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

Mingquan LiuYahui WangYu LiFeng WuHuanyu LiYing LiXin FengBo LongQiao NiChuan WuYing Bai
Published in: Advanced materials (Deerfield Beach, Fla.) (2024)
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 Zn 2+ transport across interface through carboxyl groups of pantothenate anions, as well as a dynamic electrostatic shielding effect around Zn protuberances from Ca 2+ cations to ensure uniform Zn 2+ deposition. In consequence, interfacial side reactions are perfectly inhibited owing to reduced water molecules reaching Zn surface, and the uniform and compact deposition of Zn 2+ is achieved due to promoted Zn 2+ 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.
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