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Aqueous zinc‐ion batteries (AZIBs) suffer from rampant Zn dendrites growth, corrosion and sluggish transport kinetics, all of which have a serious impact on their performance and practical applications. Therefore, porous carbon nanofibers (BTO@PCNFs) loaded with BaTiO3 nanoparticles (BTO NPs) are constructed as a multifunctional interlayer for stabilizing the Zn anodes. Owing to the synergistic effect of BTO NPs and 3D porous carbon framework, this interlayer can achieve uniform electric field distribution, accelerate Zn2+ migration, and promote ion flux homogenization, thus leading to uniform Zn deposition. Meanwhile, the BTO@PCNFs interlayer demonstrates excellent anti‐corrosion effect, which can effectively prevent the side reactions. Benefiting from the synergistic effect of interlayers, the BTO@PCNFs multifunctional interlayers achieve a comprehensive optimization of the Zn anodes. The BTO@PCNFs‐Zn electrode exhibits lower nucleation overpotential (33.5 mV) at 0.5 mA cm−2. The Zn//Zn symmetrical cell with BTO@PCNFs interlayer exhibits ultra‐low overpotential (14 mV) and ultra‐long cycle life (5250 h at 0.5 mA cm−2). Even at high current density (30 mA cm−2), the BTO@PCNFs‐Zn electrode can be stably cycled for more than 830 h, achieving an ultra‐high cumulative capacity of 12 450 mAh cm−2. The multifunctional interlayers can provide a reference for the design of high‐performance Zn anodes.

Highlights Digital holography can realize the in situ observation of electrode/electrolyte interface and provide dynamic evolution information of the liquid phase of electrode, which is both efficient and effective in investing the interficial electrochemical mechanism and screening electrolyte additives. Thioacetamide electrolyte additive effectively enhances the electrochemical performance of Zn anode by regulating the interficial ion flux to induce dendrite-free Zn deposition and constructing adsorption molecule layers to inhibit side reactions.

Because of their high safety, low cost, and high volumetric specific capacity, zinc-ion batteries (ZIBs) are considered promising next-generation energy storage devices, especially given their high potential for large-scale energy storage. Despite these advantages, many problems remain for ZIBs—such as Zn dendrite growth, hydrogen evolution, and Zn anode corrosion—which significantly reduce the coulomb efficiency and reversibility of the battery and limit its cycle lifespan, resulting in much uncertainty in terms of its practical applications. Numerous electrolyte additives have been proposed in recent years to solve the aforementioned problems. This review focuses on electrolyte additives and discusses the different substances employed as additives to overcome the problems by altering the Zn ^2+ solvation structure, creating a protective layer at the anode–electrolyte interface, and modulating the Zn ^2+ distribution to be even and Zn deposition to be uniform. On the basis of the review, the possible research strategies, future directions of electrolyte additive development, and the existing problems to be solved are also described.

Abstract The need for large‐scale electrochemical energy storage devices in the future has spawned several new breeds of batteries in which aqueous zinc ion batteries (AZIBs) have attracted great attention due to their high safety, low cost, and excellent electrochemical performance. In the current research, the dendrite and corrosion caused by aqueous electrolytes are the main problems being studied. However, the research on the zinc metal anode is still in its infancy. We think it really needs to provide clear guidelines about how to reasonably configure the system of AZIBs to realize high‐energy density and long cycle life. Therefore, it is worth analyzing the works on the zinc anode, and several strategies are proposed to improve the stability and cycle life of the battery in recent years. Based on the crystal chemistry and interface chemistry, this review reveals the key factors and essential causes that inhibit dendrite growth and side reactions and puts forward the potential prospects for future work in this direction. It is foreseeable that guiding the construction of AZIBs with high‐energy density and long cycle life in various systems would be quite possible by following this overview as a roadmap.

Rechargeable Zn-based batteries (RZBs) have garnered a great interest and are thought to be among the most promising options for next-generation energy storage technologies due to their low price, high levels of safety, adequate energy density and environmental friendliness. However, dendrite formation during stripping/plating prevents rechargeable zinc-based batteries from being used in real-world applications. Dendrite formation is still a concern, despite the fact that inhibitory strategies have been put up recently to eliminate the harmful effects of zinc dendrites. Thus, in order to direct the strategies for inhibiting zinc dendrite growth, it is vital to understand the formation mechanism of zinc dendrites. Hence, for the practical application of zinc-based batteries, is essential to use techniques that effectively prevent the creation and growth of zinc dendrites. The development and growth principles of zinc dendrites are first made clear in this review. The recent advances of solutions to the zinc dendrite problem are then discussed, including strategies to prevent dendrite growth and subsequent creation as much as possible, reduce the negative impacts of dendrites, and create dendrite-free deposition processes. Finally, the challenges and perspective for the development of zinc-based batteries are discussed.

Abstract Zinc‐ion batteries (ZIBs) have been extensively investigated and discussed as promising energy storage devices in recent years owing to their low cost, high energy density, inherent safety, and low environmental impact. Nevertheless, several challenges remain that need to be prioritized before realizing the widespread application of ZIBs. In particular, the development of zinc anodes has been hindered by many challenges, such as inevitable zinc dendrites, corrosion passivation, and the hydrogen evolution reaction (HER), which have severely limited the practical application of high‐performance ZIBs. This review starts with a systematic discussion of the origins of zinc dendrites, corrosion passivation, and the HER, as well as their effects on battery performance. Subsequently, we discuss solutions to the above problems to protect the zinc anode, including the improvement of zinc anode materials, modification of the anode–electrolyte interface, and optimization of the electrolyte. In particular, this review emphasizes design strategies to protect zinc anodes from an integrated perspective with broad interest rather than a view with limited focus. In the final section, comments and perspectives are provided for the future design of high‐performance zinc anodes.

Abstract Aqueous zinc‐ion batteries (ZIBs) have been intensively investigated as potential energy storage devices on account of their low cost, environmental benignity, and intrinsically safe merits. With the exploitation of high‐performance cathode materials, electrolyte systems, and in‐depth mechanism investigation, the electrochemical performances of ZIBs have been greatly enhanced. However, there are still some challenges that need to be overcome before its commercialization. Among them, the obstinate dendrites, corrosion, and hydrogen evolution reaction (HER) on Zn anodes are critical issues that severely limit the practical applications of ZIBs. To address these issues, various strategies have been proposed, and tremendous progress has been achieved in the past few years. In this article, we analyze the origins and effects of the dendrites, corrosion, and HER on Zn anodes in neutral and mildly acid aqueous solutions at first. And then, a scientific understanding of the fundamental design principles and strategies to suppress these problems are emphasized. Apart from these, this article also puts forward some requirements for the practical applications of Zn anodes as well as several cost‐effective‐modifying strategies. Finally, perspectives on the future development of Zn anodes in aqueous solutions are also briefly anticipated. This article provides pertinent insights into the challenges on anodes for the development of high‐performance ZIBs, which will greatly contribute to their practical applications.

Abstract Rechargeable Zn‐based batteries (RZBs) have attracted much attention and been regarded as one of the most promising candidates for next‐generation energy storage featured with high safety, low costs, environmental friendliness, and satisfactory energy density. The aqueous electrolyte system exhibits great potential to power the future wearable electronics. Apart from the achievements of high capacity cathode and stable electrolyte, the anode suffers from problems of dendrite growth, hydrogen evolution, and passivation with limited attention. The dendrite formation strongly restricts the battery lifespan. Therefore, strategies focused on dendrite suppression are carefully categorized and summarized in this review, including crystallographic orientation manipulation, electric field control, ion flux regulation, and mechanical shield. Each strategy and the detailed approaches are critically dissected. Finally, remaining challenges are emphasized in this review, expecting to supply further research with potential directions to fulfill the high performance of the Zn anodes.