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Title: Low-Cost, Efficient, and Durable H2 Production by Photoelectrochemical Water Splitting with CuGa3Se5 Photocathodes

Abstract

Photoelectrochemical (PEC) water-splitting is an elegant method of converting sunlight and water into H2 fuel. To be commercially advantageous, PEC devices must become cheaper, more efficient and much more durable. This work examines low-cost polycrystalline chalcopyrite films, which are successful as photovoltaic absorbers, for application as PEC absorbers. In particular, Cu-Ga-Se films with wide band gaps can be employed as top cell photocathodes in tandem devices as a realistic route to high efficiencies. In this report, we demonstrate that decreasing Cu/Ga composition from 0.66 to 0.31 in Cu-Ga-Se films increased the band gap from 1.67 to 1.86 eV and decreased saturated photocurrent density from 18 to 8 mA/cm2 as measured by chopped-light current-voltage (CLIV) measurements in 0.5 M sulfuric acid electrolyte. Buffer and catalyst surface treatments were not applied to the Cu-Ga-Se films, and they exhibited promising stability, evidenced by unchanged CLIV after 9 months of storage in air. Finally, films with Cu/Ga = 0.36 (approximately stoichiometric CuGa3Se5) and 1.86 eV band gaps had exceptional durability, and continuously split water for 17 days (~12 mA/cm2 at -1 V vs. RHE). This is equivalent to ~17200 C/cm2, which is a world record for any polycrystalline PEC absorber. These results indicate thatmore » CuGa3Se5 films are prime candidates for cheaply achieving efficient and durable PEC water splitting.« less

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [2]; ORCiD logo [1];  [2]
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  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Univ. of Hawaii, Honolulu, HI (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Hawaii, Honolulu, HI (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1456867
Alternate Identifier(s):
OSTI ID: 1570462
Report Number(s):
NREL/JA-5K00-71606
Journal ID: ISSN 1944-8244
Grant/Contract Number:  
AC36-08GO28308; EE0006670
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 23; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; chalcopyrite; hydrogen; photoelectrochemical; polycrystalline; water splitting

Citation Formats

Muzzillo, Christopher P., Klein, W. Ellis, Li, Zhen, DeAngelis, Alexander Daniel, Horsley, Kimberly, Zhu, Kai, and Gaillard, Nicolas. Low-Cost, Efficient, and Durable H2 Production by Photoelectrochemical Water Splitting with CuGa3Se5 Photocathodes. United States: N. p., 2018. Web. doi:10.1021/acsami.8b01447.
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Muzzillo, Christopher P., Klein, W. Ellis, Li, Zhen, DeAngelis, Alexander Daniel, Horsley, Kimberly, Zhu, Kai, & Gaillard, Nicolas. Low-Cost, Efficient, and Durable H2 Production by Photoelectrochemical Water Splitting with CuGa3Se5 Photocathodes. United States. https://doi.org/10.1021/acsami.8b01447
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Muzzillo, Christopher P., Klein, W. Ellis, Li, Zhen, DeAngelis, Alexander Daniel, Horsley, Kimberly, Zhu, Kai, and Gaillard, Nicolas. Wed . "Low-Cost, Efficient, and Durable H2 Production by Photoelectrochemical Water Splitting with CuGa3Se5 Photocathodes". United States. https://doi.org/10.1021/acsami.8b01447. https://www.osti.gov/servlets/purl/1456867.
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@article{osti_1456867,
title = {Low-Cost, Efficient, and Durable H2 Production by Photoelectrochemical Water Splitting with CuGa3Se5 Photocathodes},
author = {Muzzillo, Christopher P. and Klein, W. Ellis and Li, Zhen and DeAngelis, Alexander Daniel and Horsley, Kimberly and Zhu, Kai and Gaillard, Nicolas},
abstractNote = {Photoelectrochemical (PEC) water-splitting is an elegant method of converting sunlight and water into H2 fuel. To be commercially advantageous, PEC devices must become cheaper, more efficient and much more durable. This work examines low-cost polycrystalline chalcopyrite films, which are successful as photovoltaic absorbers, for application as PEC absorbers. In particular, Cu-Ga-Se films with wide band gaps can be employed as top cell photocathodes in tandem devices as a realistic route to high efficiencies. In this report, we demonstrate that decreasing Cu/Ga composition from 0.66 to 0.31 in Cu-Ga-Se films increased the band gap from 1.67 to 1.86 eV and decreased saturated photocurrent density from 18 to 8 mA/cm2 as measured by chopped-light current-voltage (CLIV) measurements in 0.5 M sulfuric acid electrolyte. Buffer and catalyst surface treatments were not applied to the Cu-Ga-Se films, and they exhibited promising stability, evidenced by unchanged CLIV after 9 months of storage in air. Finally, films with Cu/Ga = 0.36 (approximately stoichiometric CuGa3Se5) and 1.86 eV band gaps had exceptional durability, and continuously split water for 17 days (~12 mA/cm2 at -1 V vs. RHE). This is equivalent to ~17200 C/cm2, which is a world record for any polycrystalline PEC absorber. These results indicate that CuGa3Se5 films are prime candidates for cheaply achieving efficient and durable PEC water splitting.},
doi = {10.1021/acsami.8b01447},
journal = {ACS Applied Materials and Interfaces},
number = 23,
volume = 10,
place = {United States},
year = {2018},
month = {5}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acsami.8b01447
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Cited by: 25 works
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Figures / Tables:

Figure 1 Figure 1: XRD data for Cu-Ga-Se films with Cu/Ga compositions of 0.66 (top black), 0.52 (middle red), and 0.36 (bottom blue). Standard diffraction pattern peak positions for CuGaSe2 (green triangles) and CuGa3Se5 (purple circles) are included for reference.
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    Works referencing / citing this record:

    Efficiency and stability of narrow-gap semiconductor-based photoelectrodes
    journal, January 2019

    • Zheng, Jianyun; Zhou, Huaijuan; Zou, Yuqin
    • Energy & Environmental Science, Vol. 12, Issue 8
    • DOI: 10.1039/c9ee00524b

    Recent Advances and Emerging Trends in Photo-Electrochemical Solar Energy Conversion
    journal, November 2018

    Metal selenide photocatalysts for visible-light-driven Z -scheme pure water splitting
    journal, January 2019

    • Chen, Shanshan; Ma, Guijun; Wang, Qian
    • Journal of Materials Chemistry A, Vol. 7, Issue 13
    • DOI: 10.1039/c9ta00768g
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      Figures / Tables found in this record:

      Figure 1 (p. 8)figure
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      Figure 5 (p. 14)figure
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      Figure 9 (p. 17)figure
      Figure S1 (p. 27)figure
      Table S1 (p. 27)table
      Figure S2 (p. 28)figure
      Figure S3 (p. 28)figure
      Figure S4 (p. 29)figure
      Table S2 (p. 29)table
      Figure S5 (p. 30)figure
      Figure S6 (p. 31)figure
      Table S3 (p. 31)table
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