Decoupled architecture allows for independent pH control.

Redox flow batteries (RFBs) are essential for large-scale energy storage, particularly with the increasing use of renewable energy sources. The unique decoupled architecture of RFBs allows for better scalability as discharge duration increases compared to traditional battery designs. While early RFBs used transition-metal active materials, newer organic-based RFBs offer a wider range of chemistries and properties. However, one limitation has been their low open-circuit voltages (OCVs), hindering their commercial viability.

Addressing this challenge, researchers from Harvard University introduced a pH-decoupling strategy for organic-based RFBs to achieve higher OCVs, making them more commercially feasible. By maintaining a small pH difference between the posolyte and negolyte and using an acid-base regeneration cell, they were able to restore the pH values without the need for external acid or base additions, ensuring electrolyte stability.

The concept of pH-decoupled ARFB systems has shown promise in increasing OCVs, but it comes with technical challenges such as proton/hydroxide crossover and electrolyte deterioration. The Harvard team's innovative approach overcomes these hurdles by using a small regeneration cell and measuring crossover in membranes, paving the way for high-voltage ARFBs with OCVs above 2 V. This advancement can lead to cost-effective energy storage solutions for grid applications.

While the group demonstrated several pH-decoupled cells with high OCVs, further development is needed to optimize area-specific resistances and active material concentrations for practical use. The ultimate goal is to achieve OCVs around 2 V, enhancing energy density and cost efficiency. Combining the pH-decoupled concept with near-neutral pH electrolytes could further improve stability and broaden the electrochemical stability window.

Despite challenges like water-splitting reactions and membrane selection, the potential benefits of high-voltage ARFBs make them a promising solution for energy storage needs. The Harvard team's work showcases the potential of decoupled RFB architectures and the importance of innovative approaches, offering a path to organic-based ARFBs with high OCVs and long-term stability.

In conclusion, the development of pH-decoupled ARFB systems represents a significant advancement in energy storage technology, with the potential to revolutionize grid-scale applications. By addressing key limitations and introducing novel strategies, researchers are moving closer to realizing high-voltage ARFBs that can meet the demands of a sustainable energy future.

Source: https://www.nature.com/articles/s41560-024-01481-2

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