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Angewandte Chemie. international edition v.57 no.29, 2018년, pp.9073 - 9077   SCI SCIE
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A Cocatalyst that Stabilizes a Hydride Intermediate during Photocatalytic Hydrogen Evolution over a Rhodium‐Doped TiO2 Nanosheet

Ida, Shintaro (Department of Applied Chemistry and Biochemistry, Kumamoto University, 2-39-1 Kurokami, Chuo, Kumamoto, 860-8555, Japan ) ; Sato, Kenta (Department of Applied Chemistry, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka, 819-0395, Japan ) ; Nagata, Tetsuya (Department of Applied Chemistry and Biochemistry, Kumamoto University, 2-39-1 Kurokami, Chuo, Kumamoto, 860-8555, Japan ) ; Hagiwara, Hidehisa (Department of Applied Chemistry, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka, 819-0395, Japan ) ; Watanabe, Motonori (International Institute for Carbon Neutral Energy Research, Kyushu University, Motooka 744, Nishi-ku, Fukuoka, 819-0395, Japan ) ; Kim, Namhoon (Department of Mechanical Science and Engineering, University of Illinois at, Urbana-Champaign, IL, USA ) ; Shiota, Yoshihito (Institute for Materials Chemistry and Engineering, Kyushu University, Motooka, Nishi-ku, ) ; Koinuma, Michio ; Takenaka, Sakae ; Sakai, Takaaki ; Ertekin, Elif ; Ishihara, Tatsumi ;
  • 초록  

    Abstract The hydrogen evolution reaction using semiconductor photocatalysts has been significantly improved by cocatalyst loading. However, there are still many speculations regarding the actual role of the cocatalyst. Now a photocatalytic hydrogen evolution reaction pathway is reported on a cocatalyst site using TiO 2 nanosheets doped with Rh at Ti sites as one‐atom cocatalysts. A hydride species adsorbed on the one‐atom Rh dopant cocatalyst site was confirmed experimentally as the intermediate state for hydrogen evolution, which was consistent with the results of density functional theory (DFT) calculations. In this system, the role of the cocatalyst in photocatalytic hydrogen evolution is related to the withdrawal of photo‐excited electrons and stabilization of the hydride intermediate species; the presence of oxygen vacancies induced by Rh facilitate the withdrawal of electrons and stabilization of the hydride.


  • 주제어

    cocatalysts .   hydrogen evolution .   nanosheets .   photocatalysis .   water splitting.  

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