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Search: WFRF:(Suarez Alcantara Karina) > (2013)

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  • Canton, Sophie, et al. (author)
  • Toward Highlighting the Ultrafast Electron Transfer Dynamics at the Optically Dark Sites of Photocatalysts
  • 2013
  • In: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 4:11, s. 1972-1976
  • Journal article (peer-reviewed)abstract
    • Building a detailed understanding of the structure function relationship is a crucial step in the optimization of molecular photocatalysts employed in water splitting schemes. The optically dark nature of their active sites usually prevents a complete mapping of the photoinduced dynamics. In this work, transient X-ray absorption spectroscopy highlights the electronic and geometric changes that affect such a center in a bimetallic model complex. Upon selective excitation of the ruthenium chromophore, the cobalt moiety is reduced through intramolecular electron transfer and undergoes a spin flip accompanied by an average bond elongation of 0.20 +/- 0.03 angstrom. The analysis is supported by simulations based on density functional theory structures (B3LYP*/TZVP) and FEFF 9.0 multiple scattering calculations. More generally, these results exemplify the large potential of the technique for tracking elusive intermediates that impart unique functionalities in photochemical devices.
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3.
  • Ruiz-Camacho, B., et al. (author)
  • Electrochemical and XAS investigation of oxygen reduction reaction on Pt-TiO2-C catalysts
  • 2013
  • In: International Journal of Hydrogen Energy. - : Elsevier BV. - 1879-3487 .- 0360-3199. ; 38:28, s. 12648-12656
  • Journal article (peer-reviewed)abstract
    • Pt-TiO2-C composites with different titanium oxide loading were synthesized by photo-deposition and chemical vapor deposition methods. The changes in their electronic properties improve the electrochemical activity toward the oxygen reduction reaction (ORR) compared to the Pt-C catalyst synthesized at the same conditions. The platinum samples were physically characterized by means of Transmission Electron Microscopy (TEM), Small Angle X-ray Scattering (SAXS), X-ray Absorption Spectroscopy (XAS) and X-ray Photo-electron Spectroscopy (XPS). Their electrochemical activity was also investigated by cyclic and linear voltammetry techniques. TEM analysis shows homogeneously dispersed platinum nanoparticles with an average particle size of 2 nm in all the synthesized samples. Form factor (morphology model) and particle size were determined by SAXS, the data adjusted to spherical Pt nanoparticles in both synthesis methods. XAS studies at the Pt L-3-edge shows a close interaction of Pt with the support material, i.e. C or TiO2. XPS analysis reveals surface modifications that induce electronic changes on Pt-TiO2-C. Significant differences in the ORR electrochemical activity were correlated to the TiO2 loading and the synthesis procedure. Copyright (C) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
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