Constructing Hydrophobic Interface with Close-Packed Coordination Supramolecular Network for Long-Cycling and...

Commercialization of aqueous zinc-metal batteries remains unrealistic due to the substantial dendrite growth and side reaction issues on the zinc anodes. It is highly demanded to develop easy-to-handle approaches for constructing stable, dense, as well as homogeneous solid anode/electrolyte interfaces. Herein, the authors construct the zinc anode interface with a close-packed Zn-TSA (TSA = thiosalicylate) coordination supramolecular network through the facile and up-scalable wet-chemical method. The hydrophobic Zn-TSA network can block solvated water and establish a solid-state diffusion barrier to well-distribute the interfacial Zn²⁺ , thus inhibiting hydrogen evolution and zinc dendrite growth on the anode. Meanwhile, the Zn-TSA network induces the formation of a uniform and stable solid electrolyte interphase composed of multiple inorganic-organic compounds. This denser structure can accommodate and self-heal the crack/degradation of the anode interphase associated with the repeated volume changes, and suppress the generation of detrimental by-product, Zn_x (OTF^- )_y (OH)_2x-y ·nH₂ O. Such a rationally fabricated anode/electrolyte interface further endows the assembled symmetric cells with superior plating/stripping stability for over 2000 h without dendrite formation (at 1 mA cm^-2 and 1 mAh cm^-2 ). Furthermore, this zinc anode has practical application in the Zn-MoS₂ and Zn-V₂ O₅ full cells. This study provides a new train of thought for constructing the dense interface of zinc-metal anode.