Multi-electron redox chemistry is revolutionizing aqueous battery cathodes by enabling higher specific capacities through multi-electron transfer reactions. For example, Prussian blue analogs (PBAs) have demonstrated capacities exceeding 200 mAh/g by leveraging two-electron redox processes involving both Fe2+/Fe3+ and Mn2+/Mn3+ couples. This represents a >50% increase compared to traditional single-electron cathodes like LiFePO4, which typically deliver ~170 mAh/g in aqueous systems. Such materials are particularly promising for grid-scale storage due to their low cost and scalability.
The design of multi-electron anodes is equally critical, with materials like vanadium oxides (V2O5) achieving capacities up to 294 mAh/g through reversible intercalation of multiple Li+ ions per formula unit. In aqueous systems, this translates to energy densities approaching 150 Wh/kg when paired with high-capacity cathodes like PBAs or layered oxides such as Na0.44MnO2 (NMO). These advancements are driven by precise control over crystal structure and defect engineering to facilitate rapid ion diffusion and minimize capacity fade during cycling.
Advanced characterization techniques such as operando X-ray absorption spectroscopy (XAS) have provided unprecedented insights into multi-electron redox mechanisms in aqueous batteries.For instance,in situ XAS studies on Mn-based PBAs revealed reversible changes in Mn oxidation states from +2 to +4 during cycling,shedding light on the structural stability and phase transitions that govern performance.Such insights enable rational material design strategies to optimize redox activity while mitigating degradation pathways.
The integration of multi-electron redox chemistry with flow battery architectures is another emerging trend.For example,a Zn-Ce flow battery utilizing Ce3+/Ce4+ redox couples achieved an energy density of ~50 Wh/L,a significant improvement over traditional vanadium flow batteries (~25 Wh/L).This approach combines the scalability of flow batteries with the high energy density enabled by multi-electron reactions,making it suitable for large-scale renewable energy storage applications.
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