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Efficient Hydrogen Isotope Separation by Tunneling Effect Using Graphene-Based Heterogeneous Electrocatalysts in Electrochemical Hydrogen Isotope Pumping
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    Efficient Hydrogen Isotope Separation by Tunneling Effect Using Graphene-Based Heterogeneous Electrocatalysts in Electrochemical Hydrogen Isotope Pumping
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    • Satoshi Yasuda*
      Satoshi Yasuda
      Research Group for Surface and Interface Science, Advanced Science Research Center, Japan Atomic Energy Agency, 2-4 Shirakata, Tokai, Ibaraki 319-1195, Japan
      *Email: [email protected]
    • Hisayoshi Matsushima
      Hisayoshi Matsushima
      Faculty of Engineering, Hokkaido University, North 13, West 8, Kita-ku, Sapporo, Hokkaido 060-8628, Japan
    • Kenji Harada
      Kenji Harada
      Faculty of Engineering, Hokkaido University, North 13, West 8, Kita-ku, Sapporo, Hokkaido 060-8628, Japan
      More by Kenji Harada
    • Risako Tanii
      Risako Tanii
      Faculty of Engineering, Hokkaido University, North 13, West 8, Kita-ku, Sapporo, Hokkaido 060-8628, Japan
      More by Risako Tanii
    • Tomo-o Terasawa
      Tomo-o Terasawa
      Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan
      Research Group for Surface and Interface Science, Advanced Science Research Center, Japan Atomic Energy Agency, 2-4 Shirakata, Tokai, Ibaraki 319-1195, Japan
    • Masahiro Yano
      Masahiro Yano
      Research Group for Surface and Interface Science, Advanced Science Research Center, Japan Atomic Energy Agency, 2-4 Shirakata, Tokai, Ibaraki 319-1195, Japan
    • Hidehito Asaoka
      Hidehito Asaoka
      Research Group for Surface and Interface Science, Advanced Science Research Center, Japan Atomic Energy Agency, 2-4 Shirakata, Tokai, Ibaraki 319-1195, Japan
    • Jessiel Siaron Gueriba
      Jessiel Siaron Gueriba
      Department of Applied Physics, Osaka University, Suita, Osaka 565-0871, Japan
    • Wilson Agerico Diño
      Wilson Agerico Diño
      Department of Applied Physics, Osaka University, Suita, Osaka 565-0871, Japan
      Center for Atomic and Molecular Technologies, Osaka University, Suita, Osaka 565-0871, Japan
    • Katsuyuki Fukutani
      Katsuyuki Fukutani
      Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan
      Research Group for Surface and Interface Science, Advanced Science Research Center, Japan Atomic Energy Agency, 2-4 Shirakata, Tokai, Ibaraki 319-1195, Japan
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    ACS Nano

    Cite this: ACS Nano 2022, 16, 9, 14362–14369
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    https://doi.org/10.1021/acsnano.2c04655
    Published September 1, 2022
    Copyright © 2022 American Chemical Society

    Abstract

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    The fabrication of a hydrogen isotope enrichment system is essential for the development of industrial, medical, life science, and nuclear fusion fields, and therefore, efficient enrichment techniques with a high separation factor and economic feasibility are still being explored. Herein, we report a hydrogen/deuterium (H/D) separation ability with polymer electrolyte membrane electrochemical hydrogen pumping (PEM-ECHP) using a heterogeneous electrode consisting of palladium and graphene layers (PdGr). By mass spectroscopic analysis, we demonstrate significant bias voltage dependence of the H/D separation factor with a maximum of ∼25 at 0.15 V and room temperature, which is superior to those of conventional separation methods. Theoretical analysis demonstrated that the observed high H/D factor stems from tunneling of hydrogen isotopes through atomically thick graphene during the electrochemical reaction and that the bias dependence of H/D results from a transition from the quantum tunneling regime to the classical overbarrier regime for hydrogen isotopes transfer through the graphene. These findings will help us understand the origin of the isotope separation ability of graphene discussed so far and contribute to developing an economical hydrogen isotope enrichment system using two-dimensional materials.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.2c04655.

    • Chemicals, fabrication of membrane electrode assemblies, optical microscope images of membranes, Raman and AFM analyses, hydrogen isotope separation analysis method and determination of H/D separation factor, time evolution of ion current components for different MEAs, calculated molar rates of hydrogen isotope gases generated in cathode outlet, bias dependence of the molar rates for different bias voltages of PdGr-MEA, reproducibility of bias dependence of hydrogen isotope ability for PdGr-MEA, and potential energy calculation of an H atom and a proton (PDF)

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    This article is cited by 24 publications.

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    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. Rou‐Ming Wen, Hao Ye, Ming‐Bang Wu, Qiao Luo, Qi‐Hui Ye, Zhang‐Ting Hu, Yucong Yu, Juming Yao, Chao Zhang. Designing Confined Thermal‐Recognized Hydrogen Bonding Nanochannels for Effective and Energy‐Efficient Water Isotopologue Sieving. Advanced Functional Materials 2025, 31 https://doi.org/10.1002/adfm.202423564
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    10. J. Tong, Y. Fu, D. Domaretskiy, F. Della Pia, P. Dagar, L. Powell, D. Bahamon, S. Huang, B. Xin, R. N. Costa Filho, L. F. Vega, I. V. Grigorieva, F. M. Peeters, A. Michaelides, M. Lozada-Hidalgo. Control of proton transport and hydrogenation in double-gated graphene. Nature 2024, 630 (8017) , 619-624. https://doi.org/10.1038/s41586-024-07435-8
    11. Siti Munirah Mhd Yusof, Serene Sow Mun Lock, Nur Najwa Abdul Talib, Liew Chin Seng. A Mini Review on Liquid Phase Catalytic Exchange for Hydrogen Isotope Separation: Current Status and Future Potential. Sustainability 2024, 16 (11) , 4796. https://doi.org/10.3390/su16114796
    12. Kazuki Shun, Satoshi Matsukawa, Kohsuke Mori, Hiromi Yamashita. Specific Hydrogen Spillover Pathways Generated on Graphene Oxide Enabling the Formation of Non‐Equilibrium Alloy Nanoparticles. Small 2024, 20 (19) https://doi.org/10.1002/smll.202306765
    13. J.J. Gibson, P. Eby, A. Jaggi. Natural isotope fingerprinting of produced hydrogen and its potential applications to the hydrogen economy. International Journal of Hydrogen Energy 2024, 66 , 468-478. https://doi.org/10.1016/j.ijhydene.2024.04.077
    14. 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
    15. Satoshi YASUDA. Hydrogen Isotope Separation Technique by Quantum Tunneling Effect Used Graphene. Journal of The Surface Finishing Society of Japan 2024, 75 (3) , 131-135. https://doi.org/10.4139/sfj.75.131
    16. 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
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    19. Koichiro Furusawa, Toranosuke Nago, Mikito Ueda, Hisayoshi Matsushima. Application of membrane electrode assembly for water hydrogen isotope exchange. International Journal of Hydrogen Energy 2024, 50 , 629-634. https://doi.org/10.1016/j.ijhydene.2023.09.247
    20. 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
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    23. Jiahui Zhao, Changti Pan, Yue Zhang, Xiyu Li, Guozhen Zhang, Li Yang. Proton penetration mechanism and selective hydrogen isotope separation through two-dimensional biphenylene. RSC Advances 2023, 13 (39) , 27590-27598. https://doi.org/10.1039/D3RA02993J
    24. Pavan Chaturvedi, Nicole K. Moehring, Thomas Knight, Rahul Shah, Ivan Vlassiouk, Piran R. Kidambi. The parameter space for scalable integration of atomically thin graphene with Nafion for proton exchange membrane (PEM) applications. Materials Advances 2023, 4 (16) , 3473-3481. https://doi.org/10.1039/D3MA00180F

    ACS Nano

    Cite this: ACS Nano 2022, 16, 9, 14362–14369
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.2c04655
    Published September 1, 2022
    Copyright © 2022 American Chemical Society

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