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Rechargeable aqueous zinc‐ion batteries (AZBs), with their high theoretical capacity, low cost, safety, and environmental friendliness, have risen as a promising candidate for next‐generation energy storage. Despite the fruitful progress in cathode material research, the electrochemical performance of the AZB remains hindered by the physical and chemical instability of the Zn anode. The Zn anode suffers from dendrite growth and chemical reactions with the electrolyte, leading to efficiency decay and capacity loss. Recently, significant effort has been dedicated to regulating the Zn anode. Electrolyte manipulation, including tailoring the salt, additives, or concentration, is a useful strategy as the electrolyte strongly influences the anode's failure processes. It is thus worthwhile to gain an in‐depth understanding of these electrolyte‐dependent regulation mechanisms. With this in mind, this review first outlines the two main issues behind Zn anode failure, dendrite growth, and side reactions. Subsequently, an understanding of the electrolyte tailoring strategy, namely, the influence of the salt, additive, and concentration on the Zn anode, is provided. We conclude by summarizing the future prospects of the Zn metal anode and potential electrolyte‐based solutions. Schematic illustration of Zn anode regulation methods by tailoring the electrolyte.

Die Promotion beschäftigt sich mit der Entwicklung eines Batteriespeichers auf Basis der Zink-Mangandioxid-Batterietechnologie mit wässrigen Elektrolyten (ZMB). Diese Zellchemie bietet Vorteile im Bereich der Sicherheit, der Materialverfügbarkeit, der Kosten und der Umweltverträglichkeit und stellt damit eine vielversprechende Alternative zu den Lithium-Ionen-Batterien im Bereich der stationären Energiespeicherung dar. Auf Basis verschiedener Elektroden-Herstellungsverfahren (Rakelbeschichtung, Elektroabscheidung) können im Rahmen dieser Arbeit reproduzierbare Batterie-Elektroden sowie poröse 3D-Strukturen auf flexibel wählbaren Trägermaterialien hergestellt und erfolgreich zykliert werden. Der Reaktionsmechanismus der Batteriezellchemie wird anhand von pH-Untersuchung im Elektrolyten in Zinksulfat-basierten Elektrolyten tiefgehend untersucht und die wesentlichen Reaktionsmechanismen identifiziert. Die Entwicklung von wässrigen Elektrolyten mit pH-Puffereigenschaften führt zu einer signifikanten Erhöhung des Entladepotentials und damit der möglichen Energiedichte dieser Zellchemie. Die Langzeitstabilität kann ebenfalls signifikant erhöht werden. Abschließend wird ein Batteriemodul-Prototyp konstruiert und erfolgreich hergestellt. Die elektrochemische Charakterisierung bestätigt die Funktionsfähigkeit des Batteriemodul-Konzepts. Die techno-ökonomische Bewertung zeigt dabei ein hohes Kostenreduktionspotential gegenüber dem Stand der Technik bei der Lithium-Ionen-Batterietechnologie.

From basic research to industry process, battery energy storage systems have played a great role in the informatization, mobility, and intellectualization of modern human society. Some potential systems such as Li, Na, K, Mg, Zn, and Al secondary batteries have attracted much attention to maintain social progress and sustainable development. As one of the components in batteries, electrolytes play an important role in the upgrade and breakthrough of battery technology. Since room‐temperature ionic liquids (ILs) feature high conductivity, nonflammability, nonvolatility, high thermal stability, and wide electrochemical window, they have been widely applied in various battery systems and show great potential in improving battery stability, kinetics performance, energy density, service life, and safety. Thus, it is a right time to summarize these progresses. In this review, the composition and classification of various ILs and their recent applications as electrolytes in diverse metal‐ion batteries (Li, Na, K, Mg, Zn, Al) are outlined to enhance the battery performances. This manuscript reviews the classification of ionic liquids, and their potential application as electrolytes in metal‐ion batteries (Li, Na, K, Mg, Zn, Al). Their merits of nonflammable property, thermal stability, and high safety suggest that they could be a promising solution to realize high safety and high energy density for next generational battery systems.

Aqueous zinc‐ion batteries (AZIBs) stand out among many monovalent/multivalent metal‐ion batteries as promising new energy storage devices because of their good safety, low cost, and environmental friendliness. Nevertheless, there are still many great challenges to exploring new‐type cathode materials that are suitable for Zn2+ intercalation. Vanadium‐based compounds with various structures, large layer spacing, and different oxidation states are considered suitable cathode candidates for AZIBs. Herein, the research advances in vanadium‐based compounds in recent years are systematically reviewed. The preparation methods, crystal structures, electrochemical performances, and energy storage mechanisms of vanadium‐based compounds (e.g., vanadium phosphates, vanadium oxides, vanadates, vanadium sulfides, and vanadium nitrides) are mainly introduced. Finally, the limitations and development prospects of vanadium‐based compounds are pointed out. Vanadium‐based compounds as cathode materials for AZIBs are hoped to flourish in the coming years and attract more and more researchers' attention. The research advances in vanadium‐based compounds in recent years are systematically reviewed. The preparation methods, crystal structures, electrochemical performances, and energy storage mechanisms of vanadium‐based compounds are mainly introduced. Finally, the limitations and development prospects of vanadium‐based compounds are pointed out.

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. A systematic and detailed summary of the research progress on zinc ion battery anodes is presented, including the causes of zinc dendrites, corrosion passivation and hydrogen evolution reaction on zinc anodes along with the existing strategies. Perspectives are provided for the future design of high‐performance zinc anodes.

Aqueous rechargeable zinc‐metal‐based batteries are an attractive alternative to lithium‐ion batteries for grid‐scale energy‐storage systems because of their high specific capacity, low cost, eco‐friendliness, and nonflammability. However, uncontrollable zinc dendrite growth limits the cycle life by piercing the separator, resulting in low zinc utilization in both alkaline and mild/neutral electrolytes. Herein, a polyacrylonitrile coating layer on a zinc anode produced by a simple drop coating approach to address the dendrite issue is reported. The coating layer not only improves the hydrophilicity of the zinc anode but also regulates zinc‐ion transport, consequently facilitating the uniform deposition of zinc ions to avoid dendrite formation. A symmetrical cell with the polymer‐coating‐layer‐modified Zn anode displays dendrite‐free plating/stripping with a long cycle lifespan (>1100 h), much better than that of the bare Zn anode. The modified zinc anode coupled with a Mn‐doped V2O5 cathode forms a stable rechargeable full battery. This method is a facile and feasible way to solve the zinc dendrite problem for rechargeable aqueous zinc‐metal batteries, providing a solid basis for application of aqueous rechargeable Zn batteries. A polyacrylonitrile (PAN)Z coating layer is employed to confine zinc dendrite growth for rechargeable aqueous zinc‐based batteries. The cyclability and Coulombic efficiency of the zinc anode porous PAN coating layer show that the polymer coating film is a feasible artificial membrane for a dendrite‐free zinc anode.

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 polydopamine‐functionalized PVDF (PVDF@PDA) nanofibrous membrane is designed as a separator for aqueous zinc‐ion batteries. The PVDF@PDA separator homogenizes the Zn‐ion flux distribution to achieve the dendrite‐free Zn deposition via the metal‐PDA coordination chemistry. Moreover, the PVDF@PDA separator inhibits the shuttle of V‐species. Benefiting from the separator, the Zn/NH4V4O10 full cell retains 92.3% capacity after 1000 cycles at 5 A g−1.

Rechargeable aqueous zinc‐ion batteries (ZIBs) show promise for use in energy storage. However, the development of ZIBs has been plagued by the limited cathode candidates, which usually show low capacity or poor cycling performance. Here, a reversible Zn//(Na,Mn)V8O20·nH2O system is reported, the introduction of manganese (Mn) ions in NaV8O20 to form (Na,Mn)V8O20 exhibits an outstanding electrochemical performance with a capacity of 377 mA h g−1 at a current density of 0.1 A g−1. Through experimental and theoretical results, it is discovered that the outstanding performance of (Na,Mn)V8O20·nH2O is ascribed to the Mn2+/Mn3+‐induced high electrical conductivity and Na+‐induced fast migration of Zn2+. Other cathode materials derived from (Na,Mn)V8O20·nH2O by substituting Mn with Fe, Co, Ni, Ca, and K are explored to confirm the unique advantages of transition metal ions. With an increase in Mn content in NaV8O20, (Na0.33,Mn0.65)V8O20 ·nH2O can deliver a reversible capacity of 150 mA h g−1 and a capacity retention of 99% after 1000 cycles, which may open new opportunities for the development of high‐performance aqueous ZIBs. Mn‐doped NaV8O20 is synthesized via a one‐step hydrothermal reaction. The Mott–Schottky plots, Tafel curves and calculation results are given to explain the improved cycling performance of Mn‐doped NaV8O20. Other cathode materials derived from (Na,Mn)V8O20·nH2O by substituting Mn with Fe, Co, Ni, Ca, and K are explored to confirm the unique advantages of transition metal ions in NaV8O20.

Battery technology is constantly changing, and the concepts and applications of these changes are rapidly becoming increasingly more important as more and more industries and individuals continue to make \"greener\" choices in their energy sources. As global dependence on fossil fuels slowly wanes, there is a heavier and heavier importance placed on cleaner power sources and methods for storing and transporting that power. Battery technology is a huge part of this global energy revolution. Zinc batteries are an advantageous choice over lithium-based batteries, which have dominated the market for years in multiple areas, most specifically in electric vehicles and other battery-powered devices. Zinc is the fourth most abundant metal in the world, which is influential in its lower cost, making it a very attractive material for use in batteries. Zinc-based batteries have been around since the 1930s, but only now are they taking center stage in the energy, automotive, and other industries.

Zn metal holds grand promise as the anodes of aqueous batteries for grid‐scale energy storage. However, the rampant zinc dendrite growth and severe surface side reactions significantly impede the commercial implementation. Herein, a universal Zn‐metal oxide Ohmic contact interface model is demonstrated for effectively improving Zn plating/stripping reversibility. The high work function difference between Zn and metal oxides enables the building of an interfacial anti‐blocking layer for dendrite‐free Zn deposition. Moreover, the metal oxide layer can function as a physical barrier to suppress the pernicious side reactions. Consequently, the proof‐of‐concept CeO2‐modified Zn anode delivers ultrastable durability of over 1300 h at 0.5–5 mA cm−2 and improved Coulombic efficiency, the feasibility of which is also evidenced in MoS2//Zn full cells. This study enriches the fundamental comprehension of Ohmic contact interfaces on the Zn deposition, which may shed light on the development of other metal battery anodes. A universal Zn‐metal oxide Ohmic contact interface model is demonstrated to effectively enable improved Zn2+ diffusion kinetics and a reduced Zn nucleation barrier, thus achieving a dendrite‐free and side‐reaction‐free Zn deposition chemistry for significant improvement of the electrochemical performance in both the symmetric cells and full cells.