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In Situ Spectroelectrochemical Studies into the Formation and Stability of Robust Diazonium-Derived Interfaces on Gold Electrodes for the Immobilization of an Oxygen-Tolerant Hydrogenase
Citation key ISI:000439007700055
Author Harris, Tomos G. A. A. and Heidary, Nina and Kozuch, Jacek and Frielingsdorf, Stefan and Lenz, Oliver and Mroginski, Maria-Andrea and Hildebrandt, Peter and Zebger, Ingo and Fischer, Anna
Pages 23380-23391
Year 2018
ISSN 1944-8244
DOI 10.1021/acsami.8b02273
Address 1155 16TH ST, NW, WASHINGTON, DC 20036 USA
Volume 10
Number 27
Month JUL 11
Abstract Surface-enhanced infrared absorption spectroscopy is used in situ to determine the electrochemical stability of organic interfaces deposited onto the surface of nanostructured, thin-film gold electrodes via the electrochemical reduction of diazonium salts. These interfaces are shown to exhibit a wide electrochemical stability window in both acetonitrile and phosphate buffer, far surpassing the stability window of thiol-derived self-assembled monolayers. Using the same in situ technique, the application of radical scavengers during the electrochemical reduction of diazonium salts is shown to moderate interface formation. Consequently, the heterogeneous charge-transfer resistance can be reduced sufficiently to enhance the direct electron transfer between an immobilized redox-active enzyme and the electrode. This was demonstrated for the oxygen-tolerant [NiFe] hydrogenase from the ``Knallgas'' bacterium Ralstonia eutropha by relating its electrochemical activity for hydrogen oxidation to the interface properties.
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