A four-electron Zn-I<sub>2</sub> aqueous battery enabled by reversible I<sup>-</sup>/I<sub>2</sub>/I<sup>+</sup> conversion.

Zou, Yiping; Liu, Tingting; Du, Qijun; Li, Yingying; Yi, Haibo; Zhou, Xing; Li, Zhuxin; Gao, Lujie et al. · Nat Commun · 2021

basic_science · Level V

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Abstract

Electrochemically reversible redox couples that embrace more electron transfer at a higher potential are the eternal target for energy storage batteries. Here, we report a four-electron aqueous zinc-iodine battery by activating the highly reversible I<sub>2</sub>/I<sup>+</sup> couple (1.83 V vs. Zn/Zn<sup>2+</sup>) in addition to the typical I<sup>-</sup>/I<sub>2</sub> couple (1.29 V). This is achieved by intensive solvation of the aqueous electrolyte to yield ICl inter-halogens and to suspend its hydrolysis. Experimental characterization and modelling reveal that limited water activity and sufficient free chloride ions in the electrolyte are crucial for the four-electron process. The merits of the electrolyte also afford to stabilize Zn anode, leading to a reliable Zn-I<sub>2</sub> aqueous battery of 6000 cycles. Owing to high operational voltage and capacity, energy density up to 750 Wh kg<sup>-1</sup> based on iodine mass was achieved (15-20 wt% iodine in electrode). It pushes the Zn-I<sub>2</sub> battery to a superior level among these available aqueous batteries.