Originally derived by Walther Nernst more than a century ago, the Nernst equation for the open-circuit voltage is a cornerstone in the analysis of electrochemical systems. Unfortunately, the assumptions behind its derivation are often overlooked in the literature, leading to incorrect forms of the equation when applied to complex systems (for example, those with ion-exchange membranes or involving mixed potentials). Such flaws can be avoided by applying a correct thermodynamic derivation independently of the form in which the electrochemical reactions are written. The proper derivation of the Nernst equation becomes important, for instance, in modeling of vanadium redox flow batteries or zinc-air batteries. The rigorous path towards the Nernst equation derivation starts in non-equilibrium thermodynamics.
We report a comprehensive modeling-based study of electroactive suspensions in slurry redox flow batteries undergoing discharge. A three-dimensional kinetic Monte Carlo model based on the variable step size method is used to describe the electrochemical discharge of a silicon/carbon slurry electrode in static mode (i.e., no fluid flow conditions). The model accounts for Brownian motion of particles, volume expansion of silicon upon lithium insertion, and formation and destruction of conducting carbon networks. Coupled to an electrochemical model, this study explores the impact of carbon fraction in the slurry and applied c-rate on the specific capacity. The trends obtained are analyzed by following the behavior of parameters such as number of contacts between electroactive particles and the percentage of electroactive silicon particles. Furthermore, instead of studying the bulk behavior of the slurry, here the focus is given to the slurry/current collector interface in order to illustrate its importance. Hereby, it is demonstrated how this modeling tool can lead to deeper understanding and optimization of electroactive particle suspensions in redox flow batteries.
The flow field design and material composition of the electrode plays an important role in the performance of redox flow batteries, especially when using highly viscous liquids. To enhance the discharge power density of zinc slurry air flow batteries, an optimum slurry distribution in the cell is key. Hence, several types of flow fields (serpentine, parallel, plastic flow frames) were tested in this study to improve the discharge power density of the battery. The serpentine flow field delivered a power density of 55 mW·cm −2 , while parallel and flow frame resulted in 30 mW·cm −2 and 10 mW·cm −2 , respectively. Moreover, when the anode bipolar plate material was changed from graphite to copper, the power density of the flow frame increased to 65 mW·cm −2 , and further improvement was attained when the bipolar plate material was further changed to copper-nickel. These results show the potential to increase the power density of slurry-based flow batteries by flow field optimization and design of bipolar plate materials.
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