Abstract
Aqueous organic redox flow batteries (AORFBs) offer promise for large-scale energy storage due to
inherent safety and abundant sourcing. While significant advances have produced stable, soluble
negative electrolytes (negolytes), cost-effective positive electrolytes
(posolytes) simultaneously achieving high solubility, redox potential, and stability remain limited,
restricting the overall energy density and lifetime of the battery system. Herein, we report a highperformance
organo-ferrocyanide posolyte, sodium pentacyano(pyrazine-2-carboxylate)iron(II)
(FePz), for AORFBs. Derived from commercial nitroprusside through organic ligand engineering,
FePz exhibits a high redox potential of 0.62 V and a record 2.3 M aqueous solubility. FePz
demonstrates universal pairing capability and unprecedented cycling stability across diverse negolytes
like viologen, phenazine derivatives, and zinc anode. Notably, when coupled with a phenazine-based
negolyte at 2.0 M FePz concentration, the system maintains steady operation with a super low capacity
fade (0.025% per day) over 71 days. Integration with a Zn-based configuration achieves a 1.4 V cell
voltage, delivering a maximum power density of 0.22 W m−2 and a high energy density of 38 Wh L−1.
Furthermore, modular ligand engineering of organo-ferrocyanides unlocks vast electrolyte design
possibilities for energy storage and conversion applications.



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