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

Journal Article · Wed May 16 00:00:00 UTC 2018 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.8b01447 · OSTI ID:1456867

Muzzillo, Christopher P.  ^[1]; Klein, W. Ellis ^[1]; Li, Zhen ^[1]; DeAngelis, Alexander Daniel ^[2]; Horsley, Kimberly ^[2]; Zhu, Kai  ^[1]; Gaillard, Nicolas ^[2]

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1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
2. Univ. of Hawaii, Honolulu, HI (United States)

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.

• Research Organization: National Renewable Energy Laboratory (NREL), Golden, CO (United States); Univ. of Hawaii, Honolulu, HI (United States)
• Sponsoring Organization: USDOE Office of Energy Efficiency and Renewable Energy (EERE)
• Grant/Contract Number: AC36-08GO28308; EE0006670
• OSTI ID: 1456867
• Report Number(s): NREL/JA--5K00-71606
• Journal Information: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 23 Vol. 10; ISSN 1944-8244
• Publisher: American Chemical Society (ACS)Copyright Statement
• Country of Publication: United States
• Language: English