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

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Abstract
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. The alternative text for this image may have been generated using AI.
Funding Information
  • Core Research for Evolutional Science and Technology (JPMJCR24S6)
  • Core Research for Evolutional Science and Technology (JPMJCR24S6)
  • Japan Science and Technology Agency (JPMJFR203F)
  • Japan Science and Technology Agency (JPMJMI23G2)
  • Japan Society for the Promotion of Science (JP25H01999)
  • Japan Society for the Promotion of Science (JP24K01494)
  • Japan Society for the Promotion of Science (JP23H03937)
  • Japan Society for the Promotion of Science (JP25H01644)
  • Japan Society for the Promotion of Science (JP23KJ1388)
  • Japan Society for the Promotion of Science (JP23H02061)
  • Japan Society for the Promotion of Science (JP23K18001)
  • Japan Society for the Promotion of Science (JP22H05145)
  • Japan Society for the Promotion of Science (JP20H05838)
  • Japan Society for the Promotion of Science (JP25H01674)
  • Japan Society for the Promotion of Science (JP24K01528)
  • Japan Society for the Promotion of Science (JP20H00398)
  • Asahi Glass Foundation
  • Japan Agency for Medical Research and Development (JP25ama121006)
  • Nippon Sheet Glass Foundation for Materials Science and Engineering
  • Izumi Science and Technology Foundation

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