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Eliminating degradation in solid oxide electrochemical cells by reversible operation

Nature Materials volume 14, pages 239–244 (2015)Cite this article

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Abstract

One promising energy storage technology is the solid oxide electrochemical cell (SOC), which can both store electricity as chemical fuels (electrolysis mode) and convert fuels to electricity (fuel-cell mode). The widespread use of SOCs has been hindered by insufficient long-term stability, in particular at high current densities. Here we demonstrate that severe electrolysis-induced degradation, which was previously believed to be irreversible, can be completely eliminated by reversibly cycling between electrolysis and fuel-cell modes, similar to a rechargeable battery. Performing steam electrolysis continuously at high current density (1 A cm−2), initially at 1.33 V (97% energy efficiency), led to severe microstructure deterioration near the oxygen-electrode/electrolyte interface and a corresponding large increase in ohmic resistance. After 4,000 h of reversible cycling, however, no microstructural damage was observed and the ohmic resistance even slightly improved. The results demonstrate the viability of applying SOCs for renewable electricity storage at previously unattainable reaction rates, and have implications for our fundamental understanding of degradation mechanisms that are usually assumed to be irreversible.

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Figure 1: Storage of intermittent renewable electricity using a reversible SOC.
Figure 2: Comparison of the SOC stability during a constant-current electrolysis test and a reversible cycling test (cycles with 1 h in electrolysis mode and 5 h in fuel-cell mode).
Figure 3: Micrographs of the deteriorated oxygen-electrode/electrolyte interface in the cell operated continuously in electrolysis mode.
Figure 4: Change in the ohmic resistance of two SOCs during consecutive reversible charge–discharge cycles with different duty cycles for the fuel-cell mode (FC) and electrolysis mode (EL) time periods.

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Acknowledgements

This work was supported by the Program Commission on Sustainable Energy and Environment, The Danish Council for Strategic Research, through the SERC project (http://www.serc.dk), contract no. 2104-06-0011, and the Nordic Energy Research Council (NER) project no. 40000. We thank A. Hauch, M. Davodi and H. Henriksen for help and assistance with the experimental work, and other colleagues at DTU Energy Conversion for support and valuable discussions.

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  1. Department of Energy Conversion and Storage, Technical University of Denmark, Risø Campus, Frederiksborgvej 399, DK-4000 Roskilde, Denmark

    Christopher Graves, Sune Dalgaard Ebbesen, Søren Højgaard Jensen, Søren Bredmose Simonsen & Mogens Bjerg Mogensen

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  1. Christopher Graves
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  2. Sune Dalgaard Ebbesen
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Contributions

C.G. conceived the project and executed the electrochemical experiments and scanning electron microscopy analysis. C.G., M.B.M., S.D.E. and S.H.J. designed the electrochemical experiments. S.D.E. improved/developed the experimental set-up. S.B.S. executed the transmission electron microscopy analysis. C.G. wrote the paper with contributions from S.D.E., S.B.S., S.H.J. and M.B.M.

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Correspondence to Christopher Graves.

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Graves, C., Ebbesen, S., Jensen, S. et al. Eliminating degradation in solid oxide electrochemical cells by reversible operation. Nature Mater 14, 239–244 (2015). https://doi.org/10.1038/nmat4165

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