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

Kottrup, K.G.; D'Agostini, S.; Langevelde, P.H. van; Siegler, M.A.; Hetterscheid, D.G.H. (2018)

Article / Letter to editor

The synthesis, characterization, and electrochemical studies of the dinuclear complex [(MeOH)Fe(Hbbpya)-mu-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.

• All authors: Kottrup, K.G.; D'Agostini, S.; Langevelde, P.H. van; Siegler, M.A.; Hetterscheid, D.G.H.
• Date: 2018-02-01
• Journal: ACS CATALYSIS
• Volume: 8
• Issue: 2
• Pages: 1052 - 1061
• DOI: doi:10.1021/acscatal.7b03284