Multifunctional Interface Layer Constructed by Trace Zwitterions for Highly Reversible Zinc Anodes

The inhomogeneous plating/stripping of Zn anode, attributed to dendrite growth and parasitic reactions at the electrode/electrolyte interface, severely restricts its cycling life‐span. Here, trace zwitterions (trifluoroacetate pyridine, TFAPD) are introduced into the aqueous electrolyte to construct a multifunctional interface that enhances the reversibility of Zn anode. The TFA− anions with strong specific adsorption adhere onto the Zn surface to reconstruct the inner Helmholtz plane (IHP), preventing the hydrogen evolution and corrosion side reactions caused by free H2O. The Py+ cations accumulate on the outer Helmholtz plane (OHP) of Zn anode with the force of electric field during Zn2+ plating, forming a shielding layer to uniformize the deposition of Zn2+. Besides, the adsorbed TFA− and Py+ promote the desolvation process of Zn2+ resulting in fast reaction kinetics. Thus, the Zn||Zn cells present an outstanding cycling performance of more than 10000 hours. And even at 85% utilization rate of Zn, it can stably cycle for over 200 hours at 10 mA cm−2 and 10 mAh cm−2. The Zn||I2 full cell exhibits a capacity retention of over 95% even after 30000 cycles. Remarkably, the Zn||I2 pouch cells (95 mAh) deliver a high‐capacity retention of 99% after 750 cycles.