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Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%

Author

Listed:
  • Yong Yan

    (Chemistry and Nanoscience Center, National Renewable Energy Laboratory
    New Jersey Institute of Technology)

  • Ryan W. Crisp

    (Chemistry and Nanoscience Center, National Renewable Energy Laboratory
    Colorado School of Mines)

  • Jing Gu

    (Chemistry and Nanoscience Center, National Renewable Energy Laboratory
    San Diego State University)

  • Boris D. Chernomordik

    (Chemistry and Nanoscience Center, National Renewable Energy Laboratory)

  • Gregory F. Pach

    (Chemistry and Nanoscience Center, National Renewable Energy Laboratory
    University of Colorado)

  • Ashley R. Marshall

    (Chemistry and Nanoscience Center, National Renewable Energy Laboratory
    University of Colorado)

  • John A. Turner

    (Chemistry and Nanoscience Center, National Renewable Energy Laboratory)

  • Matthew C. Beard

    (Chemistry and Nanoscience Center, National Renewable Energy Laboratory)

Abstract

Multiple exciton generation (MEG) in quantum dots (QDs) has the potential to greatly increase the power conversion efficiency in solar cells and in solar-fuel production. During the MEG process, two electron–hole pairs (excitons) are created from the absorption of one high-energy photon, bypassing hot-carrier cooling via phonon emission. Here we demonstrate that extra carriers produced via MEG can be used to drive a chemical reaction with quantum efficiency above 100%. We developed a lead sulfide (PbS) QD photoelectrochemical cell that is able to drive hydrogen evolution from aqueous Na2S solution with a peak external quantum efficiency exceeding 100%. QD photoelectrodes that were measured all demonstrated MEG when the incident photon energy was larger than 2.7 times the bandgap energy. Our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.

Suggested Citation

  • Yong Yan & Ryan W. Crisp & Jing Gu & Boris D. Chernomordik & Gregory F. Pach & Ashley R. Marshall & John A. Turner & Matthew C. Beard, 2017. "Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%," Nature Energy, Nature, vol. 2(5), pages 1-7, May.
    • Handle: RePEc:nat:natene:v:2:y:2017:i:5:d:10.1038_nenergy.2017.52
    DOI: 10.1038/nenergy.2017.52
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