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Real time determination of the electronic structure of unstable reaction intermediates during Au₂O₃ Reduction

  • Szlachetko, Jakub Paul Scherrer Institut, Villigen, Switzerland - Institute of Physics, Jan Kochanowski University, Kielce, Poland
  • Sá, Jacinto Paul Scherrer Institut, Villigen, Switzerland - LSU Group, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland§
  • Nachtegaal, Maarten Paul Scherrer Institut, Villigen, Switzerland
  • Hartfelder, Urs Paul Scherrer Institut, Villigen, Switzerland - Department for Chemical and Bioengineering, ETH Zurich, Switzerland
  • Dousse, Jean-Claude Department of Physics, University of Fribourg, Switzerland
  • Hoszowska, Joanna Department of Physics, University of Fribourg, Switzerland
  • Fernandes, Daniel Luis Abreu Department of Chemistry, University of Aveiro, Portugal
  • Shi, Hongqing School of Physics, The University of Sydney, Australia
  • Stampfl, Catherine School of Physics, The University of Sydney, Australia
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    02.01.2014
Published in:
  • The Journal of Physical Chemistry Letters. - 2014, vol. 5, no. 1, p. 80–84
English Chemical reactions are always associated with electronic structure changes of the involved chemical species. Determining the electronic configuration of an atom allows probing its chemical state and gives understanding of the reaction pathways. However, often the reactions are too complex and too fast to be measured at in situ conditions due to slow and/or insensitive experimental techniques. A short-lived Au₂O compound has been detected for the first time under in situ conditions during the temperature-programmed reduction of Au₂O₃. A time-resolved resonant inelastic X-ray scattering experiment (RIXS) allowed the determination of changes in the Au electronic structure, enabling a better understanding of the reaction mechanism of Au(III) reduction. On the basis of time-resolved RIXS data analysis combined with genetic algorithm methodology, we determined the electronic structure of the metastable Au₂O intermediate species. The data analysis showed a notably larger value for the lattice constant of the intermediate Au as compared to the theoretical predictions. With support of DFT calculations, we found that such a structure may indeed be formed and that the expanded lattice constant is due to the termination of Au₂O on the Au₂O₃ structure.during Au₂O₃ Reduction
Faculty
Faculté des sciences
Department
Physique
Language
  • English
Classification
Physics
License
License undefined
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Persistent URL
https://folia.unifr.ch/unifr/documents/303695
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