Zn-based batteries have attracted extensive attention due to their high theoretical energy density, safety, abundant resources, environmental friendliness, and low cost. They are a new energy storage and conversion technology with significant development potential and have been widely used in renewable energy and portable electronic devices. Considerable attempts have been devoted to improving the performance of Zn-based batteries. Specifically, battery cycle life and energy efficiency can be improved by electrolyte modification and the construction of highly efficient rechargeable Zn anodes. This review compiles the progress of the research related to Zn anodes and electrolytes, especially in the last five years. This review will introduce fundamental concepts, summarize recent development, and inspire further systematic research for high-performance Zn-based batteries in the future. 

https://www.sciopen.com/article_pdf/1589910638268375041.pdf

Recent advances and perspectives for Zn-based batteries: Zn anode and electrolyte

The aqueous zinc‐ion battery has the advantages of environmental friendliness, safety, and reliability, which is expected to be used for large‐scale energy storage. However, due to the high activity of water, the hydrogen evolution reaction (HER) easily occurs on the surface of the zinc anode during the charge–discharge process, which is accompanied by corrosion, by‐products, and dendrite formation. Herein, a new‐type eutectic electrolyte consisting of ZnCl2, tetramethylurea (TMU), and H2O with the optimal molar ratio of 1:3:1 (ZT‐1) is developed for the high‐stability zinc anodes. The H2O in this system is doubly bound through the coordination with Zn2+ and the hydrogen bonding with TMU, thus leading to the greatly inhibited activity of H2O. In addition, the H2O and TMU are successively stripped during the desolvation process of ZnCl2(TMU)(H2O), followed by the deposition of [ZnCl2] at the zinc interface. In this way, the tendency of HER, corrosion, dendrites, and by‐products induced by the decomposition of H2O molecules at the zinc interface is minimized, enabling a much more stable plating/stripping process of Zn2+. Consequently, the Zn//Zn symmetric cell can stably cycle for >2000 h, while the Zn//Cu half cell can stably cycle 800 times with an average Coulombic efficiency of 99.5%.

Eutectic Electrolytes with Doubly‐Bound Water for High‐Stability Zinc Anodes

Aqueous zinc metal batteries (AZMBs) are promising candidates for next-generation energy storage due to the excellent safety, environmental friendliness, natural abundance, high theoretical specific capacity, and low redox potential of zinc (Zn) metal. However, several issues such as dendrite formation, hydrogen evolution, corrosion, and passivation of Zn metal anodes cause irreversible loss of the active materials. To solve these issues, researchers often use large amounts of excess Zn to ensure a continuous supply of active materials for Zn anodes. This leads to the ultralow utilization of Zn anodes and squanders the high energy density of AZMBs. Herein, the design strategies for AZMBs with high Zn utilization are discussed in depth, from utilizing thinner Zn foils to constructing anode-free structures with theoretical Zn utilization of 100%, which provides comprehensive guidelines for further research. Representative methods for calculating the depth of discharge of Zn anodes with different structures are first summarized. The reasonable modification strategies of Zn foil anodes, current collectors with pre-deposited Zn, and anode-free aqueous Zn metal batteries (AF-AZMBs) to improve Zn utilization are then detailed. In particular, the working mechanism of AF-AZMBs is systematically introduced. Finally, the challenges and perspectives for constructing high-utilization Zn anodes are presented. 

Design Strategies for Aqueous Zinc Metal Batteries with High Zinc Utilization: From Metal Anodes to Anode-Free Structures

Aqueous Zn metal batteries are considered as competitive candidates for next-generation energy storage systems due to their excellent safety, low cost and environmental friendliness. However, the inevitable dendrite growth, severe hydrogen evolution, surface passivation and sluggish reaction kinetics of Zn metal anodes hinder the practical application of Zn metal batteries. Detailed summaries and prospects have been reported focusing on the research progress and challenges of Zn metal anodes, including electrolyte engineering, electrode structure design and surface modification. However, the essential electrical mechanisms that significantly influence Zn2+ ion migration and deposition behaviors have not been reviewed yet. Herein, in this review, we systematically discuss the regulation mechanisms of electrical-related electrostatic repulsive/attractive interactions on Zn2+ ions migration, desolvation and deposition behaviors. Meanwhile, electric field regulation strategies to promote the Zn2+ ions diffusion and uniform Zn deposition are comprehensively reviewed, including enhancing and homogenizing electric field intensity inside the batteries and adding external magnetic/pressure/thermal fields to couple with the electric field. Finally, we offer future perspectives on the research directions of the electrical-related strategies for building better Zn metal batteries in practical applications. This article is protected by copyright. All rights reserved.

Understanding the Electrical Mechanisms in Aqueous Zinc Metal Batteries: from Electrostatic Interactions to Electric Field Regulation.

Abstract In aqueous electrolytes, the uncontrollable interfacial evolution caused by a series of factors such as pH variation and unregulated Zn 2+ diffusion would usually result in the rapid failure of metallic Zn anode. Considering the high correlation among various triggers that induce the anode deterioration, a synergistic modulation strategy based on electrolyte modification is developed. Benefitting from the unique pH buffer mechanism of the electrolyte additive and its capability to in situ construct a zincophilic solid interface, this synergistic effect can comprehensively manage the thermodynamic and kinetic properties of Zn anode by inhibiting the pH variation and parasitic side reactions, accelerating de‐solvation of hydrated Zn 2+ , and regulating the diffusion behavior of Zn 2+ to realize uniform Zn deposition. Thus, the modified Zn anode can achieve an impressive lifespan at ultra‐high current density and areal capacity, operating stably for 609 and 209 hours at 20 mA cm −2 , 20 mAh cm −2 and 40 mA cm −2 , 20 mAh cm −2 , respectively. Based on this exceptional performance, high loading Zn||NH 4 V 4 O 10 batteries can achieve excellent cycle stability and rate performance. Compared with those previously reported single pH buffer strategies, the synergistic modulation concept is expected to provide a new approach for highly stable Zn anode in aqueous zinc‐ion batteries. 

Synergistic Modulation of In-Situ Hybrid Interface Construction and pH Buffering Enabled Ultra-Stable Zn Anode at High Current Density and Areal Capacity.

An ultrahigh rate dendrite-free Zn metal deposition/striping enabled by silver nanowire aerogel with optimal atomic affinity with Zn

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An ultrahigh rate dendrite-free Zn metal deposition/striping enabled by silver nanowire aerogel with optimal atomic affinity with Zn