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All-Electrochemically Grown Sb2Se3/a-MoSx Photocathodes for Hydrogen Production: The Effect of the MoSx Layer on the Surface Recombination and Photocorrosion of Sb2Se3 Films

  • Magno B. Costa
    Magno B. Costa
    Federal University of São Carlos, Washington Luiz Road, km 235, São Carlos, São Paulo 13565-905, Brazil
  • Francisco W. S. Lucas
    Francisco W. S. Lucas
    Department of Chemical and Biological Engineering and Renewable and Sustainable Energy Institute, University of Colorado Boulder, Boulder, Colorado 80309, United States
  • Marina Medina
    Marina Medina
    Federal University of São Carlos, Washington Luiz Road, km 235, São Carlos, São Paulo 13565-905, Brazil
  • , and 
  • Lucia H. Mascaro*
    Lucia H. Mascaro
    Federal University of São Carlos, Washington Luiz Road, km 235, São Carlos, São Paulo 13565-905, Brazil
    *Email: [email protected]
Cite this: ACS Appl. Energy Mater. 2020, 3, 10, 9799–9808
Publication Date (Web):September 11, 2020
https://doi.org/10.1021/acsaem.0c01413
Copyright © 2020 American Chemical Society

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    Abstract

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    Sb2Se3 is considered a promising photocathode material for hydrogen production via solar water splitting. Nevertheless, losses caused by photocorrosion and slow charge transfer at the semiconductor/electrolyte interface require the presence of a cocatalyst to improve the kinetic factors. In this work, the activity of all-electrochemically grown Sb2Se3/amorphous-MoSx photocathodes was studied in function of the number of cocatalyst deposition cycles. MoSx, a noble-metal-free electrocatalyst, has shown high activity toward the hydrogen evolution reaction. It promoted an ∼70-time higher improvement in the photocurrent of the Sb2Se3-absorber. An antagonistic effect was observed as the number of cycles increased: thin MoSx layers promoted the maximum enhancement in photocurrent and the decrease in surface recombination, but the photocorrosion inhibition was compromised. In the counterpart, thick MoSx layers allowed the material to be less susceptible to photocorrosion, but the photocurrent was inhibited. Therefore, the relationship between cocatalyst thickness and photocurrent enhancement/inhibition, variation in surface recombination, and photocorrosion stability was evaluated.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsaem.0c01413.

    • Experimental Methods; cyclic voltammograms for MoSx electrodeposition; SEM micrographs; EDS quantification plots; X-ray diffractograms; tables and selenium XPS spectrum data; UV–vis Tauc plots; Mott–Schottky graphs; schematic representation of the band edge position; LSV under solar illumination with 1 s of on/off pulses; EIS equivalent circuit fitting parameters; cyclic voltammograms under constant illumination for accelerated photocorrosion experiments; tests of stability for the different films. (PDF)

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