Journal
ELECTROCHIMICA ACTA
Volume 69, Issue -, Pages 301-307Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.electacta.2012.03.006
Keywords
Flow battery; Semi-solid; Modeling; Energy storage; Lithium-ion
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Funding
- Defense Advanced Research Projects Agency (DARPA) [FA8650-09-D-5037]
- Advanced Research Projects Agency-Energy (ARPA-E)
- US Department of Energy [DE-AR0000065]
- agency of the United States Government
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A mathematical model of flow cell operation incorporating hydrodynamic and electrochemical effects in three dimensions is developed. The model and resulting simulations apply to recently demonstrated high energy-density semi-solid flow cells. In particular, state of charge gradients that develop during low flow rate operation and their effects on the spatial non-uniformity of current density within flow cells are quantified. A one-dimensional scaling model is also developed and compared to the full three-dimensional simulation. The models are used to demonstrate the impact of the choice of electrochemical couple on flow cell performance. For semi-solid flow electrodes, which can use solid active materials with a wide variety of voltage-capacity responses, we find that cell efficiency is maximized for electrochemical couples that have a relatively flat voltage vs. capacity curve, operated under slow flow conditions. For example, in flow electrodes limited by macroscopic charge transport, an LiFePO4-based system requires one-third the polarization to reach the same cycling rate as an LiCoO2-based system, all else being equal. Our conclusions are generally applicable to high energy density flow battery systems, in which flow rates can be comparatively low for a given required power. (C) 2012 Elsevier Ltd. All rights reserved.
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