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.

Interfacial Double‐Coordination Effect Guiding Uniform Electrodeposition for Reversible Zinc Metal Anode

Dual-Function Electrolyte Additive Enabling Simultaneous Electrode Interface and Coordination Environment Regulation for Zinc-Ion Batteries

Hydrogen Bond Acceptor Lined Hydrogel Electrolyte toward Dendrite-Free Aqueous Zn Ion Batteries with Low Temperature Adaptability

The practical application of aqueous zinc-ion batteries (AZIBs) is limited due to the inherent side reactions and dendrites growth of Zn anode. Herein, we propose a solution to the issue...

Highly Reversible and Stable Zn Metal Anodes Realized by Trifluoroacetamide Electrolyte Additive

The Zn dendrite issue, which is closely related to the creation of the space-charge region upon local anion depletion during cycling, has plagued the practical applications of aqueous Zn metal batteries (ZMBs). Herein, we propose a Kevlar-derived hydrogel (KevlarH) electrolyte with immobilized anions to diminish the space-charge layer effect. SO42– anions are strongly tethered to amide groups of polymer chains, which mitigates the concentration polarization of interfacial Zn2+ ions by preventing the anion depletion. Furthermore, the relatively weak interaction between Zn2+ cations and carbonyl groups can redistribute Zn2+-ion flux without sacrificing the ion diffusion rate. The synergistic “zincophilic” and “anionphilic” building blocks enable dendrite-free Zn deposition behavior and suppressed side reactions, thereby extending the lifespan of a Zn metal anode up to 3500 h with an ultrahigh Coulombic efficiency of 99.87%. Importantly, the KevlarH electrolyte can be directly used to assemble high-voltage bipolar ZMBs and break the 2 V barrier in aqueous ZMBs. 

Diminishing Space-Charge Layer Effect of Zinc Anodes by an Anion-Immobilized Electrolyte Membrane

In situ construction of zinc-rich polymeric solid–electrolyte interface for high-performance zinc anode

2-Methyl Imidazole Electrolyte Additive Enabling Ultra-Stable Zn Anode

Zn-ion batteries are re-evaluated as a potential choice to address the safety issue and cost concerns of current energy storage systems. Unfortunately, further application is severely hindered by low coulombic efficiency and poor cycle life, which are caused by the undesirable dendrite growth and side reactions on metal Zn anode. Herein, ethylenediaminetetraacetic acid (EDTA) is employed as an electrolyte additive to solve the problem. The functional groups of EDTA adsorption layer on Zn foil results in refined grains by providing abundant nucleation sites for initial deposition and further induces uniform and flat Zn deposition without dendrites. Moreover, the chelation of EDTA with Zn2+ changes the coordination environment of hydrated Zn2+ and suppresses the side reactions. The smooth deposition of Zn endows the Zn anodes with super stability in both symmetric cells and Zn–V2O5 full cells. This work provides a simple and feasible approach for solving anode issues in high-performance and safe Zn-ion batteries. 

Toward Stable Zinc-Ion Batteries: Use of a Chelate Electrolyte Additive for Uniform Zinc Deposition

This work presents the first example of utilization of amphiphilic block copolymer PCL-PEG-PCL as a stationary phase for capillary gas chromatographic (GC) separations. The PCL-PEG-PCL capillary column fabricated by static coating provides a high column efficiency of 3951 plates/m for n-dodecane at 120 °C. McReynolds constants and Abraham system constants were also determined in order to evaluate the polarity and possible molecular interactions of the PCL-PEG-PCL stationary phase. Its selectivity and resolving capability were investigated by using a complex mixture covering analytes of diverse types and positional, structural, and cis-/trans-isomers. Impressively, it exhibits high resolution performance for aliphatic and aromatic isomers with diverse polarity, including those critical isomers such as butanol, dichlorobenzene, dimethylnaphthalene, xylenol, dichlorobenzaldehyde, and toluidine. Moreover, it was applied for the determination of isomer impurities in real samples, suggesting its potential for practical use. The superior separation performance demonstrates the potential of PCL-PEG-PCL and related block copolymers as stationary phases in GC and other separation technologies.

Amphiphilic Block Copolymer PCL-PEG-PCL as Stationary Phase for Capillary Gas Chromatographic Separations.

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. 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. Zinc ion batteries are considered as potential energy storage devices due to their advantages of low-cost, high-safety, and high theoretical capacity. However, dendrite growth and chemical corrosion occurring on Zn anode limit their commercialization. These problems can be tackled through the optimization of the electrolyte. However, the screening of electrolyte additives using normal electrochemical methods is time-consuming and labor-intensive. Herein, a fast and simple method based on the digital holography is developed. It can realize the in situ monitoring of electrode/electrolyte interface and provide direct information concerning ion concentration evolution of the diffusion layer. It is effective and time-saving in estimating the homogeneity of the deposition layer and predicting the tendency of dendrite growth, thus able to value the applicability of electrolyte additives. The feasibility of this method is further validated by the forecast and evaluation of thioacetamide additive. Based on systematic characterization, it is proved that the introduction of thioacetamide can not only regulate the interficial ion flux to induce dendrite-free Zn deposition, but also construct adsorption molecule layers to inhibit side reactions of Zn anode. Being easy to operate, capable of in situ observation, and able to endure harsh conditions, digital holography method will be a promising approach for the interfacial investigation of other battery systems.

Thioacetamide Additive Homogenizing Zn Deposition Revealed by In Situ Digital Holography for Advanced Zn Ion Batteries

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