Performance Loss of Activated Carbon Electrodes in Capacitive Deionization: Mechanisms and Material Property Predictors

Understanding the material property origins of performance decay in carbon electrodes is critical to maximizing the longevity of capacitive deionization (CDI) systems. This study investigates the cycling stability of electrodes fabricated from six commercial and two post-processed activated carbons. We find that the capacity decay rate of electrodes in half cells is positively correlated with the specific surface area and total surface acidity of the activated carbons. We also demonstrate that half-cell cycling stability is consistent with full cell desalination performance durability. Additionally, our results suggest that increase in internal resistance and physical pore blockage resulting from extensive cycling may be important mechanisms for the specific capacitance decay of activated carbon electrodes in this study. Our findings provide crucial guidelines for selecting activated carbon electrodes for stable CDI performance over long-term operation and insight into appropriate parameters for electrode performance and longevity in models assessing the techno-economic viability of CDI. Finally, our half-cell cycling protocol also offers a method for evaluating the stability of new electrode materials without preparing large, freestanding electrodes.