Directionally Modulated Zinc Deposition by a Robust Zincophilic Cu-Phthalocyanine Protective Layer in Dendrite-Free Aqueous Zinc Ion Batteries.

Wang, Yidi; Jiang, Xinwei; Liang, Wenhao; Tawiah, Benjamin; Wang, Yang; Jia, Hao; Wong, Wai-Yeung · Adv Mater · 2025

basic_science · Level V

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Abstract

The directional modulation of zinc (Zn) deposition with further investigation of the dendrite-formation mechanism is vital in artificial anode protective layer for aqueous Zn-ion batteries (AZIBs). Herein, a robust metalated covalent organic framework (CuPc-COF) used as the artificial anode protective layer is proposed, in which the zincophilic sites of π-conjugated periodic skeletons are precisely designed to modulate the directional migration of Zn<sup>2+</sup>, the multiple redox-active sites facilitate the Zn<sup>2+</sup> confinement and transfer, and the central metal copper (Cu) serves as the inhibitor to eliminate the hydrogen evolution side reactions. By combining theoretical calculations with experiments, the π-conjugated planar CuPc-COF layer is a desired protective coating of AZIB anodes with directionally transport channels and abundant redox active sites, thus inducing two-dimensional deposition of Zn. Attributed to these superiorities, the fabricated CuPc-COF@Zn anode demonstrates excellent cycling lifespan in both symmetrical cell (exceeding 2500 h at 1 mA cm<sup>-2</sup>) and full cell with different cathodes (more than 3000 cycles at 1 A g<sup>-1</sup>), outperforming most reported zinc anodes with COF-based layers.