TY  - JOUR
AU  - Valov, I.
AU  - Luerssen, B.
AU  - Mutoro, E.
AU  - Gregoratti, L.
AU  - deSouza, R.A.
AU  - Bredow, T.
AU  - Günther, S.
AU  - Barinov, A.
AU  - Dudin, P.
AU  - Martin, M.
AU  - Janek, J.
TI  - Electrochemical activation of molecular nitrogen at the Ir/YSZ interface
JO  - Physical Chemistry Chemical Physics
VL  - 13
SN  - 1463-9076
CY  - Cambridge
PB  - RSC Publ.
M1  - PreJuSER-18278
SP  - 3394 - 3410
PY  - 2011
N1  - Record converted from VDB: 12.11.2012
AB  - 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 situ photoelectron spectroscopy (XPS) that at a temperature of 450 °C dinitrogen can be electrochemically activated at the three phase boundary between N(2), 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 situ SIMS analysis confirmed that nitrogen is incorporated and migrates into the electrolyte beneath the electrode.
KW  - J (WoSType)
LB  - PUB:(DE-HGF)16
C6  - pmid:21221435
UR  - <Go to ISI:>//WOS:000287041700046
DO  - DOI:10.1039/c0cp01024c
UR  - https://juser.fz-juelich.de/record/18278
ER  -