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Heteroatom doping enables hydrogen spillover via H+/e− diffusion pathways on a non-reducible metal oxide

Author

Listed:
  • Kazuki Shun

    (Suita)

  • Kohsuke Mori

    (Suita
    Suita)

  • Takumi Kidawara

    (Suita)

  • Satoshi Ichikawa

    (Osaka University)

  • Hiromi Yamashita

    (Suita
    Suita)

Abstract

Hydrogen spillover, the simultaneous diffusion of protons (H+) and electrons (e−) is considered to be applicable to ubiquitous technologies related to hydrogen but limited to over reducible metal oxides. The present work demonstrates that a non-reducible MgO with heteroatom Al dopants (Al–MgO) allows hydrogen spillover in the same way as reducible metal oxides. Furthermore, a H+ storage capacity of this material owing to hydrogen spillover is more than three times greater than those of various standard metal oxides based on H+ transport channels within its bulk region. Atomic hydrogen diffuses over the non-reducible Al–MgO produces active H+-e− pairs, as also occurs on reducible metal oxides, to enhance the catalytic performance of Ni during CO2 hydrogenation. The H+ and e− diffusion pathways generated by the heteroatom Al doping are disentangled based on systematic characterizations and calculations. This work provides a new strategy for designing functional materials intended to hydrogen spillover for diverse applications in a future hydrogen-based society.

Suggested Citation

  • Kazuki Shun & Kohsuke Mori & Takumi Kidawara & Satoshi Ichikawa & Hiromi Yamashita, 2024. "Heteroatom doping enables hydrogen spillover via H+/e− diffusion pathways on a non-reducible metal oxide," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50217-z
    DOI: 10.1038/s41467-024-50217-z
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    References listed on IDEAS

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    1. Waiz Karim & Clelia Spreafico & Armin Kleibert & Jens Gobrecht & Joost VandeVondele & Yasin Ekinci & Jeroen A. van Bokhoven, 2017. "Catalyst support effects on hydrogen spillover," Nature, Nature, vol. 541(7635), pages 68-71, January.
    2. Kohsuke Mori & Naoki Hashimoto & Naoto Kamiuchi & Hideto Yoshida & Hisayoshi Kobayashi & Hiromi Yamashita, 2021. "Hydrogen spillover-driven synthesis of high-entropy alloy nanoparticles as a robust catalyst for CO2 hydrogenation," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    3. Jiankang Zhang & Zhe Gao & Sen Wang & Guofu Wang & Xiaofeng Gao & Baiyan Zhang & Shuangfeng Xing & Shichao Zhao & Yong Qin, 2019. "Origin of synergistic effects in bicomponent cobalt oxide-platinum catalysts for selective hydrogenation reaction," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    4. Davis, Steven J & Lewis, Nathan S. & Shaner, Matthew & Aggarwal, Sonia & Arent, Doug & Azevedo, Inês & Benson, Sally & Bradley, Thomas & Brouwer, Jack & Chiang, Yet-Ming & Clack, Christopher T.M. & Co, 2018. "Net-Zero Emissions Energy Systems," Institute of Transportation Studies, Working Paper Series qt7qv6q35r, Institute of Transportation Studies, UC Davis.
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