The operating temperature of vanadium redox flow batteries (VRFBs) affects their performance and reliability. However, previous studies focused on evaluating the effects on the performance of lab-scale single cells, in which electrolyte flow rates and current densities are different from those in stack-scale VRFBs, leading to a lack of guidance for the design of stacks. In this work, we investigate thermal effects on the performance of stack-scale VRFBs. It is found that as the operating temperature increases from 25 to 50°C, the discharge capacity increases by 42%, whereas the energy efficiency increases by 10%, implying that the temperature has greater effects on the discharge capacity than that on the energy efficiency. Additionally, the enhancement effect of temperature on the energy efficiency is gradually weakened with increasing flow rate, while that on the discharge capacity is almost unchanged. Furthermore, the enhancement effect of temperature on energy efficiency increases with the operating current density. Notably, an optimum operating condition of the stack-scale VRFBs is identified with a critical flow rate (2.88 mL min-1 cm-2) at 40°C to achieve a high system efficiency. This work provides guidance for the design of stack-scale VRFBs with high performance and safety.
Polybenzimidazole (PBI)-based membranes are one of the most promising proton exchange membranes for vanadium redox flow batteries (VRFBs) due to their excellent ion selectivity. However, their relatively lower proton conductivity limits their application. Herein, a PBI membrane with both high proton conductivity and ion selectivity is prepared through a secondary phosphoric acid-doping method. The secondary-doped PBI membrane has a lower doping level in the surface layer while a higher doping level at the inner layer, forming a significant gradient-doped structure. In this structure, the former ensures an excellent ion selectivity while the latter enables a preferable proton conductivity. As a result, the VRFB with the secondary-doped PBI membrane exhibits an ultrahigh coulombic efficiency (CE) of 99.2% at the operating current density of 200 mA cm-2, which is significantly higher than that of the Nafion 212 membrane (97.7%), signifying an excellent ion selectivity. Meanwhile, the corresponding voltage efficiency is high, up to 87.1%, which is also better than that of the Nafion 212 membrane (84.8%), indicating a high proton conductivity. Therefore, the secondary-doped PBI membrane might be a promising candidate for the highly efficient membrane for VRFB, and the secondary-doping method is simple and facile to realize engineering applications.
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