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The cost‐effectiveness and environmentally friendly nature of aqueous zinc‐ion batteries (ZIBs) have garnered significant attention. Nevertheless, obstacles such as dendrite growth and side reactions have hindered their practical application. Here, an alkaline earth metal ion, strontium ions (Sr2+), is chosen as a dual‐functional electrolyte additive to improve the reversibility of ZIBs. Importantly, Sr2+ ions adsorb on the anode surface, creating a dynamic electrostatic shield layer, thus regulating the Zn2+ deposition behavior and suppressing side reactions. Meanwhile, Sr2+ ions prefer to adsorb on (002) and (110) planes of Zn, thus inducing the preferential deposition of (100) crystal plane and achieving dendrite‐free zinc anode. Consequently, the assembled Zn||Zn symmetric battery delivers an ultralong lifespan of 3500 h, and the Zn||Ti asymmetric battery shows a superior Coulombic efficiency of 99.8% for Zn stripping/plating at 2 mA cm−2. Further, the Zn||NH4V4O10 battery presents an excellent retention of 97.7% over 800 cycles under 2 A g−1. This research introduces a novel alkaline earth metal ion electrolyte additive and establishes its persistent dynamic electrostatic shielding effect and preferentially oriented (100) plane plating, ensuring dendrite‐free zinc deposition. These findings chart a course for further exploration of unexplored alkaline earth elements in enhancing metal battery technologies. [ABSTRACT FROM AUTHOR]

Constructing artificial solid electrolyte interface on the Zn anode surface is recognized as an appealing method to inhibit zinc dendrites and side reactions, whereas the current techniques are complex and time‐consuming. Here, a robust and zincophilic zinc tungstate (ZnWO4) layer has been in situ constructed on the Zn anode surface (denoted as ZWO@Zn) by an ultrafast chemical solution reaction. Comprehensive characterizations and theoretical calculations demonstrate that the ZWO layer can effectively modulate the interfacial electric field distribution and promote the Zn2+ uniform diffusion, thus facilitating the uniform Zn2+ nucleation and suppressing zinc dendrites. Besides, ZWO layer can prevent direct contact between the Zn/water and increase the hydrogen evolution reaction overpotential to eliminate side reactions. Consequently, the in situ constructed ZWO layer facilitates remarkable reversibility in the ZWO@Zn||Ti battery, achieving an impressive Coulombic efficiency of 99.36 % under 1.0 mA cm−2, unprecedented cycling lifespan exceeding 1800 h under 1.0 mA cm−2 in ZWO@Zn||ZWO@Zn battery, and a steady and reliable operation of the overall ZWO@Zn||VS2 battery. The work provides a simple, low cost, and ultrafast pathway to crafting protective layers for driving advancements in aqueous zinc‐metal batteries. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries (AZIBs) are highly promising for grid‐scale energy storage due to their high‐safety and low‐cost characteristics. Nevertheless, the progress in AZIBs has been impeded due to challenges encompassing corrosion, hydrogen evolution reaction, and the formation of dendrites on Zn anodes. These issues arise from the decomposition of active water molecules in the Zn2+ solvation structure in the electrolyte. Various strategies have been proposed to regulate the electrode/electrolyte interface to effectively address these problems. In spite of remarkable headway, an inadequacy of comprehensive studies addressing the mechanisms and evolutionary dynamics of the electrode/electrolyte interface is evident within scientific literature. This overview aims to provide a comprehensive overview of the strategies for regulating the electrode/electrolyte interface, focusing on dendrite‐free and side reactions‐suppressed AZIBs. These strategies include the introduction of metal ion additives, inorganic additives, surfactant additives, polymer additives and organic additives. Furthermore, a detailed examination is made on the effects and underlying mechanisms associated with modifying the electrolyte at the interface between the electrode and electrolyte. Moreover, an appraisal is provided on the performance metrics of diverse strategies and prospective research directions are recommended as well. [ABSTRACT FROM AUTHOR]

Aqueous zinc-ion battery (ZIBs) has garnered considerable attention for its economic, safe, and high-energy-density characteristics. However, impediments, such as undesirable side reactions and uneven dendrites, have restrained its progress. To overcome these challenges, diverse strategies have been proposed, with electrolyte modification emerging as a preferred approach due to its simplicity and practicality. Here, we introduced ethylenediamine (EDA) as an additive into ZnSO4 solution. Through a combination of theoretical calculations and experimental validation, we have demonstrated that EDA plays a pivotal role in reducing the free active H2O by modifying the solvation structure of Zn2+, thereby enhancing the stability of the zinc anode. Upon the incorporation of EDA into the ZnSO4 electrolyte, the symmetrical battery assembled showcased remarkable cycling stability, surpassing 1500 h at 1 mA cm−2 and 1 mAh cm−2. Notably, the coulombic efficiency and durability of Zn/Ti asymmetric batteries under identical conditions were significantly improved. Furthermore, the positive impact of EDA extended to Zn/NH4V4O10 full batteries assembled using the modified electrolyte, providing robust evidence of the practical efficacy of EDA additive. This study not only highlights the transformative potential of EDA in enhancing the stability and performance of ZIBs but also reinforces its practicality for advanced energy storage applications. [ABSTRACT FROM AUTHOR]

The long‐term reversible plating/stripping of Zn metal anode is a critical aspect within aqueous zinc‐ion batteries (ZIBs). However, it is limited by uncontrolled electrodeposition and side reactions occurring at the anode/electrolyte interface. Guided by the metal‐coordination chemistry, a novel additive, sodium diphenylamine sulfonate (DASS), is added into ZnSO4 electrolyte to guide stably invertible zinc deposition. Theoretical calculations and experimental results reveal that the DASS can adsorbed on the Zn anode surface due to the strong double coordination effect between N, S sites and Zn (Zn─N, Zn─S), and this adsorbed DASS layer can not only prevent the intimate contact between H2O and anode to inhibit interfacial side reactions, but also guide the 3D Zn2+ion diffusion and uniform electrodeposition to inhibit zinc dendrites. Consequently, the DASS additive enables an ultra‐long stable cycling up to 2400 h at 1 mA cm−2 (1 mAh cm−2), even at an ultra‐high current density of 20 mA cm−2, a stable cycling of 250 h is demonstrated, highlighting the reliable coordination effect at the anode/electrolyte interface. This study offers a new perspective on the interfacial double‐coordination effect for achieving highly reversible Zn metal anodes in aqueous rechargeable zinc‐ion batteries. [ABSTRACT FROM AUTHOR]

The main obstacle for developing aqueous zinc-ion batteries (ZIBs) with long-term stability lies in the suppression of side reactions and zinc dendrites, which are derived from decomposition of active water molecules belonging to Zn2+ solvation layer in the electrolyte. Herein, an inorganic colloidal electrolyte composed of lithium magnesium silicate and zinc sulfate (LMS+ZSO) is utilized to improve the reversibility of Zn plating/stripping behavior for high-performance ZIBs. As revealed by the experimental and theoretical results, LMS's superior adsorption capacity for water molecules modulates the Zn2+ solvation structure via converting the free water molecules into adsorbed water of LMS and weakening the electrostatic coupling of anions and cations, thus restraining the corrosion, hydrogen evolution reaction and by-products. Concomitantly, the LMS lowers the energy barrier of de-solvation process to promote the Zn2+ ions transfer kinetics and induce the homogeneous deposition, thus inhibiting the dendrites formation. Consequently, the cycling stability of symmetric battery and zinc-based full battery are significantly boosted with LMS+ZSO electrolyte. This reasonable and effective strategy offers a promising prospect for developing long life ZIBs. [Display omitted] • Lithium magnesium silicate (LMS) can regulate the solvation structure via adsorbing the free water molecules. • LMS in electrolyte can lower the energy barrier of de-solvation process and increase the Zn2+ transfer number. • The inorganic colloidal electrolyte (LMS+ZSO) can suppress the dendrites growth and by-products. • The cycling stability of symmetric battery and zinc-based full battery are boosted via LMS+ZSO electrolyte. [ABSTRACT FROM AUTHOR]

The artificial interface layer on the Zn anode can effectively suppress by-product formation and dendrite growth, playing a crucial role in achieving high-rate and long-life aqueous zinc-ion batteries. However, the current galvanizing mode, where plating occurs separately below or inside the interface layer after its introduction, poses risks of detachment or swelling during cycling, limiting practical applications. In this study, we fabricate a three-dimensional porous NiO interface layer with enhanced anode dynamics that forms a Schottky contact with the zinc substrate. Through the synergistic effect of this excellent structure and Schottky barrier, zinc is rapidly and uniformly plated both inside and below the interface layer simultaneously. Symmetrical cells based on NiO@Zn exhibit exceptional stability over 10,000 cycles at an ultrahigh current density of 20 mA cm−2. Furthermore, NiO@Zn||MnO 2 full cells deliver a capacity of 228 mAh g−1 and retain 94% of their initial capacities for 500 cycles at a density of 1 A g−1. This work not only presents highly reversible zinc anodes but also proposes an innovative galvanizing model. • A novel strategy combining Schottky contact and three-dimensional porous structure to improve galvanizing uniformity. • Stable dendrite free stripping/plating was successfully achieved at a current density of 20 mA cm−2 for 10,000 cycles. • An innovative galvanizing model was proposed, wherein zinc is simultaneously plated both inside and below the interface layer. [ABSTRACT FROM AUTHOR]

Aqueous zinc-ion batteries (ZIBs) hold great promise in electrochemical applications due to their cost-effectiveness and high safety. However, the practical utilization of ZIBs faces challenges from detrimental zinc dendrite formation and side reactions, which adversely impact their cycling lifespan and electrochemical stability. In this research, we proposed a commonly available and cost-effective organic solvent, N, N-dimethylformamide (DMF), as an electrolyte additive to stabilize Zn anode. According to the experimental characterizations and theoretical calculations, DMF exhibits a strong interaction with Zn2+ ions, which can not only regulate the Zn2+ solvation structure to mitigate side reactions, but also promote the uniform deposition of Zn2+ to suppress Zn dendrites. Hence, the symmetrical Zn/Zn cell assembled with a mixed electrolyte of ZnSO 4 and DMF (ZSO+DMF) demonstrated an impressive cycle lifespan of up to 1600 h under a current density of 1 mA cm−2. Moreover, the coulombic efficiency (CE) of Zn/Ti batteries operating at 1 mA cm−2 was significantly improved to 98.36%, surpassing that in ZnSO 4 electrolytes (95.34%). Additionally, the performance of Zn/VO 2 cells further validates the effectiveness of the DMF additive. These findings highlight the potential of DMF as a valuable electrolyte additive to enhance the electrochemical performance and cycling stability of Zn-based batteries, offering a practical and cost-efficient approach to advancing the development of ZIBs. [Display omitted] • A comment used organic solvent has been utilized as electrolyte additive. • DMF shows strong interaction with Zn2+ ions and regulate the Zn2+ solvation sheath. • DMF additive can inhibit the harmful zinc dendrites and side reactions. • DMF additive can boost the electrochemical performance of full zinc-ion batteries. [ABSTRACT FROM AUTHOR]

Zinc-ion batteries (ZIBs) are promising energy storage system owing to the low cost and high safety features. As the most-used anode material, zinc metal always encounters poor coulombic efficiency (CE) and cycling stability, because of the serious zinc dendrite and harmful side reactions on Zn surface. Here, a solid-phase non-adhesive homogeneous Nano-Si layer has been embedded on the Zn surface (Zn-Si) via an ultra-facile grinding method. The Nano-Si layer can regulate an even electric field distribution to achieve a homogeneous zinc deposition, and it also can greatly lower the charge transfer resistance and nucleation energy barrier of Zn2+ to facilitate the zinc deposition, thus achieving a dendrites-free and long-life Zn anode. Encouragingly, the zinc symmetrical battery with Zn-Si anode delivers a superior CE of 99.6 % in 1000 cycles under 5 mA cm−2, and a stable cycle lifespan of 3600 h under 1 mA cm−2 with much lower polarization potential (42 mV), outperforming the symmetrical battery with pure Zn anode (455 h, 59 mV) and various previously reported strategies. Additionally, the effectiveness of Nano-Si layer is further proved in the Zn-Si/MnO 2 battery, which presents a greatly improved capacity retention and cycling performance. [Display omitted] • Zn-Si anode has been prepared via a facile grinding process with sandpaper and Nano-Si powder. • Zn-Si anode shows lower the charge transfer resistance and nucleation energy overpotential. • Zn-Si can prevent the formation of zinc dendrites and by-products. • Zn-Si anode can further improve the electrochemical performance of full battery. [ABSTRACT FROM AUTHOR]