Deflection and control of the mixing region in membraneless vanadium micro redox flow batteries: Modeling and experimental validation

Membraneless micro redox flow batteries operate within the laminar flow regime to mitigate the convective mixing between catholyte and anolyte. The absence of an ion-exchange membrane reduces manufacturing costs and overall cell resistance, thereby enhancing battery performance. However, it also poses a new challenge: the precise control of the thin mixing layer established between the two co-flowing electrolytes. Undesired displacements of the mixing region lead to increased crossover losses and significant liquid transfer between tanks. This work addresses the deflection of the mixing region under varying flow conditions, considering electrolyte viscosity variations due to the changes in the local state of charge arising during battery operation. This is achieved through a combination of mathematical analysis, numerical simulations, and experimental results. The conservation equations and non-dimensional parameters governing the problem are first written and discussed. The model is then integrated numerically incorporating different inlet and outlet boundary conditions to simulate the effect of various flow control strategies. Next, the numerical results are validated against experimental realizations of the flow. Finally, three case studies are presented and discussed. This work highlights the relevance of variable viscosity in the operation of co-laminar membraneless micro redox flow batteries, and proposes for the first time feasible control methods to mitigate undesired disturbances in the hydraulic circuit, thereby minimizing crossover losses.