Abstract
Despite their excellent photophysical properties and record-high solar-to-hydrogen conversion efficiency, the high cost and limited stability of III–V compound semiconductors prohibit their practical application in solar-driven photoelectrochemical water splitting. Here we present a strategy for III–V photocatalysis that can circumvent these difficulties via printed assemblies of epitaxially grown compound semiconductors. A thin film stack of GaAs-based epitaxial materials is released from the growth wafer and printed onto a non-native transparent substrate to form an integrated photocatalytic electrode for solar hydrogen generation. The heterogeneously integrated electrode configuration together with specialized epitaxial design serve to decouple the material interfaces for illumination and electrocatalysis. Subsequently, this allows independent control and optimization of light absorption, carrier transport, charge transfer, and material stability. Using this approach, we construct a series-connected wireless tandem system of GaAs photoelectrodes and demonstrate 13.1% solar-to-hydrogen conversion efficiency of unassisted-mode water splitting.
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Acknowledgements
D.K., H.L., H.C., Y.X., B.G. and J.Y. gratefully acknowledge National Science Foundation (ECCS-1202522, ECCS-1509897), USC startup fund, and Hanwha Advanced Materials Non-tenured faculty award. T.G.D., J.L.Y. and W.E.K. acknowledge support by the US Department of Energy (DOE), Office of Energy Efficiency & Renewable Energy, Fuel Cell Technologies Office under Contract No. DE-AC36-08GO28308 with the National Renewable Energy Laboratory. The authors thank D. Zhu and J. Curulli for help using facilities at Keck Photonics Laboratory and Center for Electron Microscope and MicroAnalysis (CEMMA) at USC, respectively.
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J.Y. and D.K. conceived the idea and designed the experiment. D.K., J.L.Y., H.L., W.E.K., H.C., Y.X., B.G., T.G.D. and J.Y. performed the experiments. D.K., J.L.Y., H.L., W.E.K., H.C., T.G.D. and J.Y. analysed the data. D.K., J.L.Y., W.E.K., T.G.D. and J.Y. wrote the paper.
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Supplementary Methods, Supplementary Figures 1–14, Supplementary Tables 1–3. (PDF 1145 kb)
Supplementary Video 1
Unassisted solar water splitting with a wireless, tandem system of GaAs photoelectrodes. This video shows unassisted water splitting using two series-connected GaAs photoelectrodes in 0.5M H2SO4 aqueous solution under simulated AM1.5G solar illumination. While the light is turned on from the back side, oxygen and hydrogen gases are produced on the front side (the catalytic interface) of the photoanode (left) and the photocathode (right), respectively. (MP4 20060 kb)
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Kang, D., Young, J., Lim, H. et al. Printed assemblies of GaAs photoelectrodes with decoupled optical and reactive interfaces for unassisted solar water splitting. Nat Energy 2, 17043 (2017). https://doi.org/10.1038/nenergy.2017.43
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DOI: https://doi.org/10.1038/nenergy.2017.43
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