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Efficient Hydrogen Isotope Separation by Tunneling Effect Using Graphene-Based Heterogeneous Electrocatalysts in Electrochemical Hydrogen Isotope Pumping

  • 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
  • , and 
  • 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
Cite this: ACS Nano 2022, 16, 9, 14362–14369
Publication Date (Web):September 1, 2022
https://doi.org/10.1021/acsnano.2c04655
Copyright © 2022 American Chemical Society

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    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.

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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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    Cited By

    This article is cited by 2 publications.

    1. Teppei Watanabe, Yurina Sekine, Tomoko Ikeda-Fukazawa. Fractionation of Hydrogen Isotopes in a Hydrogel during Dehydration. Macromolecules 2023, 56 (16) , 6217-6221. https://doi.org/10.1021/acs.macromol.3c00991
    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

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