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

Yong Yan (), Ryan W. Crisp, Jing Gu, Boris D. Chernomordik, Gregory F. Pach, Ashley R. Marshall, John A. Turner and Matthew C. Beard ()
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Yong Yan: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Ryan W. Crisp: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Jing Gu: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Boris D. Chernomordik: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Gregory F. Pach: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Ashley R. Marshall: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
John A. Turner: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Matthew C. Beard: Chemistry and Nanoscience Center, National Renewable Energy Laboratory

Nature Energy, 2017, vol. 2, issue 5, 1-7

Abstract: 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.

Date: 2017
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DOI: 10.1038/nenergy.2017.52

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