The Role of Hole Localization in Sacrificial Hydrogen Production by Semiconductor-Metal Heterostructured Nanocrystals

ORAL

Abstract

The effect of hole localization on photocatalytic activity of Pt-tipped semiconductor nanocrystals is investigated. By tuning the energy balance at the semiconductor-ligand interface, we demonstrate that hydrogen production on Pt sites is efficient only when electron-donating molecules are used for stabilizing semiconductor surfaces. These surfactants play an important role in enabling an efficient and stable reduction of water by heterostructured nanocrystals as they fill vacancies in the valence band of the semiconductor domain, preventing its degradation. In particular, we show that the energy of oxidizing holes can be efficiently transferred to a ligand molecule, leaving the semiconductor domain intact. This allows re-using the inorganic portion of the ``degraded'' nanocrystal-ligand system simply by recharging these nanoparticles with fresh ligands.

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Authors

  • Scott Lambright

  • Dale Igram

    Cornell University, Air Force Research Labs, The Center for Photochemical Sciences and Department of Physics, BGSU, Department of Physics, BGSU, Department of Physics and Astronomy, Ball State University, Miami University, Johannes-Gutenberg-Universitat, Mainz, Germany, Martin-Luther-Universitat, Halle, Germany, The Ohio State University, Department of Physics, Columbus, OH 43210, USA, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA, Ohio Northern University, The Ohio State University, Department of Physics, Columbus, OH 43210, Sciprint.org, Ball State University, Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, PA 16802

  • Dale Igram

    Cornell University, Air Force Research Labs, The Center for Photochemical Sciences and Department of Physics, BGSU, Department of Physics, BGSU, Department of Physics and Astronomy, Ball State University, Miami University, Johannes-Gutenberg-Universitat, Mainz, Germany, Martin-Luther-Universitat, Halle, Germany, The Ohio State University, Department of Physics, Columbus, OH 43210, USA, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA, Ohio Northern University, The Ohio State University, Department of Physics, Columbus, OH 43210, Sciprint.org, Ball State University, Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, PA 16802

  • Dale Igram

    Cornell University, Air Force Research Labs, The Center for Photochemical Sciences and Department of Physics, BGSU, Department of Physics, BGSU, Department of Physics and Astronomy, Ball State University, Miami University, Johannes-Gutenberg-Universitat, Mainz, Germany, Martin-Luther-Universitat, Halle, Germany, The Ohio State University, Department of Physics, Columbus, OH 43210, USA, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA, Ohio Northern University, The Ohio State University, Department of Physics, Columbus, OH 43210, Sciprint.org, Ball State University, Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, PA 16802

  • Dale Igram

    Cornell University, Air Force Research Labs, The Center for Photochemical Sciences and Department of Physics, BGSU, Department of Physics, BGSU, Department of Physics and Astronomy, Ball State University, Miami University, Johannes-Gutenberg-Universitat, Mainz, Germany, Martin-Luther-Universitat, Halle, Germany, The Ohio State University, Department of Physics, Columbus, OH 43210, USA, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA, Ohio Northern University, The Ohio State University, Department of Physics, Columbus, OH 43210, Sciprint.org, Ball State University, Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, PA 16802

  • Dale Igram

    Cornell University, Air Force Research Labs, The Center for Photochemical Sciences and Department of Physics, BGSU, Department of Physics, BGSU, Department of Physics and Astronomy, Ball State University, Miami University, Johannes-Gutenberg-Universitat, Mainz, Germany, Martin-Luther-Universitat, Halle, Germany, The Ohio State University, Department of Physics, Columbus, OH 43210, USA, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA, Ohio Northern University, The Ohio State University, Department of Physics, Columbus, OH 43210, Sciprint.org, Ball State University, Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, PA 16802

  • Dale Igram

    Cornell University, Air Force Research Labs, The Center for Photochemical Sciences and Department of Physics, BGSU, Department of Physics, BGSU, Department of Physics and Astronomy, Ball State University, Miami University, Johannes-Gutenberg-Universitat, Mainz, Germany, Martin-Luther-Universitat, Halle, Germany, The Ohio State University, Department of Physics, Columbus, OH 43210, USA, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA, Ohio Northern University, The Ohio State University, Department of Physics, Columbus, OH 43210, Sciprint.org, Ball State University, Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, PA 16802

  • Dale Igram

    Cornell University, Air Force Research Labs, The Center for Photochemical Sciences and Department of Physics, BGSU, Department of Physics, BGSU, Department of Physics and Astronomy, Ball State University, Miami University, Johannes-Gutenberg-Universitat, Mainz, Germany, Martin-Luther-Universitat, Halle, Germany, The Ohio State University, Department of Physics, Columbus, OH 43210, USA, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA, Ohio Northern University, The Ohio State University, Department of Physics, Columbus, OH 43210, Sciprint.org, Ball State University, Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, PA 16802

  • Dale Igram

    Cornell University, Air Force Research Labs, The Center for Photochemical Sciences and Department of Physics, BGSU, Department of Physics, BGSU, Department of Physics and Astronomy, Ball State University, Miami University, Johannes-Gutenberg-Universitat, Mainz, Germany, Martin-Luther-Universitat, Halle, Germany, The Ohio State University, Department of Physics, Columbus, OH 43210, USA, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA, Ohio Northern University, The Ohio State University, Department of Physics, Columbus, OH 43210, Sciprint.org, Ball State University, Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, PA 16802

  • Dale Igram

    Cornell University, Air Force Research Labs, The Center for Photochemical Sciences and Department of Physics, BGSU, Department of Physics, BGSU, Department of Physics and Astronomy, Ball State University, Miami University, Johannes-Gutenberg-Universitat, Mainz, Germany, Martin-Luther-Universitat, Halle, Germany, The Ohio State University, Department of Physics, Columbus, OH 43210, USA, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA, Ohio Northern University, The Ohio State University, Department of Physics, Columbus, OH 43210, Sciprint.org, Ball State University, Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, PA 16802

  • Mikhail Zamkov