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Coordinated Water as New Binding Sites for the Separation of Light Hydrocarbons in Metal–Organic Frameworks with Open Metal Sites

  • Pia Vervoorts
    Pia Vervoorts
    Inorganic and Metal−Organic Chemistry, Technical University of Munich, Lichtenbergstrasse 4, 85748 Garching, Germany
    Inorganic Chemistry II, Ruhr-University Bochum, Universitätsstrasse 150, 44801 Bochum, Germany
  • Andreas Schneemann
    Andreas Schneemann
    Inorganic and Metal−Organic Chemistry, Technical University of Munich, Lichtenbergstrasse 4, 85748 Garching, Germany
  • Inke Hante
    Inke Hante
    Inorganic Chemistry II, Ruhr-University Bochum, Universitätsstrasse 150, 44801 Bochum, Germany
    More by Inke Hante
  • Jenny Pirillo
    Jenny Pirillo
    Institute for Chemical Reaction Design and Discovery (WPI-ICReDD), Hokkaido University, Sapporo 001-0021, Japan
  • Yuh Hijikata
    Yuh Hijikata
    Institute for Chemical Reaction Design and Discovery (WPI-ICReDD), Hokkaido University, Sapporo 001-0021, Japan
    More by Yuh Hijikata
  • Takashi Toyao
    Takashi Toyao
    Institute for Catalysis, Hokkaido University, Sapporo 001-0020, Japan
    Elements Strategy Initiative for Catalysis and Batteries, Kyoto University, Katsura, Kyoto 615-8520, Japan
  • Kenichi Kon
    Kenichi Kon
    Institute for Catalysis, Hokkaido University, Sapporo 001-0020, Japan
    More by Kenichi Kon
  • Ken-ichi Shimizu
    Ken-ichi Shimizu
    Institute for Catalysis, Hokkaido University, Sapporo 001-0020, Japan
    Elements Strategy Initiative for Catalysis and Batteries, Kyoto University, Katsura, Kyoto 615-8520, Japan
  • Takayoshi Nakamura
    Takayoshi Nakamura
    Research Institute for Electronic Science, Hokkaido University, Sapporo 001-0020, Japan
  • Shin-ichiro Noro*
    Shin-ichiro Noro
    Faculty of Environmental Earth Science, Hokkaido University, Sapporo 060-0810, Japan
    *Email: [email protected]
  • , and 
  • Roland A. Fischer*
    Roland A. Fischer
    Inorganic and Metal−Organic Chemistry, Technical University of Munich, Lichtenbergstrasse 4, 85748 Garching, Germany
    *Email: [email protected]
Cite this: ACS Appl. Mater. Interfaces 2020, 12, 8, 9448–9456
Publication Date (Web):January 27, 2020
https://doi.org/10.1021/acsami.9b21261
Copyright © 2020 American Chemical Society

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    Abstract

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    Metal–organic frameworks with open metal sites are promising materials for gas separations. Particularly, the M2(dobdc) (dobdc4– = 2,5-dioxidobenzenedicarboxylate, M2+ = Co2+, Mn2+, Fe2+, ...) framework has been the Drosophila of this research field and has delivered groundbreaking results in terms of sorption selectivity. However, many studies focus on perfect two-component mixtures and use theoretical models, e.g., the ideal adsorbed solution theory, to calculate selectivities. Within this work, we shed light on the comparability of these selectivities with values obtained from propane/propene multicomponent measurements on the prototypical Co2(dobdc) framework, and we study the impact of impurities like water on the selectivity. Despite the expected capacity loss, the presence of water does not necessarily lead to a decreased selectivity. Density functional theory calculations of the binding energies prove that the water molecules adsorbed to the metal centers introduce new binding sites for the adsorbates.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.9b21261.

    • Full details of syntheses and characterization (PXRD, IR, 1H NMR, TGA, and TPD measurements), all single and coadsorption measurements, description and principle of the measurement setup, dual-site Langmuir–Freundlich fits, selectivity, and DFT calculations (PDF)

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    Cited By

    This article is cited by 12 publications.

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    2. Arianjel F. Hernandez, Rebekah K. Impastato, Mohammad I. Hossain, Brooks D. Rabideau, T. Grant Glover. Water Bridges Substitute for Defects in Amine-Functionalized UiO-66, Boosting CO2 Adsorption. Langmuir 2021, 37 (35) , 10439-10449. https://doi.org/10.1021/acs.langmuir.1c01149
    3. Arpan Hazra, Aashima Jain, M. S. Deenadayalan, Stephen Adie Adalikwu, Tapas Kumar Maji. Acetylene/Ethylene Separation and Solid-State Structural Transformation via [2 + 2] Cycloaddition Reactions in 3D Microporous ZnII Metal–Organic Frameworks. Inorganic Chemistry 2020, 59 (13) , 9055-9064. https://doi.org/10.1021/acs.inorgchem.0c00932
    4. Yuqing Xiao, Shenhui Li, Bin Jiang, Xinmiao Liang, Yueying Chu, Feng Deng. Effect of Co‐Adsorbed Guest Adsorbates on the Separation of Ethylene/Ethane Mixtures on Metal‐Organic Frameworks with Open Metal Sites. Chemistry – A European Journal 2024, https://doi.org/10.1002/chem.202401006
    5. Lan Yang, Qiang Gao, Ya-Nan Li, Qian-Nan Liu, Xiao-Ting Liu, Sihui Wang, Jia-Bin Hu, Li-Zhuang Chen. Efficient purification of CH4 from ternary mixtures by a microporous heterometal-organic framework. Separation and Purification Technology 2024, 335 , 126235. https://doi.org/10.1016/j.seppur.2023.126235
    6. Yifan Gu, Jia-Jia Zheng, Ken-ichi Otake, Shigeyoshi Sakaki, Hirotaka Ashitani, Yoshiki Kubota, Shogo Kawaguchi, Ming-Shui Yao, Ping Wang, Ying Wang, Fengting Li, Susumu Kitagawa. Soft corrugated channel with synergistic exclusive discrimination gating for CO2 recognition in gas mixture. Nature Communications 2023, 14 (1) https://doi.org/10.1038/s41467-023-39470-w
    7. Brendon Lalchawimawia, Anirban Sil, Tirthankar Banerjee, Neera Singh, Amit Bhatnagar, Raj Mukhopadhyay, Abhishek Mandal. Metal-organic framework-pesticide interactions in water: Present and future perspectives on monitoring, remediation and molecular simulation. Coordination Chemistry Reviews 2023, 490 , 215214. https://doi.org/10.1016/j.ccr.2023.215214
    8. M. Priyadarshini, A. Ahmad, S. Das, M. M. Ghangrekar. Metal organic frameworks as emergent oxygen-reducing cathode catalysts for microbial fuel cells: a review. International Journal of Environmental Science and Technology 2022, 19 (11) , 11539-11560. https://doi.org/10.1007/s13762-021-03499-5
    9. Andreas Schneemann, Yuan Jing, Jack D. Evans, Takashi Toyao, Yuh Hijikata, Yuichi Kamiya, Ken-ichi Shimizu, Nicholas C. Burtch, Shin-ichiro Noro. Alkyl decorated metal–organic frameworks for selective trapping of ethane from ethylene above ambient pressures. Dalton Transactions 2021, 50 (30) , 10423-10435. https://doi.org/10.1039/D1DT01477C
    10. Éadaoin Whelan, Friedrich W. Steuber, Thorfinnur Gunnlaugsson, Wolfgang Schmitt. Tuning photoactive metal–organic frameworks for luminescence and photocatalytic applications. Coordination Chemistry Reviews 2021, 437 , 213757. https://doi.org/10.1016/j.ccr.2020.213757
    11. Vanesa del C. Cotlame-Salinas, Alfredo López-Olvera, Alejandro Islas-Jácome, Eduardo González-Zamora, Ilich A. Ibarra. CO 2 capture enhancement in MOFs via the confinement of molecules. Reaction Chemistry & Engineering 2021, 6 (3) , 441-453. https://doi.org/10.1039/D0RE00410C
    12. Miroslav Almáši, Vladimír Zeleňák, Róbert Gyepes, Ľuboš Zauška, Sandrine Bourrelly. A series of four novel alkaline earth metal–organic frameworks constructed of Ca( ii ), Sr( ii ), Ba( ii ) ions and tetrahedral MTB linker: structural diversity, stability study and low/high-pressure gas adsorption properties. RSC Advances 2020, 10 (54) , 32323-32334. https://doi.org/10.1039/D0RA05145D

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