The zinc ion concentration dynamically regulated by an ionophore in the outer Helmholtz layer for stable Zn anode

The Zn dendrite limits the practical application of aqueous zinc-ion batteries in the large-scale energy storage systems. To suppress the growth of Zn dendrites, a zinc ionophore of hydroxychloroquine (defined as HCQ) applied in vivo treatment is investigated as the electrolyte additive. HCQ dynamically regulates zinc ion concentration gradient, promoting even Zn plating at the anode/electrolyte interface. This is evidenced by the scanning electron microscopy delivering planar Zn plating after cycling, which is further supported by the X-ray diffraction spectroscopy revealing the growth of Zn (0 0 2) plane. Additionally, the reduced produced H2 during Zn plating/stripping is detected by the in-situ differential electrochemical mass spectrometry (DEMS), which shows the resistance of Zn (0 0 2) to hydrogen evolution reaction. The mechanism of dynamic regulation for zinc ion concentration is demonstrated by the in-situ optical microscopy. The hydrated zinc ion can be further plated more rapidly to the uneven location than the case in other regions, which is resulted from the dynamic regulation for zinc ion concentration. Therefore, the uniform Zn plating is formed. A cycling life of 1100 h is exhibited in the Zn||Zn symmetric cell at 1.6 mA cm−2 with the capacity of 1.6 mAh cm−2. The Zn||Cu battery exhibits a cycling life of 200 cycles at 4 mA cm−2 with a capacity of 4 mAh cm−2 and the average Coulombic efficiency is larger than 99 %. The Zn||VO2 battery with HCQ modified electrolyte can operate for 1500 cycles at 4 A g−1 with a capacity retention of 90 %. This strategy in the present work is wished to advance the development of zinc-ion batteries for practical application.