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Nickel-Containing Keggin-Type Polyoxometalates as Hydrogen Evolution Catalysts: Photochemical Structure-Activity
Kim von Allmen1, René Moré1, Rafael Müller1
1Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich (Switzerland), Fax: (+41) 44-635-6802.
Abstract:
In search of structure-activity relationships for polyoxometalate (POM)-based water reduction catalysts, nickel-monosubstituted Keggin-type POMs ([Ni(H2 O)XW11 O39 ]n- ; XP, 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.
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