Dual-Functional Interfacial Layer Enabled by Gating-Shielding Effects for Ultra-Stable Zn Anode.

Abstract

Large-scale application of low-cost, high-safety and environment-compatible aqueous Zn metal batteries (ZMBs) is hindered by Zn dendrite failure and side reactions. Herein, highly reversible ZMBs are obtained by addition of trace D-pantothenate calcium additives to engineer a dual-functional interfacial layer, which is enabled by a bioinspired gating effect for excluding competitive free water near Zn surface due to the trapping and immobilization of water by hydroxyl groups, and guiding target Zn²⁺ transport across interface through carboxyl groups of pantothenate anions, as well as a dynamic electrostatic shielding effect around Zn protuberances from Ca²⁺ cations to ensure uniform Zn²⁺ deposition. In consequence, interfacial side reactions are perfectly inhibited owing to reduced water molecules reaching Zn surface, and the uniform and compact deposition of Zn²⁺ is achieved due to promoted Zn²⁺ transport and deposition kinetics. The ultra-stable symmetric cells with beyond 9000 h at 0.5 mA cm^-2 with 0.5 mAh cm^-2 and over 5000 h at 5 mA cm^-2 with 1 mAh cm^-2, and an average Coulombic efficiency of 99.8% at 1 mA cm^-2 with 1 mAh cm^-2, are amazingly realized. The regulated-electrolyte demonstrates high compatibility with verified cathodes for stable full cells. This work opens a brand-new pathway to regulate Zn/electrolyte interface to promise reversible ZMBs.