4.8 Article

Photochemical Charge Separation in Nanocrystal Photocatalyst Films: Insights from Surface Photovoltage Spectroscopy

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 5, Issue 5, Pages 782-786

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jz500136h

Keywords

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Funding

  1. Research Corporation for Science Advancement (Scialog award)
  2. National Science Foundation (NSF) [1152250, 1133099]
  3. Direct For Mathematical & Physical Scien
  4. Division Of Chemistry [1152250] Funding Source: National Science Foundation
  5. Directorate For Engineering [1133099] Funding Source: National Science Foundation
  6. Div Of Chem, Bioeng, Env, & Transp Sys [1133099] Funding Source: National Science Foundation

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Photochemical charge generation, separation, and transport at nanocrystal interfaces are central to photoelectrochemical water splitting, a pathway to hydrogen from solar energy. Here, we use surface photovoltage spectroscopy to probe these processes in nanocrystal films of HCa2Nb3O10, a proven photocatalyst. Charge injection from the nanoparticles into the gold support can be observed, as well as oxidation and reduction of methanol and oxygen adsorbates on the nanosheet films. The measured photovoltage depends on the illumination intensity and substrate material, and it varies with illumination time and with film thickness. The proposed model predicts that the photovoltage is limited by the built-in potential of the nanosheet-metal junction, that is, the difference of Fermi energies in the two materials. The ability to measure and understand these light-induced charge separation processes in easy-to-fabricate films will promote the development of nanocrystal applications in photoelectrochemical cells, photovoltaics, and photocatalysts.

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