Aqueous zinc-ion batteries (AZIBs) are one of the promising energy storage systems, which consist of electrode materials, electrolyte, and separator. The first two have been significantly received ample development, while the prominent role of the separators in manipulating the stability of the electrode has not attracted sufficient attention. In this work, a separator (UiO-66-GF) modified by Zr-based metal organic framework for robust AZIBs is proposed. UiO-66-GF effectively enhances the transport ability of charge carriers and demonstrates preferential orientation of (002) crystal plane, which is favorable for corrosion resistance and dendrite-free zinc deposition. Consequently, Zn|UiO-66-GF-2.2|Zn cells exhibit highly reversible plating/stripping behavior with long cycle life over 1650 h at 2.0 mA cm-2, and Zn|UiO-66-GF-2.2|MnO2 cells show excellent long-term stability with capacity retention of 85% after 1000 cycles. The reasonable design and application of multifunctional metal organic frameworks modified separators provide useful guidance for constructing durable AZIBs. 

/pdf/metal-organic-frameworks-functionalized-separators-for-2nfyl7ug.pdf

Metal–Organic Frameworks Functionalized Separators for Robust Aqueous Zinc-Ion Batteries

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

Designing a multifunctional separator with abundant ion migration paths is crucial for tuning the ion transport in rocking-chair-type batteries. Herein, a polydopamine-functionalized PVDF (PVDF@PDA) nanofibrous membrane is designed to serve as a separator for aqueous zinc-ion batteries (AZIBs). The functional groups (OH and NH) in PDA facilitate the formation of ZnO and ZnN coordination bonds with Zn ions, homogenizing the Zn-ion flux and thus enabling dendrite-free Zn deposition. Moreover, the PVDF@PDA separator effectively inhibits the shuttling of V-species through the formation of VO coordination bonds. As a result, the Zn/NH4V4O10 battery with the PVDF@PDA separator exhibits enhanced cycling stability (92.3% after 1000 cycles at 5 A g−1) and rate capability compared to that using a glass fiber separator. This work provides a new avenue to design functionalized separators for high-performance AZIBs. 

A functionalized separator enables dendrite‐free Zn anode via metal‐polydopamine coordination chemistry

Aqueous zinc‐ion batteries (ZIBs) enjoy a good reputation for being safe, affordable to produce, and ecologically friendly due to the use of water‐based electrolytes. The main factors restricting the development of ZIBs, however, are the negative effects of dendrite deposition on the zinc anode and the dissolution of common cathodes such as Mn and V‐based cathodes. Various techniques have been used to address these issues, including regulating the electrolyte concentration or solvation structure, developing a coating or current collector to lessen anode dendrite growth, and improving the structural stability of the cathode. Recently, functionalized separator strategies have gained popularity as effective ways to improve ZIB performance. The use of a functionalized separator is also a practical technique to save costs and increase the volumetric energy density of the battery by substituting a functionalized separator for the usual thick and expensive glass fiber separator. The development of functionalized separators in ZIBs is the subject of ongoing research, and this work presents the most recent findings in a systematic manner, focusing on both the effects and the methods to prepare or modify them. Finally, a brief explanation of the constraints and future potential of current functionalized separator development is provided.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/aenm.202300403

Functionalized Separator Strategies toward Advanced Aqueous Zinc‐Ion Batteries

Ultrathin separators are indispensable to high‐energy‐density zinc‐ion batteries (ZIBs), but their easy failure caused by zinc dendrites poses a great challenge. Herein, 23 µm‐thick functional ultrathin separators (FUSs), realizing superb electrochemical stability of zinc anodes and outstanding long‐term durability of ultrathin separators, are reported. In the FUSs, an ultrathin but mechanically strong nanoporous membrane substrate benefits fast and flux‐homogenized Zn2+ transport, while a metal–organic framework (MOF)‐derived C/Cu nanocomposite decoration layer provides rich low‐barrier zinc nucleation sites, thereby synergistically stabilizing zinc anodes to inhibit zinc dendrites and dendrite‐caused separator failure. Investigation of the zinc affinity of the MOF‐derived C/Cu nanocomposites unravels the high zincophilicity of heteroatom‐containing C/Cu interfaces. Zinc anodes coupled with the FUSs present superior electrochemical stability, whose operation lifetime exceeds 2000 h at 1 mA cm−2 and 600 h at 10 mA cm−2, 40–50 times longer than that of the zinc anodes using glass‐fiber separators. The reliability of the FUSs in ZIBs and zinc‐ion hybrid supercapacitors is also validated. This work proposes a new strategy to stabilize zinc anodes and provides theoretical guidance in developing ultrathin separators for high‐energy‐density zinc‐based energy storage.

Functional Ultrathin Separators Proactively Stabilizing Zinc Anodes for Zinc‐Based Energy Storage

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

Abstract The ripple effect induced by uncontrollable Zn deposition is considered as the Achilles heel for developing high-performance aqueous Zn-ion batteries. For this problem, this work reports a design concept of 3D artificial array interface engineering to achieve volume stress elimination, preferred orientation growth and dendrite-free stable Zn metal anode. The mechanism of MXene array interface on modulating the growth kinetics and deposition behavior of Zn atoms were firstly disclosed on the multi-scale level, including the in-situ optical microscopy and transient simulation at the mesoscopic scale, in-situ Raman spectroscopy and in-situ X-ray diffraction at the microscopic scale, as well as density functional theory calculation at the atomic scale. As indicated by the electrochemical performance tests, such engineered electrode exhibits the comprehensive enhancements not only in the resistance of corrosion and hydrogen evolution, but also the rate capability and cyclic stability. High-rate performance (20 mA cm −2 ) and durable cycle lifespan (1350 h at 0.5 mA cm −2 , 1500 h at 1 mA cm −2 and 800 h at 5 mA cm −2 ) can be realized. Moreover, the improvement of rate capability (214.1 mAh g −1 obtained at 10 A g −1 ) and cyclic stability also can be demonstrated in the case of 3D MXene array@Zn/VO 2 battery. Beyond the previous 2D closed interface engineering, this research offers a unique 3D open array interface engineering to stabilize Zn metal anode, the controllable Zn deposition mechanism revealed is also expected to deepen the fundamental of rechargeable batteries including but not limited to aqueous Zn metal batteries. 

/pdf/3d-artificial-array-interface-engineering-enabling-dendrite-2pbvakgm.pdf

3D Artificial Array Interface Engineering Enabling Dendrite-Free Stable Zn Metal Anode

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

3D Artificial Array Interface Engineering Enabling Dendrite-Free Stable Zn Metal Anode