Lattice-driven gating in a Cu-based zeolitic imidazolate framework for efficient high-temperature hydrogen isotope separation
Abstract For the separation of hydrogen isotopes (H2/D2), traditional kinetic quantum sieving (KQS) takes advantage of the diffusion barriers created by the flexibility of organic linkers and the breathing frameworks in porous solids. While the phenomena have been observed typically below 77 K, in t...
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Nature Portfolio
2025-02-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56649-5 |
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| author | Minji Jung Jaewoo Park Raeesh Muhammad Taeung Park Sung-Yeop Jung Jungwon Yi Cheolwon Jung Jacques Ollivier Anibal J. Ramirez-Cuesta Jitae T. Park Jaheon Kim Margarita Russina Hyunchul Oh |
| author_facet | Minji Jung Jaewoo Park Raeesh Muhammad Taeung Park Sung-Yeop Jung Jungwon Yi Cheolwon Jung Jacques Ollivier Anibal J. Ramirez-Cuesta Jitae T. Park Jaheon Kim Margarita Russina Hyunchul Oh |
| author_sort | Minji Jung |
| collection | DOAJ |
| description | Abstract For the separation of hydrogen isotopes (H2/D2), traditional kinetic quantum sieving (KQS) takes advantage of the diffusion barriers created by the flexibility of organic linkers and the breathing frameworks in porous solids. While the phenomena have been observed typically below 77 K, in this study, we present that a copper-based zeolite imidazolate framework (Cu-ZIF-gis) can show KQS above 120 K. Since Cu-ZIF-gis has narrow channels with ca. 2.4 Å in aperture, the small pore size itself acts as a diffusion barrier. This barrier changes with temperatures, leading to pore contraction or expansion through lattice-driven gating (LDG). The H2 adsorption isotherms measured at 40 – 150 K reflect the temperature sensitivity of the pore properties. Quasi-elastic neutron scattering (QENS) experiments indicate a notable difference in the molecular mobility of H2 and D2, even at temperatures exceeding 150 K. Temperature-variation powder X-ray diffraction measurements at 20 – 300 K show a small but gradual increase in the unit cell volume, indicating that LDG gives rise to the KQS at temperatures above 120 K. These findings can be applied to develop sustainable isotope separation technologies using existing LNG cryogenic infrastructure. |
| format | Article |
| id | doaj-art-6f6d6644df244c38b22f9504a9c9cf55 |
| institution | DOAJ |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Nature Portfolio |
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| series | Nature Communications |
| spelling | doaj-art-6f6d6644df244c38b22f9504a9c9cf552025-08-20T03:10:07ZengNature PortfolioNature Communications2041-17232025-02-0116111110.1038/s41467-025-56649-5Lattice-driven gating in a Cu-based zeolitic imidazolate framework for efficient high-temperature hydrogen isotope separationMinji Jung0Jaewoo Park1Raeesh Muhammad2Taeung Park3Sung-Yeop Jung4Jungwon Yi5Cheolwon Jung6Jacques Ollivier7Anibal J. Ramirez-Cuesta8Jitae T. Park9Jaheon Kim10Margarita Russina11Hyunchul Oh12Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST)Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST)Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST)Graduate School of Carbon Neutrality, Ulsan National Institute of Science and Technology (UNIST)Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST)Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST)Department of Chemistry, Soongsil UniversityInstitute Laue-Langevin, 71 avenue des Martyrs CS 20156, 38042Neutron Scattering Division, Oak Ridge National LaboratoryHeinz Maier-Leibnitz Zentrum (MLZ), Technische Universität MünchenDepartment of Chemistry, Soongsil UniversityHelmholtz Zentrum Berlin fur Materialien und Energie Hahn-Meitner-Platz 1Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST)Abstract For the separation of hydrogen isotopes (H2/D2), traditional kinetic quantum sieving (KQS) takes advantage of the diffusion barriers created by the flexibility of organic linkers and the breathing frameworks in porous solids. While the phenomena have been observed typically below 77 K, in this study, we present that a copper-based zeolite imidazolate framework (Cu-ZIF-gis) can show KQS above 120 K. Since Cu-ZIF-gis has narrow channels with ca. 2.4 Å in aperture, the small pore size itself acts as a diffusion barrier. This barrier changes with temperatures, leading to pore contraction or expansion through lattice-driven gating (LDG). The H2 adsorption isotherms measured at 40 – 150 K reflect the temperature sensitivity of the pore properties. Quasi-elastic neutron scattering (QENS) experiments indicate a notable difference in the molecular mobility of H2 and D2, even at temperatures exceeding 150 K. Temperature-variation powder X-ray diffraction measurements at 20 – 300 K show a small but gradual increase in the unit cell volume, indicating that LDG gives rise to the KQS at temperatures above 120 K. These findings can be applied to develop sustainable isotope separation technologies using existing LNG cryogenic infrastructure.https://doi.org/10.1038/s41467-025-56649-5 |
| spellingShingle | Minji Jung Jaewoo Park Raeesh Muhammad Taeung Park Sung-Yeop Jung Jungwon Yi Cheolwon Jung Jacques Ollivier Anibal J. Ramirez-Cuesta Jitae T. Park Jaheon Kim Margarita Russina Hyunchul Oh Lattice-driven gating in a Cu-based zeolitic imidazolate framework for efficient high-temperature hydrogen isotope separation Nature Communications |
| title | Lattice-driven gating in a Cu-based zeolitic imidazolate framework for efficient high-temperature hydrogen isotope separation |
| title_full | Lattice-driven gating in a Cu-based zeolitic imidazolate framework for efficient high-temperature hydrogen isotope separation |
| title_fullStr | Lattice-driven gating in a Cu-based zeolitic imidazolate framework for efficient high-temperature hydrogen isotope separation |
| title_full_unstemmed | Lattice-driven gating in a Cu-based zeolitic imidazolate framework for efficient high-temperature hydrogen isotope separation |
| title_short | Lattice-driven gating in a Cu-based zeolitic imidazolate framework for efficient high-temperature hydrogen isotope separation |
| title_sort | lattice driven gating in a cu based zeolitic imidazolate framework for efficient high temperature hydrogen isotope separation |
| url | https://doi.org/10.1038/s41467-025-56649-5 |
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