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Cobalt-Doped Black TiO2 Nanotube Array as a Stable Anode for Oxygen Evolution and Electrochemical Wastewater Treatment

  • Yang Yang
    Yang Yang
    Division of Engineering and Applied Science, Linde-Robinson Laboratory, California Institute of Technology, Pasadena, California 91125, United States
    More by Yang Yang
  • Li Cheng Kao
    Li Cheng Kao
    Department of Geosciences, National Taiwan University, P.O. Box 13-318, Taipei 106, Taiwan
    More by Li Cheng Kao
  • Yuanyue Liu
    Yuanyue Liu
    Department of Mechanical Engineering and Texas Materials Institute, University of Texas at Austin, Austin, Texas 78712, United States
    More by Yuanyue Liu
  • Ke Sun
    Ke Sun
    Divisions of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States
    More by Ke Sun
  • Hongtao Yu
    Hongtao Yu
    School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, People’s Republic of China
    More by Hongtao Yu
  • Jinghua Guo
    Jinghua Guo
    Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    Department of Chemistry and Biochemistry, University of California, Santa Cruz, California 95064, United States
    More by Jinghua Guo
  • Sofia Ya Hsuan Liou
    Sofia Ya Hsuan Liou
    Department of Geosciences, National Taiwan University, P.O. Box 13-318, Taipei 106, Taiwan
  • , and 
  • Michael R. Hoffmann*
    Michael R. Hoffmann
    Division of Engineering and Applied Science, Linde-Robinson Laboratory, California Institute of Technology, Pasadena, California 91125, United States
    *E-mail for M.R.H.: [email protected]
Cite this: ACS Catal. 2018, 8, 5, 4278–4287
Publication Date (Web):April 10, 2018
https://doi.org/10.1021/acscatal.7b04340
Copyright © 2018 American Chemical Society
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Abstract

TiO2 has long been recognized as a stable and reusable photocatalyst for water splitting and pollution control. However, it is an inefficient anode material in the absence of photoactivation due to its low electron conductivity. To overcome this limitation, a series of conductive TiO2 nanotube array electrodes have been developed. Even though nanotube arrays are effective for electrochemical oxidation initially, deactivation is often observed within a few hours. To overcome the problem of deactivation, we have synthesized cobalt-doped Black-TiO2 nanotube array (Co-Black NTA) electrodes that are stable for more than 200 h of continuous operation in a NaClO4 electrolyte at 10 mA cm–2. Using X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, electron paramagnetic resonance spectroscopy, and DFT simulations, we are able to show that bulk oxygen vacancies (Ov) are the primary source of the enhanced conductivity of Co-Black. Cobalt doping both creates and stabilizes surficial oxygen vacancies, Ov, and thus prevents surface passivation. The Co-Black electrodes outperform dimensionally stable IrO2 anodes (DSA) in the electrolytic oxidation of organic-rich wastewater. Increasing the loading of Co leads to the formation of a CoOx film on top of Co-Black electrode. The CoOx/Co-Black composite electrode was found to have a lower OER overpotential (352 mV) in comparison to a DSA IrO2 (434 mV) electrode and a stability that is greater than 200 h in a 1.0 M KOH electrolyte at a current density of 10 mA cm–2.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acscatal.7b04340.

  • Details of DFT calculations and additional results of XRD, XPS, SEM-EDS, TEM, two-point solid state measurements, EIS, stability tests, and activity evaluation (PDF)

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