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

Kazuki Shun, Kohsuke Mori (), Takumi Kidawara, Satoshi Ichikawa and Hiromi Yamashita
Additional contact information
Kazuki Shun: Suita
Kohsuke Mori: Suita
Takumi Kidawara: Suita
Satoshi Ichikawa: Osaka University
Hiromi Yamashita: Suita

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-50217-z

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