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Title: Low-Cost, Efficient, and Durable H 2 Production by Photoelectrochemical Water Splitting with CuGa 3Se 5 Photocathodes

Photoelectrochemical (PEC) water splitting is an elegant method of converting sunlight and water into H 2 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/cm 2 as measured by chopped-light current-voltage (CLIV) measurements in a 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 CuGa 3Se 5) and 1.86 eV band gaps had exceptional durability and continuously split water for 17 days (~12 mA/cm 2 at -1 V vs RHE). This is equivalent to ~17 200 C/cm 2, which is a world recordmore » for any polycrystalline PEC absorber. These results indicate that CuGa 3Se 5 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]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Univ. of Hawaii, Honolulu, HI (United States)
Publication Date:
Report Number(s):
NREL/JA-5K00-71606
Journal ID: ISSN 1944-8244
Grant/Contract Number:
AC36-08GO28308
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)
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; chalcopyrite; hydrogen; photoelectrochemical; polycrystalline; water splitting
OSTI Identifier:
1456867

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., Web. doi:10.1021/acsami.8b01447.
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. doi:10.1021/acsami.8b01447.
Muzzillo, Christopher P., Klein, W. Ellis, Li, Zhen, DeAngelis, Alexander Daniel, Horsley, Kimberly, Zhu, Kai, and Gaillard, Nicolas. 2018. "Low-Cost, Efficient, and Durable H2 Production by Photoelectrochemical Water Splitting with CuGa3Se5 Photocathodes". United States. doi:10.1021/acsami.8b01447.
@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 a 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 ~17 200 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}
}