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Issue 8, 2011
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Electrochemical activation of molecular nitrogen at the Ir/YSZ interface

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Nitrogen is often used as an inert background atmosphere in solid state studies of electrode and reaction kinetics, of solid state studies of transport phenomena, and in applications e.g. solid oxide fuel cells (SOFC), sensors and membranes. Thus, chemical and electrochemical reactions of oxides related to or with dinitrogen are not supposed and in general not considered. We demonstrate by a steady state electrochemical polarisation experiments complemented with in situphotoelectron spectroscopy (XPS) that at a temperature of 450 °C dinitrogen can be electrochemically activated at the three phase boundary between N2, a metal microelectrode and one of the most widely used solid oxide electrolytes—yttria stabilized zirconia (YSZ)—at potentials more negative than E = −1.25 V. The process is neither related to a reduction of the electrolyte nor to an adsorption process or a purely chemical reaction but is electrochemical in nature. Only at potentials more negative than E = −2 V did new components of Zr 3d and Y 3d signals with a lower formal charge appear, thus indicating electrochemical reduction of the electrolyte matrix. Theoretical model calculations suggest the presence of anionic intermediates with delocalized electrons at the electrode/electrolyte reaction interface. The ex situSIMS analysis confirmed that nitrogen is incorporated and migrates into the electrolyte beneath the electrode.

Graphical abstract: Electrochemical activation of molecular nitrogen at the Ir/YSZ interface

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Publication details

The article was received on 29 Jun 2010, accepted on 01 Nov 2010 and first published on 11 Jan 2011

Article type: Paper
DOI: 10.1039/C0CP01024C
Citation: Phys. Chem. Chem. Phys., 2011,13, 3394-3410
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    Electrochemical activation of molecular nitrogen at the Ir/YSZ interface

    I. Valov, B. Luerssen, E. Mutoro, L. Gregoratti, R. A. De Souza, T. Bredow, S. Günther, A. Barinov, P. Dudin, M. Martin and J. Janek, Phys. Chem. Chem. Phys., 2011, 13, 3394
    DOI: 10.1039/C0CP01024C

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