Simultaneous modulation interface adsorption and H-bonds network realizing highly reversible zinc metal anodes

Furious dendritic growth and destructive parasitic reactions (hydrogen evolution reaction, corrosion, and passivation) severely degraded the development of aqueous Zn-ion batteries (AZIBs) in the field of grid and stationary energy storage. Herein, trace amount of tetracycline hydrochloride (TC-HCl) additive (only 0.5 mM) is employed as a mediator to steer a stable Zn anode-electrolyte interface. Informed by theoretical calculations and experiment analysis, TC molecule with zincophilic groups can remodel the solvation sheath and disrupt H-bonds network due to its high electronegative O atoms, which effectively expedites the desolvation process and reduces the electrochemical activity of solvent water. Additionally, the TC molecules are preferentially adsorbed on the Zn electrode than active water molecules, which are beneficial for steering uniform nucleation and restricting the erosion of electrode. Benefitting from these synergistic effects, the Zn//Zn symmetric cell containing TC-HCl additive exhibits an ultra-long cycle life of exceeding 2200 h at 1.0 mA cm −2 and 1.0 mAh cm −2 . Accordingly, the practical Zn//α-MnO 2 full cell using the modified electrolyte also demonstrates the enhanced performance. This study provides valuable insights into the widespread use of trace electrolyte additives and facilitates the industrialization of AZIBs with long lifespans.