Constructing Hydrophobic Interface with Close‐Packed Coordination Supramolecular Network for Long‐Cycling and Dendrite‐Free Zn‐Metal Batteries

Abstract

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, Znx(OTF‐)y(OH)2x−y·nH2O. 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‐V2O5 full cells. This study provides a new train of thought for constructing the dense interface of zinc‐metal anode.

Tuning Ion Transport at the Anode‐Electrolyte Interface via a Sulfonate‐Rich Ion‐Exchange Layer for Durable Zinc‐Iodine Batteries

“…Besides, the introduction of PVDF into SC-PPS appears to reduce the hydrophilicity of the SC-PPS layer (Figure S16, Supporting Information), while a hydrophobic layer could enhance the corrosion resistance of zinc toward aqueous electrolytes. [40][41][42] The interfacial environment between the SC-PPS@Zn electrode and ZnSO 4 electrolyte was further analyzed by conducting cyclic voltammetry (CV) tests in a three-electrode system. As plotted in Figure 4d, the point located at the intersection of nucleation processes is well-known as the crossover potential (E co ).…”

Regulation of Outer Solvation Shell Toward Superior Low‐Temperature Aqueous Zinc‐Ion Batteries

“…Notably, the corrosion current of the Zn electrode in 30% 2-propanol electrolyte (0.282 µA cm −2 ) is much reduced compared with that of Zn electrode in conventional electrolyte (81.5 µA cm −2 ) (Figure S28b, Supporting Information). [35,36] In Figure S29 (Supporting Information), by the comparison of the Zn-Ti cell with/without the addition of 2-propanol, the 2-propanol/water/Zn(OTf) 2 composite electrolyte shows a higher Coulombic efficiency (99.06%) compared with conventional electrolyte (95.07%) with limited HER, and less Zn corrosion and dead Zn formation.…”

Artificial Interphase Layer for Stabilized Zn Anodes: Progress and Prospects

“…Tao et al constructed a novel Zn anode interface with close-packed Zn-TSA (TSA = thiosalicylate) coordination supramolecular network. [170] During the cycling process, a hybrid AIL mainly composed of ZnF 2 , ZnS, and organisms was spontaneously formed in the Zn-TSA network. This AIL can not only block solvated water and establish a solid-state diffusion barrier to well-distribute the interfacial Zn 2+ , but also have a self-healing capability to accommodate the crack of anode interface.…”