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Fabricating a [email protected]2 Plasmonic System To Elucidate Alkali-Induced Enhancement of Photocatalytic H2 Evolution: Surface Potential Shift or Methanol Oxidation Acceleration?

  • Ming Zhao
    Ming Zhao
    TJU-NIMS International Collaboration Laboratory, School of Materials Science and Engineering, Tianjin University, 92 Weijin Road, Nankai District, Tianjin 300072, People’s Republic of China
    Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, People’s Republic of China
    More by Ming Zhao
  • Hua Xu
    Hua Xu
    TJU-NIMS International Collaboration Laboratory, School of Materials Science and Engineering, Tianjin University, 92 Weijin Road, Nankai District, Tianjin 300072, People’s Republic of China
    Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, People’s Republic of China
    More by Hua Xu
  • Shuxin Ouyang*
    Shuxin Ouyang
    TJU-NIMS International Collaboration Laboratory, School of Materials Science and Engineering, Tianjin University, 92 Weijin Road, Nankai District, Tianjin 300072, People’s Republic of China
    Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, People’s Republic of China
    *E-mail for S.O.: [email protected]
  • Hua Tong
    Hua Tong
    School of Materials Science and Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, People’s Republic of China
    More by Hua Tong
  • Huayu Chen
    Huayu Chen
    TJU-NIMS International Collaboration Laboratory, School of Materials Science and Engineering, Tianjin University, 92 Weijin Road, Nankai District, Tianjin 300072, People’s Republic of China
    Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, People’s Republic of China
    More by Huayu Chen
  • Yunxiang Li
    Yunxiang Li
    Graduate School of Chemical Science and Engineering, Hokkaido University, Sapporo 060-0814, Japan
    Environmental Remediation Materials Unit, International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba 305-0047, Japan
    More by Yunxiang Li
  • Lizhu Song
    Lizhu Song
    TJU-NIMS International Collaboration Laboratory, School of Materials Science and Engineering, Tianjin University, 92 Weijin Road, Nankai District, Tianjin 300072, People’s Republic of China
    Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, People’s Republic of China
    More by Lizhu Song
  • , and 
  • Jinhua Ye
    Jinhua Ye
    TJU-NIMS International Collaboration Laboratory, School of Materials Science and Engineering, Tianjin University, 92 Weijin Road, Nankai District, Tianjin 300072, People’s Republic of China
    Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, People’s Republic of China
    Graduate School of Chemical Science and Engineering, Hokkaido University, Sapporo 060-0814, Japan
    Environmental Remediation Materials Unit, International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba 305-0047, Japan
    More by Jinhua Ye
Cite this: ACS Catal. 2018, 8, 5, 4266–4277
Publication Date (Web):April 4, 2018
https://doi.org/10.1021/acscatal.8b00317
Copyright © 2018 American Chemical Society
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Abstract

Enhancement in photocatalytic H2 evolution induced by an alkaline reaction environment has been experimentally recognized, but there is not yet a consensus regarding the promotion mechanism (surface potential shift (SPS) or methanol oxidation (MO)). Herein, we construct a [email protected]2 plasmonic system, since this architecture can easily separate the proton reduction process (only related to SPS) and the electron donor oxidation process (only related to MO) in physical space. The H2 evolution rate over the [email protected]2 system in a strongly basic environment is exponentially greater (by approximately 2 orders of magnitude) than that of the same reaction in a neutral environment. To explore which of these two processes is the dominant factor for the enhancement of the H2 evolution, two investigation schemes are proposed. For [email protected] (ST01, a commercial anatase TiO2), the decisive role of the SPS on the enhancement of H2 evolution is semiquantitatively deduced from the open-circuit potential (OCP) test (exceeds 80% at pH <13.5 and more than 50% at pH ≥13.5) and is further confirmed by electrochemical impedance spectroscopy (EIS) and photoresponse current tests. For [email protected]100 and [email protected]101 (T100 and T101, facet-controlled anatase TiO2), the irregular fluctuation of the ratio of H2 evolution rates (rH2([email protected]100)/rH2([email protected]101)) suggests a secondary role of MO. This study clarifies the mechanism of the alkali-induced enhancement of H2 evolution and provides a perspective for the modulation of reaction environments.

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