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Improved Photoelectrochemical Hydrogen Gas Generation on Sb2S3 Films Modified with an Earth-Abundant MoSx Co-Catalyst

  • Moisés A. de Araújo
    Moisés A. de Araújo
    Departamento de Química, Universidade Federal de São Carlos, Rodovia Washington Luiz, km 235, São Carlos, São Paulo 13565-905, Brazil
  • Magno B. Costa
    Magno B. Costa
    Departamento de Química, Universidade Federal de São Carlos, Rodovia Washington Luiz, km 235, São Carlos, São Paulo 13565-905, Brazil
  • , and 
  • Lucia H. Mascaro*
    Lucia H. Mascaro
    Departamento de Química, Universidade Federal de São Carlos, Rodovia Washington Luiz, km 235, São Carlos, São Paulo 13565-905, Brazil
    *Email: [email protected]
Cite this: ACS Appl. Energy Mater. 2022, 5, 1, 1010–1022
Publication Date (Web):January 13, 2022
https://doi.org/10.1021/acsaem.1c03374
Copyright © 2022 American Chemical Society

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    Abstract

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    Antimony(III) sulfide (Sb2S3) has recently emerged as an outstanding potential photoelectrode due to its superlative optoelectronic properties for light-driven water splitting application. However, the occurrence of the recombination process in this material is regarded as one of the main limiting factors to date. Herein, we greatly suppressed the occurrence of recombination and improved carrier transfer via photoelectrodepositing an earth-abundant MoSx co-catalyst over Sb2S3 films. The Sb2S3/MoSx films displayed a remarkable 2-fold increase of their photoresponse for H2 generation and also resulted in shifting the onset potential approximately 100 mV to less negative values. Based on an in-depth analysis of the transients’ photocurrent density, the enhanced photoresponse was assigned to a smaller probability of the electron–hole recombination process, as noted from the substantial reduction of the accumulated negative charge density values at the surface of the Sb2S3 films. The minimization of carriers recombination was also verified from the decrease of the charge transfer resistance values by approximately 2-fold for the Sb2S2/MoSx films. Additionally, Sb2S3/MoSx featured an increase of the space charge thickness, which suggests an improvement of carrier separation or a minimized recombination process due to the enlarged gradient of the (quasi-)Fermi level in the space charge region of the Sb2S3 films.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsaem.1c03374.

    • Cyclic voltammograms for MoSx photoelectrodeposition; linear sweep voltammograms in the dark and under illumination for UT-Sb2S3/MoSx and PT-Sb2S3/MoSx films; high-resolution XPS spectra for UT-Sb2S3/MoSx film; particle size distribution histograms for PT-Sb2S3 and PT-Sb2S3/(1, 10, or 20 min)-MoSx films; EDS spectra and EDS quantification plots for PT-Sb2S3 and PT-Sb2S3/(1, 10, or 20 min)-MoSx films; atomic percentage of Sb and S; binding energy assignment; and percentage error values for each circuit element to fit the complex-plane impedance diagrams (PDF)

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    Cited By

    This article is cited by 2 publications.

    1. Zaichun Sun, Shaoyong Qin, Daichi Oka, Huijuan Zhang, Tomoteru Fukumura, Yuji Matsumoto, Bingchu Mei. Near-Ultraviolet Light-Driven Photocathodic Activity for (001)-Oriented BiOCl Thin Films Synthesized by Mist Chemical Vapor Deposition. Inorganic Chemistry 2023, 62 (23) , 8914-8922. https://doi.org/10.1021/acs.inorgchem.3c00466
    2. Huijuan Zhang, Wenyan Luo, Zaichun Sun, Chunya Li. Highly Sensitive and Stable Visible-Light Self-Power Photodetectors Based on Solution-Processed Bi4O5I2. Crystal Growth & Design 2023, 23 (4) , 2852-2859. https://doi.org/10.1021/acs.cgd.3c00036

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