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Interfacial Electron Flow Control by Double Nano-architectures for Efficient Ru-Dye-Sensitized Hydrogen Evolution from Water

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Title: Interfacial Electron Flow Control by Double Nano-architectures for Efficient Ru-Dye-Sensitized Hydrogen Evolution from Water
Authors: Yoshimura, Nobutaka Browse this author
Kobayashi, Atsushi Browse this author →KAKEN DB
Kondo, Tomoki Browse this author
Abe, Ryu Browse this author →KAKEN DB
Yoshida, Masaki Browse this author →KAKEN DB
Kato, Masako Browse this author →KAKEN DB
Keywords: electron flow
hydrogen evolution
Issue Date: 27-Dec-2021
Publisher: American Chemical Society
Journal Title: ACS applied energy materials
Volume: 4
Issue: 12
Start Page: 14352
End Page: 14362
Publisher DOI: 10.1021/acsaem.1c03028
Abstract: Interfacial electron flow is crucial for an efficient two-step (Z-scheme) solar water-splitting reaction. Dye-sensitization of a wide-gap oxide semiconductor has attracted considerable attention for decades as a means of producing hydrogen from water; however, it suffers from back electron transfer reactions at solid-solid and solid-solution interfaces. Here, we demonstrate that a combination of two nano-architectures, Ru-dye double layering and Pt cocatalyst intercalation to layered niobate semiconductor, effectively suppresses the back electron transfers at interfaces, leading to the complete oxidation of the [Co(bpy)(3)]-type electron mediator (bpy = 2,2'-bipyridine) as a result of efficient photocatalytic hydrogen production. Our systematic study on the Ru-dye double layers revealed that the double layering of two different Ru dyes and surface modification with the Zr4+ cation not only suppress the back electron transfer from an electron-injected semiconductor to oxidized dye but also accelerate the electron injection from the mediator to the oxidized dye. In addition, the re-reduction of the oxidized Co(III) mediator at the Pt cocatalyst surface was effectively suppressed by intercalation of Pt to the layered niobate semiconductor. The present work clearly shows that double nano-architectures controlling the surfaces of the semiconductor and cocatalyst have great potential for photo-induced charge separation at the solid-solution interface and expands the possibilities of layered semiconductor materials toward Z-scheme water splitting.
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS applied energy materials, copyright c American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Type: article (author version)
Appears in Collections:理学院・理学研究院 (Graduate School of Science / Faculty of Science) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 小林 厚志

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