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Catalytic Activity of an Iron-Based Water Oxidation Catalyst: Substrate Effects of Graphitic Electrodes.


ABSTRACT: The synthesis, characterization, and electrochemical studies of the dinuclear complex [(MeOH)Fe(Hbbpya)-?-O-(Hbbpya)Fe(MeOH)](OTf)4 (1) (with Hbbpya = N,N-bis(2,2'-bipyrid-6-yl)amine) are described. With the help of online electrochemical mass spectrometry, the complex is demonstrated to be active as a water oxidation catalyst. Comparing the results obtained for different electrode materials shows a clear substrate influence of the electrode, as the complex shows a significantly lower catalytic overpotential on graphitic working electrodes in comparison to other electrode materials. Cyclic voltammetry experiments provide evidence that the structure of complex 1 undergoes reversible changes under high-potential conditions, regenerating the original structure of complex 1 upon returning to lower potentials. Results from electrochemical quartz crystal microbalance experiments rule out that catalysis proceeds via deposition of catalytically active material on the electrode surface.

SUBMITTER: Kottrup KG 

PROVIDER: S-EPMC5805403 | biostudies-literature | 2018 Feb

REPOSITORIES: biostudies-literature

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Catalytic Activity of an Iron-Based Water Oxidation Catalyst: Substrate Effects of Graphitic Electrodes.

Kottrup Konstantin G KG   D'Agostini Silvia S   van Langevelde Phebe H PH   Siegler Maxime A MA   Hetterscheid Dennis G H DGH  

ACS catalysis 20171221 2


The synthesis, characterization, and electrochemical studies of the dinuclear complex [(MeOH)Fe(Hbbpya)-μ-O-(Hbbpya)Fe(MeOH)](OTf)<sub>4</sub> (<b>1</b>) (with Hbbpya = <i>N,N</i>-bis(2,2'-bipyrid-6-yl)amine) are described. With the help of online electrochemical mass spectrometry, the complex is demonstrated to be active as a water oxidation catalyst. Comparing the results obtained for different electrode materials shows a clear substrate influence of the electrode, as the complex shows a signi  ...[more]

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