A Framework for Characterizing Commercial Solid Oxide Electrolysis Stacks Using Electrochemical Impedance Spectroscopy and Equivalent Circuit Modeling
Authors: Drasbæk Daniel , Kungas Rainer , Blennow Peter , Heiredal-Clausen Thomas , Høgh Jens V. T. , Hauch Anne 
Published: July 2021

Electrochemical impedance spectroscopy (EIS) is a powerful diagnostic tool used in a wide range of applications, including solid oxide fuel cells (SOFCs) and solid oxide electrolysis cells (SOECs). While EIS measurements on single cell level are commonplace, implementation of EIS on stack level remains limited, primarily due to the extremely low impedance of large-footprint cells, which imposes stringent demands on the impedance spectrometer and experimental setup (1). Furthermore, compared to single-cell EIS data, stack-level data reported in the literature are rarely subjected to the same degree of equivalent circuit modeling, making a detailed analysis of underlying electrochemical processes difficult.
Here, we report a framework for analyzing stack-level impedance spectroscopy data. The quality of the acquired data is first verified using Kramers-Kronig transformations (2), followed by the application of distribution of relaxation times (DRT) and analysis of the difference of impedance spectra (ADIS) methods to experimental data collected under a set of pre-determined operating conditions (electrochemical test procedure) (3-4). DRT and ADIS results were incorporated into the complex non-linear least squares (CNLS) fitting procedure and the validity of the chosen equivalent circuit model was confirmed by reconstruction of Nyquist, Bode, the individual electrochemical contributions, and DRT plots of the fitted data.
The developed framework was successfully implemented on a commercial 75-cell SOEC stack (TSP-1) developed by Haldor Topsoe (5). An electrochemical impedance spectrum is recorded simultaneously on all 13 cell groups in the stack using Zahner instrumentation. In this work, the electrochemical impedance data obtained from a state-of-the-art TSP-1 stack, containing three different types of Ni/YSZ based cells, is reported. The stack was initially investigated by EIS, using an electrochemical test procedure including CO2 electrolysis under constant conversion, H2O electrolysis under constant conversion, variations in the pO2 on the oxygen electrode, and finally temperature variations in CO2 electrolysis operation. This electrochemical test procedure was performed to develop an equivalent circuit model for the stack. Afterward, the stack was subjected to a degradation in steam electrolysis under 580 mA/cm2 (70% conversion), with an impedance spectrum being recorded every 24 hours. The operational point for this degradation test was chosen to match the real-life operation point of these stacks and hence to give a realistic image of any potential degradation. The developed framework and the equivalent circuit model developed for the stack was finally used to model the EIS data obtained during the degradation test. The modeling of these EIS data utilizes the full potential of electrochemical impedance spectroscopy and help identify any degradation mechanisms taking place in the stack, an analysis not previously reported on stack level.
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(2) B. Boukamp, J. Electrochem. Soc., 142, 1885 – 1894 (1995).
(3) S. H. Jensen, A. Hauch, P.V. Hendriksen, M. Mogensen, N. Bonanos, and T. Jacobsen. Journal of the Electrochemical Society, 154(12), B1325-B1330, (2007)
(4) H. Schichlein, and E. Ivers-Tiffee. Journal of Applied Electrochemistry, 32, 875-882, (2002).
(5) J. Rass-Hansen, P. Blennow, T. Heiredal-Clausen, R. Küngas, T. Holt Nørby, and S. Primdahl, Proceedings of the 12th European SOFC & SOE Forum, 318-325 (2016).

Figure 1