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<p>Photocatalytic overall water splitting holds great promise for sustainable hydrogen production. For overall water splitting performed by one-step excitation, both the hydrogen evolution and oxygen evolution reactions are hindered kinetically; hence, it is necessary to employ site-selective modification of photocatalysts with hydrogen-evolving and oxygen-evolving cocatalysts. However, critical challenges remain, including the need for cumbersome, multi-step photodeposition processes and durable blocking layers to inhibit the reverse reactions. Here we find a conductive, two-dimensional metal–organic framework to serve as a simple, multifunctional cocatalyst. We loaded this framework on SrTiO<sub>3</sub>:Al, an overall water-splitting photocatalyst, using a one-step self-assembly method. The framework cocatalyst promoted steady photocatalysis with an apparent quantum efficiency of 31.5% at 350 nm, free from the reverse reaction even without blocking layers. We proposed the operational principles for the cocatalyst activity using spectroscopic, electrochemical and theoretical analyses. This two-dimensional metal–organic framework offers an all-in-one approach for designing efficient and practical one-step excitation overall water-splitting systems.</p><p></p>

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Two-dimensional metal–organic frameworks offer all-in-one cocatalysts for photocatalytic overall water splitting

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月23日

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  • Jingyan Guan,
  • Hajime Suzuki,
  • Kazuhide Kamiya,
  • Takashi Harada,
  • Rintaro Adachi,
  • Osamu Tomita,
  • Hirofumi Kurokawa,
  • Daisuke Unabara,
  • Koji Yonekura,
  • Naoya Fukui,
  • Hiroaki Maeda,
  • Kunihisa Sugimoto,
  • Yuichi Yamaguchi,
  • Akinori Saeki,
  • Akira Yamakata,
  • Akihiko Kudo,
  • Ryu Abe,
  • Ryota Sakamoto

摘要

Photocatalytic overall water splitting holds great promise for sustainable hydrogen production. For overall water splitting performed by one-step excitation, both the hydrogen evolution and oxygen evolution reactions are hindered kinetically; hence, it is necessary to employ site-selective modification of photocatalysts with hydrogen-evolving and oxygen-evolving cocatalysts. However, critical challenges remain, including the need for cumbersome, multi-step photodeposition processes and durable blocking layers to inhibit the reverse reactions. Here we find a conductive, two-dimensional metal–organic framework to serve as a simple, multifunctional cocatalyst. We loaded this framework on SrTiO3:Al, an overall water-splitting photocatalyst, using a one-step self-assembly method. The framework cocatalyst promoted steady photocatalysis with an apparent quantum efficiency of 31.5% at 350 nm, free from the reverse reaction even without blocking layers. We proposed the operational principles for the cocatalyst activity using spectroscopic, electrochemical and theoretical analyses. This two-dimensional metal–organic framework offers an all-in-one approach for designing efficient and practical one-step excitation overall water-splitting systems.