed to a D2/H2 mixture of 5:95, D2 enriches to 75% in a single cycle. Given the commercial availability of the ligand and the scalability of the dia-framework topology across divalent transition metals, upscaling for industrial-scale deuterium separation is a realistic prospect. Our results give crucial molecular-level insights into isotopologue-induced structural dynamics in triazolate-based MOFs and provide guidance for improvement of isotope separation materials.

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Isotopologue-induced structural dynamics of a triazolate metal-organic framework for efficient hydrogen isotope separation

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