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Proton chemistry is becoming a focal point in the development of zinc‐ion energy storage devices due to its swift H+ insertion/extraction kinetics. This characteristic feature confers to electrodes a remarkable power density, rate capability, and prolonged cycling durability. However, the storage mechanism of H+ in electrodes based on covalent‐organic frameworks (COFs) has not been thoroughly investigated. In this work, we introduce an unprecedented concept involving a supramolecular approach based on the design of a benzotrithiophene‐sulfonate COF (COF‐BTT‐SO3H) with remarkable storage capacity for simultaneous insertion and extraction of H+ and Zn2+. The ad hoc positioning of the ‐SO3H groups within the COF‐BTT‐SO3H structure facilitates the formation of a robust H‐bonded network. Through density functional theory calculations and employing in situ and ex situ analyses, we demonstrate that this network functions as a spontaneous proton ion pump leading to enhanced ion‐diffusion kinetics and exceptional rate performance in zinc‐ion energy storage devices. COF‐BTT‐SO3H reveals a high capacity of 294.7 mA h/g (0.1 A/g), a remarkable maximum energy density of 182.5 W h/kg, and power density of 14.8 kW/kg, which are superior to most of the reported COF‐based electrodes or other organic and inorganic electrode materials in Zn2+ energy storage devices. A novel supramolecular approach is introduced using a benzotrithiophene sulfonate imine‐linked covalent‐organic framework (COF‐BTT‐SO3H), enabling remarkable co‐storage of H+ and Zn2+ via three different active sites. COF‐BTT‐SO3H exhibits high capacity of 294.7 mAh/g, outstanding maximum energy density (182.5 Wh/kg), and superior power density (14.8 kW/kg), surpassing most COF‐based electrodes and other materials in Zn2+ energy storage.

Photo‐integrated rechargeable aqueous zinc‐ion batteries (ZIBs)/zinc‐ion capacitors (ZICs) have recently attracted substantial attention as a viable strategy to realize solar to electrochemical energy conversion and storage in a single device. Herein, a timely perspective on the latest advances in photo‐integrated rechargeable ZIBs/ZICs is presented. We first provide a brief introduction for the three different device types and working principles of the photo‐integrated rechargeable ZIB/ZIC devices, including tandem connected photo‐rechargeable hybrid energy systems, photo‐electrode integrated ZIBs, and photo‐rechargeable ZIBs/ZICs. Then, the significant advances in configuration design, materials chemistry, and performance evaluation of photo‐integrated rechargeable ZIBs/ZICs are systematically discussed. At last, the current challenges and future research emphases are suggested, which is to pave the way for the photo‐integrated rechargeable ZIBs/ZICs from laboratory technology to commercialization. This short yet informative perspective aims to evoke more research interests in developing high‐performance photo‐integrated rechargeable ZIBs/ZICs and other hybrid energy systems toward the direct conversion and storage of solar energy to electrochemical energy. The photo‐integrated aqueous rechargeable zinc‐ion batteries (ZIBs)/zinc‐ion capacitors (ZICs) represent a feasible strategy toward direct solar to electrochemical energy conversion and storage. This perspective summarizes the latest progress in various types of photo‐integrated ZIB/ZIC devices. The significant advances in configuration design, materials optimization, and performance evaluation are highlighted.

Since 2020, some new breakthroughs in the field of MXene synthesis scheme such as water‐free etching, HCl‐based hydrothermal etching, halogen etching, and other novel synthesis methods have been proposed. Not only that, the application of MXene in zinc‐ion storage devices has also made great progress in the past 2 years. The understanding of zinc‐ion storage mechanism of MXene has undergone profound changes, and its applications have also become diversified, demonstrating the great potential of MXene for high performance zinc‐ion storage devices. In this review, we have summarized the preparation and synthesis of MXene materials and systematically investigated the progress of MXene in aqueous zinc‐ion storage devices. In particular, for the synthesis of MXene, we added recent reports of conventional synthesis schemes that have been widely reported to help understand their development and combined with recent novel synthesis schemes to provide a distinct partition framework. In addition, for the application of MXene, we discussed the cognitive change of zinc‐ion storage mechanism of MXene and conducted an in‐depth discussion about the design philosophy of MXene and their characteristics. Finally, a comprehensive perspective on the future development of MXene in the synthetic strategy and aqueous zinc‐ion storage applications have been outlined. In the field of electrical energy storage (EES), MXene has made great progress in organic systems, but its low capacity has limited its development in aqueous zinc‐ion batteries. This review summarizes the current main synthesis schemes of MXene and its progress in aqueous zinc‐ion batteries and zinc‐ion capacitors to guide the future design of MXene‐based electrode materials and its application prospects in aqueous zinc‐ion storage devices.

Benefiting from the advantageous features of structural diversity and resource renewability, organic electroactive compounds are considered as attractive cathode materials for aqueous Zn‐ion batteries (ZIBs). In this review, we discuss the recent developments of organic electrode materials for aqueous ZIBs. Although the proton (H+) storage chemistry in aqueous Zn‐organic batteries has triggered an overwhelming literature surge in recent years, this topic remains controversial. Therefore, our review focuses on this significant issue and summarizes the reported electrochemical mechanisms, including pure Zn2+ intercalation, pure H+ storage, and H+/Zn2+ co‐storage. Moreover, the impact of H+ storage on the electrochemical performance of aqueous ZIBs is discussed systematically. Given the significance of H+ storage, we also highlight the relevant characterization methods employed. Finally, perspectives and directions on further understanding the charge storage mechanisms of organic materials are outlined. We hope that this review will stimulate more attention on the H+ storage chemistry of organic electrode materials to advance our understanding and further its application. This review focuses on proton (H+) storage chemistry in aqueous Zn‐organic batteries and summarizes the reported electrochemical mechanisms as well as the impact of H+ storage on the electrochemical performance.

HighlightsA unique dual-ion adsorption mechanism for zinc ion capacitor is enabled by a carbon cathode with defect-rich tissue, dense heteroatom dopant and immense surface area.The active sites on carbon surface for reversible dual-ion adsorption are identified by in-depth characterizations and DFT simulations.The zinc ion capacitor delivers unrivaled combination of high energy and power characteristics. The superb energy, power and cyclability are achieved in multiple cell configurations including coin cell and flexible solid-state pouch-/cable-type cells.Aqueous zinc-based batteries (AZBs) attract tremendous attention due to the abundant and rechargeable zinc anode. Nonetheless, the requirement of high energy and power densities raises great challenge for the cathode development. Herein we construct an aqueous zinc ion capacitor possessing an unrivaled combination of high energy and power characteristics by employing a unique dual-ion adsorption mechanism in the cathode side. Through a templating/activating co-assisted carbonization procedure, a routine protein-rich biomass transforms into defect-rich carbon with immense surface area of 3657.5 m2 g−1 and electrochemically active heteroatom content of 8.0 at%. Comprehensive characterization and DFT calculations reveal that the obtained carbon cathode exhibits capacitive charge adsorptions toward both the cations and anions, which regularly occur at the specific sites of heteroatom moieties and lattice defects upon different depths of discharge/charge. The dual-ion adsorption mechanism endows the assembled cells with maximum capacity of 257 mAh g−1 and retention of 72 mAh g−1 at ultrahigh current density of 100 A g−1 (400 C), corresponding to the outstanding energy and power of 168 Wh kg−1 and 61,700 W kg−1. Furthermore, practical battery configurations of solid-state pouch and cable-type cells display excellent reliability in electrochemistry as flexible and knittable power sources.

Highlights The recent progress about zinc-ion batteries was systematically summarized in detail, including the merits and limits of aqueous and nonaqueous electrolytes, various cathode materials, zinc anode, and solid-state zinc-ion batteries. Current challenges and perspectives to future research directions are also provided. The increasing demands for environmentally friendly grid-scale electric energy storage devices with high energy density and low cost have stimulated the rapid development of various energy storage systems, due to the environmental pollution and energy crisis caused by traditional energy storage technologies. As one of the new and most promising alternative energy storage technologies, zinc-ion rechargeable batteries have recently received much attention owing to their high abundance of zinc in natural resources, intrinsic safety, and cost effectiveness, when compared with the popular, but unsafe and expensive lithium-ion batteries. In particular, the use of mild aqueous electrolytes in zinc-ion batteries (ZIBs) demonstrates high potential for portable electronic applications and large-scale energy storage systems. Moreover, the development of superior electrolyte operating at either high temperature or subzero condition is crucial for practical applications of ZIBs in harsh environments, such as aerospace, airplanes, or submarines. However, there are still many existing challenges that need to be resolved. This paper presents a timely review on recent progresses and challenges in various cathode materials and electrolytes (aqueous, organic, and solid-state electrolytes) in ZIBs. Design and synthesis of zinc-based anode materials and separators are also briefly discussed.

Pre‐intercalation of metal ions into vanadium oxide is an effective strategy for optimizing the performance of rechargeable zinc‐ion battery (ZIB) cathodes. However, the battery long‐lifespan achievement and high‐capacity retention remain a challenge. Increasing the electronic conductivity while simultaneously prompting the cathode diffusion kinetics can improve ZIB electrochemical performance. Herein, N‐doped vanadium oxide (N‐(Zn,en)VO) via defect engineering is reported as cathode for aqueous ZIBs. Positron annihilation and electron paramagnetic resonance clearly indicate oxygen vacancies in the material. Density functional theory (DFT) calculations show that N‐doping and oxygen vacancies concurrently increase the electronic conductivity and accelerate the diffusion kinetics of zinc ions. Moreover, the presence of oxygen vacancies substantially increases the storage sites of zinc ions. Therefore, N‐(Zn,en)VO exhibits excellent electrochemical performance, including a peak capacity of 420.5 mA h g−1 at 0.05 A g−1, a high power density of more than 10 000 W kg−1 at 65.3 Wh kg−1, and a long cycle life at 5 A g−1 (4500 cycles without capacity decay). The methodology adopted in our study can be applied to other cathodic materials to improve their performance and extend their practical applications. N‐doping and oxygen vacancies were introduced on the VO framework by nitridation treatment, which reduced the interaction between the intercalated Zn2+ and the framework, accelerated the migration of Zn ions, and improved the electrochemical performance of the electrode. In addition, the formation mechanism of nitrogen doping and oxygen vacancies were systematically analyzed. The proposed N‐doping mechanism provides a reference for the construction of high‐performance cathode materials.

Highlights3D flower-like architecture assembled by NH4V4O10 nanobelts (3D-NVO) was fabricated.The Zn2+ ion was intercalated into NVO cathode within the interlayer region (NH4V4O10 ↔ ZnxNH4V4O10).The 3D-NVO cathode could deliver a large reversible capacity of 485 mAh g−1 at a current density of 100 mA g−1 for zinc-ion battery.Given the advantages of being abundant in resources, environmental benign and highly safe, rechargeable zinc-ion batteries (ZIBs) enter the global spotlight for their potential utilization in large-scale energy storage. Despite their preliminary success, zinc-ion storage that is able to deliver capacity > 400 mAh g−1 remains a great challenge. Here, we demonstrate the viability of NH4V4O10 (NVO) as high-capacity cathode that breaks through the bottleneck of ZIBs in limited capacity. The first-principles calculations reveal that layered NVO is a good host to provide fast Zn2+ ions diffusion channel along its [010] direction in the interlayer space. On the other hand, to further enhance Zn2+ ion intercalation kinetics and long-term cycling stability, a three-dimensional (3D) flower-like architecture that is self-assembled by NVO nanobelts (3D-NVO) is rationally designed and fabricated through a microwave-assisted hydrothermal method. As a result, such 3D-NVO cathode possesses high capacity (485 mAh g−1) and superior long-term cycling performance (3000 times) at 10 A g−1 (~ 50 s to full discharge/charge). Additionally, based on the excellent 3D-NVO cathode, a quasi-solid-state ZIB with capacity of 378 mAh g−1 is developed.

As a new type of secondary ion battery, aqueous zinc‐ion battery has a broad application prospect in the field of large‐scale energy storage due to its characteristics of low cost, high safety, environmental friendliness, and high‐power density. In recent years, manganese dioxide (MnO2)‐based materials have been extensively explored as cathodes for Zn‐ion batteries. Based on the research experiences of our group in the field of aqueous zinc ion batteries and combining with the latest literature of system, we systematically summarize the research progress of Zn−MnO2 batteries. This article first reviews the current research progress and reaction mechanism of Zn−MnO2 batteries, and then respectively expounds the optimization of MnO2 cathode, Zn anodes, and diverse electrolytes and their effects on battery performance. Additionally, primary challenges related to different components and their respective strategies for mitigating them are discussed, with the ultimate objective of offering comprehensive guidance for the design and fabrication of high‐performance Zn−MnO2 batteries. Finally, the future research and development direction of aqueous Zn−MnO2 batteries with high energy density, high safety and long life is envisioned. In recent years, Zn−MnO2 batteries have attracted more and more attention. This review not only summarizes the battery mechanism under different pH, but also discusses the main challenges encountered and latest developments in anode and cathode materials and various electrolyte materials (liquid, solid and gel), which are crucial for enabling the design of high‐performance batteries. In the end, prospects of the sustainable development of Zn−MnO2 batteries are summarized.

Three‐dimensional (3D) printing has the potential to revolutionize the way energy storage devices are designed and manufactured. In this paper, we explore the use of 3D printing in the design and production of energy storage devices, especially zinc‐ion batteries (ZIBs) and examine its potential advantages over traditional manufacturing methods. 3D printing could significantly improve the customization of ZIBs, making it a promising strategy for the future of energy storage. In particular, 3D printing allows for the creation of complex, customized geometries, and designs that can optimize the energy density, power density, and overall performance of batteries. Simultaneously, we discuss and compare the impact of 3D printing design strategies based on different configurations of film, interdigitation, and framework on energy storage devices with a focus on ZIBs. Additionally, 3D printing enables the rapid prototyping and production of batteries, reducing leading times and costs compared with traditional manufacturing methods. However, there are also challenges and limitations to consider, such as the need for further development of suitable 3D printing materials and processes for energy storage applications. Energy storage device design and production might undergo a revolution thanks to three‐dimensional (3D) printing. In this paper, we investigate the application of 3D printing to the design and manufacture of energy storage devices, particularly zinc‐ion batteries, and we consider its potential advantages and possible challenges.