ACS Publications. Most Trusted. Most Cited. Most Read
Exploiting the Specific Isotope-Selective Adsorption of Metal–Organic Framework for Hydrogen Isotope Separation
My Activity

Figure 1Loading Img
    Communication

    Exploiting the Specific Isotope-Selective Adsorption of Metal–Organic Framework for Hydrogen Isotope Separation
    Click to copy article linkArticle link copied!

    • Raeesh Muhammad
      Raeesh Muhammad
      Department of Energy Engineering, Gyeongsang National University, Jinju 52725, Republic of Korea
    • Seohyeon Jee
      Seohyeon Jee
      Department of Chemical and Biological Engineering, Sookmyung Women’s University, 100 Cheongpa-ro 47 gil, Yongsan-gu, Seoul 04310, Republic of Korea
      More by Seohyeon Jee
    • Minji Jung
      Minji Jung
      Department of Energy Engineering, Gyeongsang National University, Jinju 52725, Republic of Korea
      More by Minji Jung
    • Jaewoo Park
      Jaewoo Park
      Department of Energy Engineering, Gyeongsang National University, Jinju 52725, Republic of Korea
      More by Jaewoo Park
    • Sung Gu Kang*
      Sung Gu Kang
      School of Chemical Engineering, University of Ulsan, Ulsan 44610, Republic of Korea
      *[email protected] (DFT calculations)
      More by Sung Gu Kang
    • Kyung Min Choi*
      Kyung Min Choi
      Department of Chemical and Biological Engineering, Sookmyung Women’s University, 100 Cheongpa-ro 47 gil, Yongsan-gu, Seoul 04310, Republic of Korea
      *[email protected] (material synthesis)
    • Hyunchul Oh*
      Hyunchul Oh
      Department of Energy Engineering, Gyeongsang National University, Jinju 52725, Republic of Korea
      Future Convergence Technology Research Institute, Jinju 52725, Republic of Korea
      *[email protected] (characterization)
      More by Hyunchul Oh
    Other Access OptionsSupporting Information (1)

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 22, 8232–8236
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.1c01694
    Published April 30, 2021
    Copyright © 2021 American Chemical Society

    Abstract

    Click to copy section linkSection link copied!
    Abstract Image

    Adsorptive separation using narrow-micropore adsorbents has demonstrated the potential to separate hydrogen isotopes. In this work, we employed an isotope-responsive separation using cobalt formate. A D2-responsive third sorption step was revealed, and consequently, a noticeable difference was observed in the uptakes of D2 and H2. This may have resulted from the additional space created for D2 due to its dense packing, as DFT calculations revealed that cobalt formate possesses 2.26 kJ/mol higher binding strength for D2 than for H2. The exploitation of this D2-responsive third sorption step renders a promising separation performance, with a D2/H2 selectivity of up to 44 at 25 K/1 bar. Lastly, cobalt formate was synthesized on a gram scale here, which makes it a prospect for commercialization.

    Copyright © 2021 American Chemical Society

    Read this article

    To access this article, please review the available access options below.

    Get instant access

    Purchase Access

    Read this article for 48 hours. Check out below using your ACS ID or as a guest.

    Recommended

    Access through Your Institution

    You may have access to this article through your institution.

    Your institution does not have access to this content. Add or change your institution or let them know you’d like them to include access.

    Supporting Information

    Click to copy section linkSection link copied!

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.1c01694.

    • Experimental details, structural characterization, thermal desorption spectra, and density functional theory calculations (PDF)

    Terms & Conditions

    Electronic Supporting Information files are available without a subscription to ACS Web Editions. The American Chemical Society holds a copyright ownership interest in any copyrightable Supporting Information. Files available from the ACS website may be downloaded for personal use only. Users are not otherwise permitted to reproduce, republish, redistribute, or sell any Supporting Information from the ACS website, either in whole or in part, in either machine-readable form or any other form without permission from the American Chemical Society. For permission to reproduce, republish and redistribute this material, requesters must process their own requests via the RightsLink permission system. Information about how to use the RightsLink permission system can be found at http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    Click to copy section linkSection link copied!

    This article is cited by 40 publications.

    1. Sung-Yeop Jung, Dajin Park, Hyunchul Oh. Dynamic Quantum Sieving of a Hydrogen Isotope Mixture: Beyond the Limitations of Small Pore Sizes. ACS Applied Energy Materials 2025, 8 (1) , 16-24. https://doi.org/10.1021/acsaem.4c02462
    2. Wenjun Dong, Jiamin Yuan, Jingyi Tan, Xiaomin Tang, Wentao Liu, Anmin Zheng, Wei Chen. Enhance Hydrogen Isotopes Separation by Alkali Earth Metal Dopant in Metal–Organic Framework. The Journal of Physical Chemistry Letters 2023, 14 (5) , 1198-1207. https://doi.org/10.1021/acs.jpclett.2c03657
    3. Xiaoyu Hu, Fengyun Ding, Renjin Xiong, Yongtao An, Xingwen Feng, Jiangfeng Song, Linsen Zhou, Peilong Li, Changlun Chen. Highly Effective H2/D2 Separation within the Stable Cu(I)Cu(II)-BTC: The Effect of Cu(I) Structure on Quantum Sieving. ACS Applied Materials & Interfaces 2023, 15 (3) , 3941-3952. https://doi.org/10.1021/acsami.2c18221
    4. Igor Bezverkhyy, Victor Boyer, Clément Cabaud, Jean-Pierre Bellat. High Efficiency of Na- and Ca-Exchanged Chabazites in D2/H2 Separation by Quantum Sieving. ACS Applied Materials & Interfaces 2022, 14 (47) , 52738-52744. https://doi.org/10.1021/acsami.2c12927
    5. Ping Zhou, Xinxin Wang, Lianglan Yue, Lihui Fan, Yabing He. A Microporous MOF Constructed by Cross-Linking Helical Chains for Efficient Purification of Natural Gas and Ethylene. Inorganic Chemistry 2021, 60 (19) , 14969-14977. https://doi.org/10.1021/acs.inorgchem.1c02363
    6. Minji Jung, Jaewoo Park, Jingwen Zhou, Taeung Park, Yoon-Chae Nah, Sally E.A. ElAshery, Sung Gu Kang, Nour F. Attia, Raeesh Muhammad, Hyunchul Oh. Thermally regulated gating phenomenon in bio-derived ultra-narrow nanoporous carbon for enhancing hydrogen isotope separation. Fuel 2025, 382 , 133754. https://doi.org/10.1016/j.fuel.2024.133754
    7. Wei Li, Jingyun Wang, Mengmeng Han, Shanshan Xu. Efficient N2/CH4 separation by mixed matrix membrane with bimetallic metal–organic framework. Inorganic Chemistry Communications 2025, 172 , 113757. https://doi.org/10.1016/j.inoche.2024.113757
    8. Hyunlim Kim, Younggyu Seo, Jaewoo Park, Eunsung Lee, Hyunchul Oh. A Gate‐Opening Control Strategy via Nitrate–Chloride Anion Exchange for Enhanced Hydrogen Isotope Separation in Metal–Organic Frameworks. Angewandte Chemie International Edition 2025, https://doi.org/10.1002/anie.202421756
    9. Hyunlim Kim, Younggyu Seo, Jaewoo Park, Eunsung Lee, Hyunchul Oh. A Gate‐Opening Control Strategy via Nitrate–Chloride Anion Exchange for Enhanced Hydrogen Isotope Separation in Metal–Organic Frameworks. Angewandte Chemie 2025, https://doi.org/10.1002/ange.202421756
    10. Yi-Peng Liu, Jing-Hong Li, Zi-Nan Chen, Wei Xue, Hao-Long Zhou, Rui-Biao Lin, Xiao-Ming Chen. Kinetic Separation of Butane Isomers Using a Formate Metal‐Organic Framework. ChemPlusChem 2025, https://doi.org/10.1002/cplu.202400756
    11. Xiufang Li, Yanxi Tan, Zhanfeng Ju, Wenjing Wang, Daqiang Yuan. Exploration of functional group effects on D 2 /H 2 separation selectivity within the UiO-66 framework. Inorganic Chemistry Frontiers 2025, 12 (2) , 701-706. https://doi.org/10.1039/D4QI02802C
    12. Sandeep Kumar, Raeesh Muhammad, Abdulkarem Amhamed, Hyunchul Oh. Unveiling the potential of ingenious copper-based metal-organic frameworks in gas storage and separation. Coordination Chemistry Reviews 2025, 522 , 216230. https://doi.org/10.1016/j.ccr.2024.216230
    13. Taku Kitayama, Tamon Yamauchi, Kaiji Uchida, Shunya Tanaka, Ryojun Toyoda, Hiroaki Iguchi, Ryota Sakamoto, Hao Xue, Naoki Kishimoto, Takefumi Yoshida, Tomoya Uruga, Shin-ichiro Noro, Shinya Takaishi. Hydrogen isotope separation at exceptionally high temperature using an unsaturated organometallic complex. Dalton Transactions 2025, 68 https://doi.org/10.1039/D4DT03018D
    14. Sandeep Kumar, Jaewoo Park, Hyunlim Kim, Sungyeop Jung, Taeung Park, Jonghyeok Park, Hye Jin Cho, Chan Woo Park, Hyunchul Oh. Quantum sieving in robust microporous zeolite SSZ-13 for efficient hydrogen isotope separation. International Journal of Hydrogen Energy 2025, 100 , 184-190. https://doi.org/10.1016/j.ijhydene.2024.12.298
    15. Huafeng Zhu, Liangbo Xu, Jia Li, Duanwei He, Jingchuan Wang. A Mini Review of Advances in Porous Materials Designing for Hydrogen Isotope Separation. Materials 2024, 17 (23) , 5708. https://doi.org/10.3390/ma17235708
    16. Hyunlim Kim, Minji Jung, Jaewoo Park, Taeung Park, Jonghyeok Park, Hyerin Lee, Balaji G. Ghule, Ji-Hyun Jang, Raeesh Muhammad, Sandeep Kumar, Hyunchul Oh. Metal-doped amorphous microporous carbon for isotope separation: Pore size modulation and selective deuterium adsorption. Carbon 2024, 230 , 119674. https://doi.org/10.1016/j.carbon.2024.119674
    17. Fei Gao, Xiaokang Wang, Wenmiao Chen, Wenjing Wang, Weidong Fan, Zixi Kang, Rongming Wang, Hailing Guo, Qin Yue, Daqiang Yuan, Daofeng Sun. Metal-organic frameworks for hydrogen isotopes separation. Coordination Chemistry Reviews 2024, 518 , 216047. https://doi.org/10.1016/j.ccr.2024.216047
    18. Yi Fang, Yizhi Han, Jialin Wang, Yehui Ding, Meng He, Jianhui Lan, Xiangdong Ding, Weiqun Shi, Xue Liu. Calix[4]arene-decorated polymers of intrinsic microporosity for lithium isotopes separation. Chemical Engineering Journal 2024, 500 , 156916. https://doi.org/10.1016/j.cej.2024.156916
    19. Hyunchul Oh, Minji Jung, Jaewoo Park, Raeesh Muhammad, Taeung Park, Jungwon Yi, Cheolwon Jung, Jacques Ollivier, Anibal J. Ramirez-Cuestae, Jitae Park, Jaheon Kim, Margarita Russina. Exploiting a Lattice-Driven Gating in a Cu-Based Zeolitic Imidazolate Framework for Efficient High-Temperature Hydrogen Isotope Separation. 2024https://doi.org/10.21203/rs.3.rs-4724831/v1
    20. Jingru Fu, Ying Wang, Saikat Das, Shuai Zhang, Xiqi Zhang, Hongyan Xiao, Jun Li, Teng Ben, Lei Jiang. Ultra-efficient deuterium separation under ambient conditions by a crystalline porous organic framework-Pd nanoparticle hybrid. Matter 2024, 7 (7) , 2460-2472. https://doi.org/10.1016/j.matt.2024.05.008
    21. Xiaolong Fu, Yu Gong, Jiamao Li, Jingwei Hou, Junyan Wang, Wenjie Ding, Chengjian Xiao, Hongwen Huang, Heyi Wang. Highly effective quantum sieving of hydrogen isotopes on flexible metal-organic frameworks with mobile ligands. Separation and Purification Technology 2024, 334 , 126025. https://doi.org/10.1016/j.seppur.2023.126025
    22. Lawrence Shere, Alfred K. Hill, Timothy J. Mays, Rachel Lawless, Rosemary Brown, Semali P. Perera. The next generation of low tritium hydrogen isotope separation technologies for future fusion power plants. International Journal of Hydrogen Energy 2024, 55 , 319-338. https://doi.org/10.1016/j.ijhydene.2023.10.282
    23. Minji Jung, Jaewoo Park, Jingwen Zhou, Taeung Park, Yoon-Chae Nah, Sally E.A. ElAshery, Sung Gu Kang, Nour Attia, Raeesh Muhammad, Hyunchul Oh. Thermally Regulated Gating Phenomenon in Bio-Derived Ultra-Narrow Nanoporous Carbon for Enhancing Hydrogen Isotope Separation. 2024https://doi.org/10.2139/ssrn.4772320
    24. Minji Jung, Jaewoo Park, Jingwen Zhou, Taeung Park, Yoon-Chae Nah, Sally E.A. ElAshery, Sung Gu Kang, Nour Attia, Raeesh Muhammad, Hyunchul Oh. Thermally Regulated Gating Phenomenon in Bio-Derived Ultra-Narrow Nanoporous Carbon for Enhancing Hydrogen Isotope Separation. 2024https://doi.org/10.2139/ssrn.4816768
    25. Hyunlim Kim, Minji Jung, Jaewoo Park, Taeung Park, Jonghyeok Park, Hyerin Lee, Raeesh Muhammad, Sandeep Kumar, Hyunchul Oh. Metal-Doped Amorphous Microporous Carbon for Isotope Separation: Pore Size Modulation and Selective Deuterium Adsorption. 2024https://doi.org/10.2139/ssrn.4901515
    26. Muruganantham Rethinasabapathy, Seyed Majid Ghoreishian, Seung‐Kyu Hwang, Young‐Kyu Han, Changhyun Roh, Yun Suk Huh. Recent Progress in Functional Nanomaterials towards the Storage, Separation, and Removal of Tritium. Advanced Materials 2023, 35 (48) https://doi.org/10.1002/adma.202301589
    27. Hyunlim Kim, Seohyeon Jee, Jaewoo Park, Minji Jung, Raeesh Muhammad, Kyungmin Choi, Hyunchul Oh. High D2/H2 selectivity performance in MOF-303 under ambient pressure for potential industrial applications. Separation and Purification Technology 2023, 325 , 124660. https://doi.org/10.1016/j.seppur.2023.124660
    28. Simon Leitner, Fridjof Sobanski, Gerhard Soja, Katharina Keiblinger, Christine Stumpp, Andrea Watzinger. Carbon isotope effects in the sorption of chlorinated ethenes on biochar and activated carbon. Heliyon 2023, 9 (10) , e20823. https://doi.org/10.1016/j.heliyon.2023.e20823
    29. Lingyun Kong, Enming Ping, Chunyan Ding, Lijuan Zhang, Yunshan Zhou, Nan Chen. Rapid diffusion of H 2 and strong adsorption of D 2 in Ni-4PyC realized the efficient separation of H 2 /D 2 by gas chromatography. Dalton Transactions 2023, 52 (30) , 10448-10456. https://doi.org/10.1039/D3DT01143G
    30. Nan Sun, Chen Yang, Jiang-Feng Song, Yin-Tao Li, Wen-Bin Yang, Yuan-Lin Zhou, De-Li Luo, Quan-Ping Zhang. Tailoring thermal resistance of porous materials with void filling for improved hydrogen adsorption. International Journal of Hydrogen Energy 2023, 48 (23) , 8588-8595. https://doi.org/10.1016/j.ijhydene.2022.11.254
    31. Jiaye Jin, Toshiki Wulf, Marcel Jorewitz, Thomas Heine, Knut R. Asmis. Vibrational spectroscopy of Cu + (H 2 ) 4 : about anharmonicity and fluxionality. Physical Chemistry Chemical Physics 2023, 25 (6) , 5262-5270. https://doi.org/10.1039/D2CP05802B
    32. Nan Chen, Xiaoxiao Chen, Enming Ping, Lijuan Zhang, Yunshan Zhou. Quantum Sieving Effects of Ni(bdc)(ted) 0.5 and Effective Separation Performance of Ni(bdc)(ted) 0.5 @γ‐Al 2 O 3 for H 2 /D 2. ChemistrySelect 2023, 8 (1) https://doi.org/10.1002/slct.202204150
    33. Enming Ping, Lingyun Kong, Mengyao Liu, Yunshan Zhou, Lijuan Zhang, Nan Chen. H 2 /D 2 separation in gas chromatography through a MOF-on-MOF strategy using γ-AlOOH@Al(OH)(1,4-NDC)@ZIF-67 as the stationary phase via additive effects of chemical affinity quantum sieving and kinetic sieving. Dalton Transactions 2023, 52 (2) , 376-383. https://doi.org/10.1039/D2DT03635E
    34. Hyunlim Kim, Seohyeon Jee, Jaewoo Park, Minji Jung, Raeesh Muhammad, Kyungmin Choi, Hyunchul Oh. Industry-Friendly D2/H2 Separation in Mof-303 at Ambient Pressure. 2023https://doi.org/10.2139/ssrn.4456751
    35. Faisal Rehman, Fida Hussain Memon, Zubeda Bhatti, Muzaffar Iqbal, Faheeda Soomro, Akbar Ali, Khalid Hussain Thebo. Graphene-based composite membranes for isotope separation: challenges and opportunities. Reviews in Inorganic Chemistry 2022, 42 (4) , 327-336. https://doi.org/10.1515/revic-2021-0035
    36. Mateusz Pokora, Agata Paneth, Piotr Paneth. Unprecedently large 37Cl/35Cl equilibrium isotopic fractionation on nano-confinement of chloride anion. Scientific Reports 2022, 12 (1) https://doi.org/10.1038/s41598-022-05629-6
    37. Donglin He, Linda Zhang, Tao Liu, Rob Clowes, Marc A. Little, Ming Liu, Michael Hirscher, Andrew I. Cooper. Hydrogen Isotope Separation Using a Metal–Organic Cage Built from Macrocycles. Angewandte Chemie 2022, 134 (32) https://doi.org/10.1002/ange.202202450
    38. Donglin He, Linda Zhang, Tao Liu, Rob Clowes, Marc A. Little, Ming Liu, Michael Hirscher, Andrew I. Cooper. Hydrogen Isotope Separation Using a Metal–Organic Cage Built from Macrocycles. Angewandte Chemie International Edition 2022, 61 (32) https://doi.org/10.1002/anie.202202450
    39. Jiahao Ren, Wenjiang Zeng, Yanling Chen, Xiaolong Fu, Qingyuan Yang. In silico screening and experimental study of anion-pillared metal-organic frameworks for hydrogen isotope separation. Separation and Purification Technology 2022, 295 , 121286. https://doi.org/10.1016/j.seppur.2022.121286
    40. Jingsong Xu, Rui Li, Xiayan Yan, Qingkai Zhao, Rongguang Zeng, Jingwen Ba, Qifa Pan, Xin Xiang, Daqiao Meng. Platinum single atom catalysts for hydrogen isotope separation during hydrogen evolution reaction. Nano Research 2022, 15 (5) , 3952-3958. https://doi.org/10.1007/s12274-022-4075-2
    41. Athira Ravi, Rajendar Nasani, Samar K. Das. Cobalt Formate, a Functional MOF: Electrocatalytic Water Oxidation. Journal of Molecular and Engineering Materials 2022, 10 (01n02) https://doi.org/10.1142/S2251237322400020
    42. 晓雪 吴. Research Progress of MOFs-Derived Porous Materials. Advances in Material Chemistry 2022, 10 (03) , 53-60. https://doi.org/10.12677/AMC.2022.103008
    43. Ryan A. Klein, Sarah Shulda, Philip A. Parilla, Pierre Le Magueres, Rachelle K. Richardson, William Morris, Craig M. Brown, C. Michael McGuirk. Structural resolution and mechanistic insight into hydrogen adsorption in flexible ZIF-7. Chemical Science 2021, 12 (47) , 15620-15631. https://doi.org/10.1039/D1SC04618G
    44. Raeesh Muhammad, Suhwan Kim, Jaewoo Park, Minji Jung, Myoung Eun Lee, Jaewoo Chung, Haenam Jang, Hyunchul Oh. Chemical affinity-assisted H 2 isotope separation using Ca-rich onion-peel-derived nanoporous carbon composite. Materials Chemistry Frontiers 2021, 5 (22) , 8018-8024. https://doi.org/10.1039/D1QM00894C
    45. Seulji Lee, Hyunchul Oh. Research Trend of Crystalline Porous Materials for Hydrogen Isotope Separation via Kinetic Quantum Sieving. Korean Journal of Materials Research 2021, 31 (8) , 465-470. https://doi.org/10.3740/MRSK.2021.31.8.465

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 22, 8232–8236
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.1c01694
    Published April 30, 2021
    Copyright © 2021 American Chemical Society

    Article Views

    5556

    Altmetric

    -

    Citations

    Learn about these metrics

    Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.

    Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.

    The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.