The hydrophobic internal cavity and hydrophilic external surface of cyclodextrins (CDs) render promising electrochemical applications. Here, we report a comparative and mechanistic study on the use of CD molecules (α-, β-, and γ-CD) as electrolyte additives for rechargeable Zn batteries. The addition of α-CD in aqueous ZnSO4 solution reduces nucleation overpotential and activation energy of Zn plating and suppresses H2 generation. Computational, spectroscopic, and electrochemical studies reveal that α-CD preferentially adsorbs in parallel on the Zn surface via secondary hydroxyl groups, suppressing water-induced side reactions of hydrogen evolution and hydroxide sulfate formation. Additionally, the hydrophilic exterior surface of α-CD with intense electron density simultaneously facilitates Zn2+ deposition and alleviates Zn dendrite formation. A formulated 3 M ZnSO4 + 10 mM α-CD electrolyte enables homogenous Zn plating/stripping (average Coulombic efficiency ∼ 99.90%) at 1 mA cm-2 in Zn|Cu cells and a considerable capacity retention of 84.20% after 800 cycles in Zn|V2O5 full batteries. This study provides insight into the use of supramolecular macrocycles to modulate and enhance the interface stability and kinetics of metallic anodes for aqueous battery chemistry.

Boosting the Kinetics and Stability of Zn Anodes in Aqueous Electrolytes with Supramolecular Cyclodextrin Additives.

Aqueous Zn-ion batteries (AZIBs) have attracted much attention due to their excellent safety, cost-effectiveness, and eco-friendliness thereby being considered as one of the most promising candidates for large-scale energy storage. Zn metal anodes with a high gravimetric/volumetric capacity are indispensable for advanced AZIBs. However, pristine Zn metal anodes encounter severe challenges in achieving adequate cycling stability, including dendrite growth, hydrogen evolution reaction, self-corrosion, and by-product formation. Because all these reactions are closely related to the electrolyte/Zn interface, the subtle interface engineering is important. Many strategies targeted to the interface engineering have been developed. In this review, a timely update on these strategies and perspectives are summarized, especially focusing on the controllable synthesis of Zn, Zn surface engineering, electrolyte formulation, and separator design. Furthermore, the corresponding internal principles of these strategies are clarified, which is helpful to help seek for new strategies. Finally, the challenges and perspectives for the future development of practical AZIBs are discussed, including the conducting of in advanced in situ testing, unification of battery models, some boundary issues, etc. This review is expected to guide the future development and provi beacon light direction for aqueous zinc ion batteries. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/aenm.202300606

Recent Progress on Zn Anodes for Advanced Aqueous Zinc‐Ion Batteries

High-Donor Electrolyte Additive Enabling Stable Aqueous Zinc-Ion Batteries

Sluggish transport kinetics and rapid dendrite growth are considered the main obstacles that impair the performance of Zn metal batteries. This work has developed a unique strategy of dual‐interface engineering (DIE) to design the separator as efficient ions transport modulator. The dual function of spontaneous polarization effect and high zincophilicity of BaTiO3 (BTO) is revealed by combining the theoretical and experimental studies. Benefiting from the decoration of BTO on glass fiber and well filling of the surface interspace, the DIE‐modified separator can not only effectively capture and accelerate Zn2+ transport between the fiber–electrolyte interface, but also redistribute the ions transport into homogenization in the separator–anode interface. Therefore, the modified Zn anodes perform highly reversible Zn plating/stripping with ultrahigh cumulative capacity even up to 9500 mAh cm−2 at the high current density of 10 mA cm−2. Meanwhile, the modified Zn‐MnO2 battery can retain a specific capacity of 108 mAh g−1 after 1800 cycles at 1 A g−1. Furthermore, the capacity retention of the battery also can be improved from 37.5% up to 115% at 0.2 A g−1 after 100 cycles. Such a novel concept for separator engineering provides a new perspective to enable ultra‐stable Zn metal anodes and high‐performance Zn metal batteries.

Novel Concept of Separator Design: Efficient Ions Transport Modulator Enabled by Dual‐Interface Engineering Toward Ultra‐Stable Zn Metal Anodes

Stabilization of Zn anode via a multifunctional cysteine additive

Hexaoxacyclooctadecane induced interfacial engineering to achieve dendrite-free Zn ion batteries

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Hexaoxacyclooctadecane induced interfacial engineering to achieve dendrite-free Zn ion batteries