Machine learning-enabled performance prediction and optimization for iron–chromium redox flow batteries

Iron-chromium flow batteries (ICRFBs) are regarded as one of the most promising large-scale energy storage devices with broad application prospects in recent years. However, transitioning from laboratory-scale development to industrial-scale deployment can be a time-consuming process due to the multitude of complex factors that impact ICRFB stack performance. Herein, a data-driven optimization methodology applying active learning, informed by an extensive survey of the literature encompassing diverse experimental conditions, is proposed to enable exceptional precision in predicting ICRFB system performance considering both operation conditions and key materials selection. Specifically, multitask ML models are trained on experimental data with a high prediction accuracy (R² > 0.92) to link ICRFB properties to energy efficiency, coulombic efficiency, and capacity. We also interpret the ML models based on Shapley additive explanations and extract valuable insights into the importance of descriptors. It is noted that the operation conditions (current density and cycle number) and the electrode type are the most critical descriptors affecting the voltage efficiency and coulombic efficiency while the electrode size strongly affects the capacity. Moreover, active learning is used to explore the most optimized cases considering the highest energy efficiency and capacity. The versatility and robustness of the approach are demonstrated by the successful validation between ML prediction and our experiments of energy efficiency (±0.15%) and capacity (±0.8%). This work not only affords fruitful data-driven insight into the property-performance relationship, but also unveils the explainability of critical properties on the performance of ICRFBs, which accelerates the rational design of next-generation ICRFBs.