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Ultrathin Cobalt Oxide Interlayer Facilitated Hole Storage for Sustained Water Oxidation over Composited Tantalum Nitride Photoanodes

  • Pengpeng Wang
    Pengpeng Wang
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China
    University of Chinese Academy of Sciences, Beijing 100049, China
  • Ping Fu
    Ping Fu
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China
    More by Ping Fu
  • Jiangping Ma
    Jiangping Ma
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China
    College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China
    More by Jiangping Ma
  • Yuying Gao
    Yuying Gao
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China
    More by Yuying Gao
  • Zheng Li
    Zheng Li
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China
    More by Zheng Li
  • Hong Wang
    Hong Wang
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China
    University of Chinese Academy of Sciences, Beijing 100049, China
    More by Hong Wang
  • Fengtao Fan
    Fengtao Fan
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China
    More by Fengtao Fan
  • Jingying Shi*
    Jingying Shi
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China
    *Email: [email protected]
    More by Jingying Shi
  • , and 
  • Can Li*
    Can Li
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China
    *Email: [email protected]
    More by Can Li
Cite this: ACS Catal. 2021, 11, 20, 12736–12744
Publication Date (Web):October 5, 2021
https://doi.org/10.1021/acscatal.1c03298
Copyright © 2021 American Chemical Society
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Abstract

The hole-storage layer (HSL) strategy has been demonstrated as an efficient interfacial modification method to overcome the instability of tantalum nitride (Ta3N5) photoanodes and further boost high performance in photoelectrochemical (PEC) water oxidation reaction. Herein, we report that the CoOx/Ni(OH)x bilayer as a typical HSL could effectively extract and store photogenerated holes from Ta3N5, resulting in a decent photocurrent enhancement and stable water oxidation for at least 30 h. Most strikingly, the reversible formation of Co(IV) species inside the ultrathin CoOx layer during PEC water oxidation is found to regulate the hole-storage process, leading to facilitated photogenerated hole extraction capacity and suppressed charge recombination. Furthermore, upon the insertion of the CoOx/Ni(OH)x bilayer for the Ta3N5/CoPi photoanode, the photocurrent could be evidently increased, emphasizing the general applicability of the HSL strategy in promoting water oxidation reaction.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.1c03298.

  • Experimental methods; (photo)electrochemical performance evaluated data; IMPS analysis; oxygen evolution measurements; and physical characterizations such as SEM, HR-TEM, XRD, UV–visible, Raman spectra, XPS spectra, UPS spectra, and SKPM images (PDF)

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