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Despite the impressive merits of low-cost and high-safety electrochemical energy storage for aqueous zinc ion batteries, researchers have long struggled against the unresolved issues of dendrite growth and the side reactions of zinc metal anodes. Herein, a new strategy of zinc-electrolyte interface charge engineering induced by amino acid additives is demonstrated for highly reversible zinc plating/stripping. Through electrostatic preferential absorption of positively charged arginine molecules on the surface of the zinc metal anode, a self-adaptive zinc-electrolyte interface is established for the inhibition of water adsorption/hydrogen evolution and the guidance of uniform zinc deposition. Consequently, an ultra-long stable cycling up to 2200 h at a high current density of 5 mA cm−2 is achieved under an areal capacity of 4 mAh cm−2. Even cycled at an ultra-high current density of 10 mA cm−2, 900 h-long stable cycling is still demonstrated, demonstrating the reliable self-adaptive feature of the zinc-electrolyte interface. This work provides a new perspective of interface charge engineering in realizing highly reversible bulk zinc anode that can prompt its practical application in aqueous rechargeable zinc batteries.

In the face of high cost and insufficient energy density of current lithium ion batteries, aqueous rechargeable Zn-air batteries with the advantages of low cost, environmental benignity, safety and high energy density are spotlighted in recent years. The practical application of Zn-air batteries, however, is severely restricted by the high overpotential, which is associated with the inherent sluggish kinetics of oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) of air electrocatalysts. Recently, engineering heterostructured/hybrid electrocatalysts by modulating the interface chemistry has been demonstrated as an effective strategy to improve the catalytic performance. Basically, there occur significant electronic effect, geometric effect, coordination effect, synergistic effect, and confinement effect at the heterostructure interface, which intensely affect electrocatalysts’ performance in terms of intrinsic activity, active site density and durability. In this review, the recent progress on development of heterostructured air electrocatalysts by interface engineering is summarized. Particularly, the potential relationship between interface chemistry and oxygen electrocatalysis kinetics is bridged and outlined. This review would provide a comprehensive and in-depth understanding of the crucial role of the well-defined interfaces towards fast oxygen electrocatalysis, and would offer a solid scientific basis for the rational design of efficient heterostructured air electrocatalysts and beyond.