Ion Highway Regulator Enables Highly Reversible Zinc Metal Anode

Employing ZrSiO₄ as Zn²⁺ highway regulator to reconstruct the original zinc anode two-phase interface (ZSP@Zn). The lower interfacial migration energy barrier and adsorption energy can facilitate Zn²⁺ rapid deposition, accelerate the deposition kinetics, and thereby effectively inhibit the dendrites formation. This Zn²⁺ highway regulator ensures the excellent cycling stability and deep reversibility performance of AZMBs.

ABSTRACT

The issue of zinc dendrites and chaotic Zn²⁺ deposition at electrode/electrolyte interface significantly hindered commercialization of aqueous zinc metal batteries (AZMBs). Therefore, we propose a Zn²⁺ highway regulator strategy by introducing nano-zirconium silicate interphase (ZSP) to address the above issues. ZSP with low Zn²⁺ migration energy barrier of ZrSiO₄ can facilitate Zn²⁺ transport efficiency and inhibit dendrite growth, thereby achieving highly reversible zinc metal anode. The featured ZSP@Zn//ZSP@Zn symmetric cell demonstrates an ultra-long cycle life exceeding 4700 h at 0.25 mA cm⁻² (0.25 mAh cm⁻²). Even under a deep depth of discharge ≈85.4%, it still maintains stable operation for over 400 h. Furthermore, the advanced NH₄V₄O₁₀//ZSP@Zn full cell, featuring a high mass loading of 15.25 mg cm⁻² (N/P = 2.1), exhibited stable performance over 520 cycles (1 A g⁻¹), retaining 80.48% of initial capacity (187.32 mAh g⁻¹). More surprisingly, the feature pouch cell with a loading of 11.96 mg cm⁻² (N/P = 2.3) demonstrated excellent performance (maximum capacity of 209.22 mAh g⁻¹), maintaining a capacity retention rate of 81.14% after 150 cycles at 0.8 A g⁻¹. This strategy provides a new avenue for highly reversible AZMBs.