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Nickel-Containing Keggin-Type Polyoxometalates as Hydrogen Evolution Catalysts: Photochemical Structure-Activity Relationships.
Journal article

Nickel-Containing Keggin-Type Polyoxometalates as Hydrogen Evolution Catalysts: Photochemical Structure-Activity Relationships.

  • von Allmen K Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich (Switzerland), Fax: (+41) 44-635-6802.
  • Moré R Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich (Switzerland), Fax: (+41) 44-635-6802.
  • Müller R Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich (Switzerland), Fax: (+41) 44-635-6802.
  • Soriano-López J Institute of Chemical Research of Catalonia (ICIQ), Avenida Països Catalans 16, 43007 Tarragona (Spain).
  • Linden A Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich (Switzerland), Fax: (+41) 44-635-6802.
  • Patzke GR Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich (Switzerland), Fax: (+41) 44-635-6802.
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  • 2020-01-25
Published in:
  • ChemPlusChem. - 2015
electrochemistry
nickel
photochemistry
polyoxometalates
structure-activity relationships
English In search of structure-activity relationships for polyoxometalate (POM)-based water reduction catalysts, nickel-monosubstituted Keggin-type POMs ([Ni(H2 O)XW11 O39 ]n- ; XP, Si, Ge) were compared with respect to their activity in photochemical hydrogen evolution. The title compound series was characterized by single-crystal X-ray diffraction methods and a wide range of spectroscopic and electrochemical techniques. Nickel substitution was identified as a crucial feature for catalytic activity through comparison with nickel-free reference POMs. Furthermore, turnover number (TON) and turnover frequency strongly depended on the heteroatom X, and the highest TON among the series was recorded for [Ni(H2 O)GeW11 O39 ]6- . Photochemical hydrogen evolution activity was compared with redox and onset potentials obtained from electrochemical analyses. Furthermore, activity trends were correlated with electronic structure properties derived from density functional theory calculations.
Language
  • English
Open access status
closed
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Persistent URL
https://folia.unifr.ch/global/documents/266979
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