Article Effects of Metal-Cation Doping on Photocatalytic H2 Evolution Activity of Layered Perovskite Oxynitride K2LaTa2O6N

Hideya Tsuchikado ; Shuji Anabuki ; Ovidiu Cretu SAMURAI ORCID ; Yuki Kinoshita ORCID ; Masashi Hattori ORCID ; Yuta Shiroma ; Dongxiao Fan ; Megumi Okazaki ORCID ; Takuto Soma ORCID ; Fumitaka Ishiwari ORCID ; Shunsuke Nozawa ORCID ; Toshiyuki Yokoi ORCID ; Michikazu Hara ORCID ; Koji Kimoto SAMURAI ORCID ; Akira Yamakata ORCID ; Akinori Saeki ORCID ; Kazuhiko Maeda ORCID

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Hideya Tsuchikado, Shuji Anabuki, Ovidiu Cretu, Yuki Kinoshita, Masashi Hattori, Yuta Shiroma, Dongxiao Fan, Megumi Okazaki, Takuto Soma, Fumitaka Ishiwari, Shunsuke Nozawa, Toshiyuki Yokoi, Michikazu Hara, Koji Kimoto, Akira Yamakata, Akinori Saeki, Kazuhiko Maeda. Effects of Metal-Cation Doping on Photocatalytic H2 Evolution Activity of Layered Perovskite Oxynitride K2LaTa2O6N. ACS Applied Energy Materials. 2025, 8 (6), 3541-3552. https://doi.org/10.1021/acsaem.4c03131

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(abstract)

Aliovalent cation doping into a heterogeneous photocatalyst affects several of its physicochemical properties, including its morphological characteristics, optical absorption behavior, and charge carrier dynamics, causing a drastic change in its photocatalytic activity. In the present work, we investigated the effects of aliovalent cation doping on the visible-light H2-evolution photocatalytic activity of the Ruddlesden–Popper layered perovskite oxynitride K2LaTa2O6N. The photocatalytic activity toward H2 evolution from an aqueous NaI solution was found to be enhanced by an increase in the specific surface area of the K2LaTa2O6N photocatalyst, which could be realized upon doping with lower-valence cations (e.g., Mg2+, Al3+, and Ga3+). Among the dopants examined at 1 mol % doping, Ga resulted in the highest activity. The activity of the Ga-doped specimen was further improved with increasing Ga concentration, where the maximal activity was obtained at 10 mol %, corresponding to an apparent quantum yield of 2.7 ± 0.4% at 420 nm from aqueous methanol. This number is the highest reported for a layered oxynitride photocatalyst. In the Ga-doped K2LaTa2O6N, a trade-off was observed between the Ga concentration and the photocatalytic activity. Although doping with Ga reduced the particle size of K2LaTa2O6N and suppressed undesirable charge recombination, it led to an enlarged bandgap, unsuitable for visible-light absorption.

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Keyword: artificial photosynthesis, heterogeneous photocatalysis, mixed-anion compounds, topochemical reaction, visible light

Date published: 2025-03-24

Publisher: American Chemical Society (ACS)

Journal:

  • ACS Applied Energy Materials (ISSN: 25740962) vol. 8 issue. 6 p. 3541-3552

Funding:

  • Core Research for Evolutional Science and Technology JPMJCR20R2
  • Japan Society for the Promotion of Science JP20H05836
  • Japan Society for the Promotion of Science JP20H05838
  • Japan Society for the Promotion of Science JP22H05142
  • Japan Society for the Promotion of Science JP22H05148
  • Japan Society for the Promotion of Science JP23H04626
  • Japan Society for the Promotion of Science JPJSCCA20200004
  • Support for Pioneering Research Initiated by the Next Generation JPMJSP2106

Manuscript type: Publisher's version (Version of record)

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First published URL: https://doi.org/10.1021/acsaem.4c03131

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Updated at: 2025-05-09 16:30:33 +0900

Published on MDR: 2025-05-09 16:21:39 +0900

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