Aqueous batteries are an emerging candidate for low‐cost and environmentally friendly grid storage systems. Designing such batteries from inexpensive, abundant, recyclable, and nontoxic organic active materials provides a logical step toward improving both the environmental and economic impact of these systems. Herein the first ever battery material that works with simultaneous uptake and release of both cations and anions is proposed by coupling p‐type (bipyridinium) and n‐type (naphthalene diimide) redox moieties. It represents one of a new family of electrode materials which demonstrates an optimal oxidation potential (−0.47 V vs saturated calomel electrode), extremely fast kinetics, a highly competitive capacity (63 mA h g−1 at 4C), and cyclability in both neutral Na+ and Mg2+ electrolytes of molar range concentration. Through a combination of UV–vis spectroelectrochemistry, electrochemical quartz‐crystal microbalance, Operando synchrotron‐X‐ray diffraction, and density functional theory calculations a novel dual cation/anion insertion mechanism was proven and rationalized. Based on these findings, this innovative p/n‐type product may well provide a viable option for use as a negative electrode material, thereby promoting the design of cutting‐edge, low‐cost, rocking‐chair dual‐ion aqueous batteries.
Thick electrodes with sodium and even anions intercalation organic compounds integrated in a neutral-pH aqueous battery offer unique advantages in terms of round trip efficiency, environmental impact, and scalability for off or in-grid renewable energy storage. Herein we report on the first anion-rocking chair / dual-ion organic battery. The latter reaches 35 Wh/kgmaterials at C/8 rate. It shows remarkable cyclability and Coulombic efficiency in a cheap and neutral NaClO4 electrolyte pouch cell with highly loaded millimeter thick electrodes (5 mAh/cm²). This achievement is based on a thorough study of a commercial benzene TEMPO compound (4-hydroxy TEMPO benzoate) and its naphthalene derivative (4-carboxy TEMPO naphthalate) as cathode materials, and a bipyridinium-naphthalene oligomer as the anode. Combined UV-vis spectroelectrochemistry and operando XRD account for the much improved cyclability of the hydrophobic 4-carboxy TEMPO naphthalate at the expense of a lower specific capacity. This trend is reversed in the case of the 4-hydroxy TEMPO benzoate derivative. Results show kinetic limitations of the 4-hydroxy TEMPO benzoate are associated with the surrounding composite electrode, while inner-grain ionic and/or electronic transports play a decisive role for the 4-carboxy TEMPO naphthalate.
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