Zinc‐Contained Alloy as a Robustly Adhered Interfacial Lattice Locking Layer for Planar and Stable Zinc Electrodeposition

Abstract

Stable zinc (Zn)/electrolyte interface is critical for developing rechargeable aqueous Zn‐metal batteries with long‐term stability, which requires the dense and stable Zn electrodeposition. Herein, an interfacial lattice locking (ILL) layer is constructed via the electro‐codeposition of Zn and Cu onto the Zn electrodes. The ILL layer shows a low lattice misfit (δ = 0.036) with Zn(002) plane and selectively locks the lattice orientation of Zn deposits, enabling the epitaxial growth of Zn deposits layer by layer. Benefiting from the unique orientation‐guiding and robustly adhered properties, the ILL layer enables the symmetric Zn||Zn cells to achieve an ultralong life span of >6000 h at 1 mA cm−2 and 1 mAh cm−2, a low overpotential (65 mV) at 10 mAh cm−2, and a stable Zn plating/stripping for >90 h at an ultrahigh Zn depth of discharge (≈85%). Even with a limited Zn supply and a high current density (8.58 mA cm−2), the ILL@Zn||Ni‐doped MnO2 cells can still survive for >2300 cycles.

Double-sided engineering for space-confined reversible Zn anodes

“…16,17,23,24 However, Zn anodes are susceptible to tremendous side reactions and severe dendrite growth at high DOD, which are much exaggerated compared with those discharged with low capacities. [25][26][27][28] More importantly, since metallic Zn anodes are ''hostless'', when they are deeply discharged, most of the Zn will be stripped out, and large volume changes together with uneven stripping process will inevitably occur (Fig. 1(a)).…”

A Universal Superhydrophobic‐Ionophilic Interfacial Strategy for Cycling Stable Aqueous Zinc Metal Electrodes under Low Current Density

“…[4] In addition, during the process of plating and stripping, zinc ions preferentially deposit at the tip due to the "tip effect", resulting in zinc dendrites or dead zinc. [5,6] These adverse DOI: 10.1002/adfm.202308661 reactions are amplified during the lowcurrent battery cycling, resulting in low coulomb efficiency and rapid capacity fading. [7][8][9] To improve the performance of zinc metal anode, there are several parallel routes of research: anode structure design, [6,10] electrolyte engineering, [11] functional separator design, [12,13] and solid electrolyte interface (SEI) design.…”

“…[5,6] These adverse DOI: 10.1002/adfm.202308661 reactions are amplified during the lowcurrent battery cycling, resulting in low coulomb efficiency and rapid capacity fading. [7][8][9] To improve the performance of zinc metal anode, there are several parallel routes of research: anode structure design, [6,10] electrolyte engineering, [11] functional separator design, [12,13] and solid electrolyte interface (SEI) design. [14,15] Among them, SEI design is the simplest and effective protection method, which has been widely studied.…”

A hydrophobic alloy-coated Zn anode for durable electrochromic devices

“…37 In the Cu-Zn phase diagram, the Zinc-rich CuZn alloy possesses a hexagonal close packed (HCP) structure, analogous to that of metallic Zn, promoting uniform Zn deposition. 38 In this work, hydrophobic CuZn 5 alloy was electrodeposited onto Zn foils, which can effectively regulate Zn 2+ desolvation and nucleation at the anode/electrolyte interface, endowing Zn@CuZn with reduced nucleation overpotential (Z 25.9 mV), extended coulombic efficiency (CE 99.4% over 350 cycles) and smaller voltage hysteresis than the bare Zn foil. The as-assembled ZECD (with PB cathode) exhibited accelerated switching time (coloration time t c = 7 s, bleaching time t b = 3 s) compared to Zn mesh||PB (t c = 10 s, t b = 12 s), and increased cycling stability over 1000 cycles.…”

“…37 In the Cu–Zn phase diagram, the Zinc-rich CuZn alloy possesses a hexagonal close packed (HCP) structure, analogous to that of metallic Zn, promoting uniform Zn deposition. 38…”