Search Results (49)

Prussian blue analogs (PBAs) are widely recognized as promising candidates for aqueous zinc-ion batteries (AZIBs) due to their stable three-dimensional framework structure. However, their further development is limited by their low specific capacity and unsatisfactory cycling performance, primarily caused by phase transformation during charge–discharge cycles. Herein, we employed a high-entropy strategy to introduce five different metal elements (Fe, Co, Ni, Mn, and Cu) into the nitrogen–coordinated M_a sites of PBAs, forming a high-entropy Prussian blue analog (HEPBA). By leveraging the cocktail effect of the high-entropy strategy, the phase transformation in the HEPBA was significantly suppressed. Consequently, the HEPBA as an AZIB cathode delivered a high reversible specific capacity of 132.1 mAh g⁻¹ at 0.1 A g⁻¹, and showed exceptional cycling stability with 84.7% capacity retention after 600 cycles at 0.5 A g⁻¹. This work provides innovative insights into the rational design of advanced cathode materials for AZIBs. Full article

Rechargeable aqueous zinc-ion batteries (AZIBs) have garnered significant research attention in the energy storage field owing to their inherent safety, cost-effectiveness, and environmental sustainability. Nevertheless, critical challenges associated with zinc anodes—including dendrite formation, hydrogen evolution corrosion, and mechanical degradation—substantially impede their practical implementation. Grain boundary engineering (GBE) emerges as an innovative solution for zinc anode optimization through the precise regulation of grain boundary density, crystallographic orientation, and chemical states in metallic materials. This study comprehensively investigates the fundamental mechanisms and application prospects of GBE in zinc-based anodes, providing pivotal theoretical insights and technical methodologies for designing highly stable electrode architectures. The findings are expected to promote the development of aqueous zinc batteries toward a high energy density and long cycle life. Full article

Layered transition metal dichalcogenides (TMDs) have gained considerable attention as promising cathodes for aqueous zinc-ion batteries (AZIBs) because of their tunable interlayer architecture and rich active sites for Zn²⁺ storage. However, unmodified TMDs face significant challenges, including limited redox activity, sluggish kinetics, and insufficient structural stability during cycling. These limitations are primarily attributed to their narrow interlayer spacing, strong electrostatic interactions, the large ionic hydration radius, and their high binding energy of Zn²⁺ ions. To address these restrictions, an in situ organic polyaniline (PANI) intercalation strategy is proposed to construct molybdenum disulfide (MoS₂)-based cathodes with extended layer spacing, thereby improving the zinc storage capabilities. The intercalation of PANI effectively enhances interplanar spacing of MoS₂ from 0.63 nm to 0.98 nm, significantly facilitating rapid Zn²⁺ diffusion. Additionally, the π-conjugated electron structure introduced by PANI effectively shields the electrostatic interaction between Zn²⁺ ions and the MoS₂ host, thereby promoting Zn²⁺ diffusion kinetics. Furthermore, PANI also serves as a structural stabilizer, maintaining the integrity of the MoS₂ layers during Zn-ion insertion/extraction processes. Furthermore, the conductive conjugated PANI boosts the ionic and electronic conductivity of the electrodes. As expected, the PANI–MoS₂ electrodes exhibit exceptional electrochemical performance, delivering a high specific capacity of 150.1 mA h g⁻¹ at 0.1 A g⁻¹ and retaining 113.3 mA h g⁻¹ at 1 A g⁻¹, with high capacity retention of 81.2% after 500 cycles. Ex situ characterization techniques confirm the efficient and reversible intercalation/deintercalation of Zn²⁺ ions within the PANI–MoS₂ layers. This work supplies a rational interlayer engineering strategy to optimize the electrochemical performance of MoS₂-based electrodes. By addressing the structural and kinetic limitations of TMDs, this approach offers new insights into the development of high-performance AZIBs for energy storage applications. Full article

Aqueous zinc-ion batteries (AZIBs) have emerged as promising candidates for large-scale energy storage due to their inherent safety, low cost, and environmental sustainability. However, in practical applications, AZIBs are constrained by the adverse reactions originating from the zinc anodes, including dendrite formation, hydrogen evolution reaction, corrosion, and passivation, which hinder their large-scale commercialization. Nowadays, alloying strategies have been recognized as efficient approaches to address these limitations and have gained significant attention. By introducing heterogeneous elements into Zn matrices, alloying strategies can suppress dendrite formation and side reactions, modulate the interfacial kinetic process, and enhance electrochemical stability. This review systematically discusses the advantages of alloying for Zn anodes, categorizes key design strategies, such as surface modifications, composite structures, functional alloying, gradient, and layered alloy designs, and meanwhile highlights their performance improvements. Furthermore, we suggest future directions for advanced alloy development, scalable fabrication design, and integrated system optimization. Alloy engineering represents a critical pathway toward high-performance, durable Zn anodes for next-generation AZIBs and other metal-ion batteries. Full article

The increasing demand for safe, cost-effective, and sustainable energy storage solutions has spotlighted aqueous zinc-ion batteries (AZIBs) as promising alternatives to lithium-ion systems. However, the practical deployment of AZIBs remains hindered by dendritic growth, hydrogen evolution, and surface corrosion at the zinc metal anode, which severely compromise electrochemical stability. In this study, we propose an interfacial engineering strategy involving ultrathin diamond-like carbon (DLC) coatings applied to Zn anodes. The DLC films serve as conformal, ion-permeable barriers that mitigate parasitic side reactions and facilitate uniform Zn plating/stripping behavior. Materials characterizations of the DLC layer on the Zn anodes revealed the tunability of sp²/sp³ hybridization and surface morphology depending on DLC thickness. Electrochemical impedance spectroscopy demonstrated a significant reduction in interfacial resistance, particularly in the optimally coated sample (DLC2, ~20 nm), which achieved a favorable balance between mechanical integrity and ionic transport. Symmetric-cell tests confirmed enhanced cycling stability over 160 h, while full-cell configurations with an ammonium vanadate nanofiber-based cathode exhibited superior capacity retention over 900 cycles at 2 A g⁻¹. The DLC2-coated Zn anodes demonstrated the most effective performance, attributable to its moderate surface roughness, reduced disorder, and minimized charge-transfer resistance. These results provide insight into the importance of fine-tuning the DLC thickness and carbon bonding structure for suppressing dendrite formation and enhancing electrochemical stability. Full article

In this study, a Zn(CN)₂–V₂O₃–C composite cathode was synthesized via AC electrophoretic deposition (EPD) and evaluated for application in aqueous zinc-ion batteries (ZIBs). Here, we report for the first time a binder-free Zn(CN)₂–V₂O₃–C composite cathode, using AC-EPD to create an ultrathin architecture optimized for probing the electrode–electrolyte interface without interference from additives or bulk effects. The composite combines Zn(CN)₂ for structural support, V₂O₃ as the redox-active material, and carbon for improved conductivity. X-ray diffraction confirmed the presence of Zn(CN)₂ and V₂O₃ phases, while scanning electron microscopy revealed a uniform, ultrathin film morphology. Electrochemical analysis demonstrated a hybrid charge storage mechanism with a b-value of 0.64, indicating both capacitive and diffusion-controlled contributions. The electrode delivered a high specific capacity (~250 mAh/g at 500 mA/g) with stable cycling performance. These results highlight the potential of metal–organic framework-derived composites for high-performance ZIB cathodes. The composite is especially effective when prepared via AC-EPD, which yields ultrathin, uniform films with strong adhesion and low agglomeration. This enhances energy storage performance and provides a reliable platform for focusing on interfacial charge storage, excluding the effect of binders on electrochemical performance. Full article

Aqueous zinc–ion batteries (AZIBs) have garnered considerable attention owing to their inherent safety, cost-effectiveness, and promising electrochemical performance. However, challenges associated with Zn metal anodes, such as dendrite formation, corrosion, and hydrogen evolution, continue to impede their widespread adoption. To overcome these limitations, a flexible and self-standing composite film anode (denoted ZCN) is engineered from a synergistic combination of Zn powder, nanocellulose, and carbon fiber to serve as a high-performance alternative to conventional Zn foil. These three constituents play the roles of enhancing the active area, improving mechanical properties and electrolyte affinity, and establishing a conductive network, respectively. This innovative design effectively mitigates dendrite growth and suppresses parasitic side reactions, thereby significantly improving the cycling stability of ZCN. As a result, this electrode enables the Zn//Zn cell to offer an ultralong lifespan of 2000 h. And the Zn-MnO₂ battery with ZCN anode demonstrates remarkable performance, realizing over 80% capacity retention after 1000 cycles. This study presents a straightforward, scalable, and cost-effective strategy for the development of dendrite-free metal electrodes, paving the way for durable and high-performance AZIBs. Full article

Despite their inherently lower energy density than lithium-ion batteries (LIBs), aqueous zinc metal batteries (AZMBs) have recently attracted interest as rechargeable energy storage devices due to their low cost and high operational and environmental safety. They are composed of metallic zinc as the anode, an aqueous zinc salt electrolyte and a cathode capable of (de)intercalating Zn²⁺ ions upon its (oxidation) reduction reaction. In this work, we studied a hybrid AZMB in which a dual-ion electrolyte containing both Zn²⁺ and Li⁺ ions was used in conjunction with a Li⁺ ion intercalation cathode, i.e., LiFePO₄ (LFP), one of the most common, reliable, and cheap cathodes for LIBs. In this study, we present evidence that, thanks to its insolubility in water, ethyl cellulose (EC) can be effectively utilized as a binder for cathode membranes in AZMBs. Furthermore, its solubility in alcohol provides a significant advantage in avoiding the use of toxic solvents, contributing to a safer and more environmentally friendly approach to the formulation process. Full article

Aqueous zinc batteries are emerging technologies for energy storage, owing to their high safety, high energy, and low cost. Among them, the development of low-cost and long-cycling cathode materials is of crucial importance. Currently, Zn-ion cathodes are heavily centered on metal-based inorganic materials and carbon-based organic materials; however, the metal–organic compounds remain largely overlooked. Herein, we report the electrochemical performance of metal phthalocyanines, a large group of underexplored compounds, as alternative cathode materials for aqueous zinc batteries. We discover that the selection of transition metal plays a vital role in affecting the electrochemical properties. Among them, iron phthalocyanine exhibits the most promising performance, with a reasonable capacity (~60 mAh g⁻¹), a feasible voltage (~1.1 V), and the longest cycling (550 cycles). The optimal performance partly results from the utilization of zinc chloride “water-in-salt” electrolyte, which effectively mitigates material dissolution and enhances battery performance. Consequently, iron phthalocyanine holds promise as an inexpensive and cycle-stable cathode for aqueous zinc batteries. Full article

MoS₂, a typical transition metal dichalcogenide, features a layered structure, multi-phase transition, and tunable band gap, which is a promising candidate for aqueous zinc-ion batteries (AZIBs). Recent studies have focused on the metastable 1T-MoS₂ phase, which exhibits superior electrical conductivity and electrochemical activity compared to the more stable 2H phase. Herein, a straightforward one-step hydrothermal method was used to synthesize three-dimensional MoS₂/polymer composites (H-MoS₂-PEDOT). Under acidic conditions, the polymerization and intercalation of EDOT molecules in the MoS₂ layers promote the phase transition from 2H to 1T, thereby enhancing its conductivity and electrochemical performance. Additionally, it was found that the intercalated PEDOT and small amounts of water molecules have contributed to enhancing Zn²⁺ ion diffusion and cycle stability. As a result, AZIBs based on the H-MoS₂-PEDOT composite deliver a high specific capacity of 173.6 mAh g⁻¹ at 1 A g⁻¹, maintaining a specific capacity of 116 mAh g⁻¹ and a capacity retention of 82.8% after 1000 cycles at 5 A g⁻¹. Full article

Vanadium-based materials have the advantages of abundant valence states and stable structures, having great application potential as cathode materials in metal-ion batteries. However, their low voltage and vanadium dissolution in traditional water-based electrolytes greatly limit their application and development in aqueous zinc metal batteries (AZMBs). Herein, phosphate- and vanadium-based cathode materials (MnVOPO₄·2H₂O) with stacked layers and few defects were prepared via a condensation reflux method and then combined with a high-concentration electrolyte (21 m LiTFSI + 1 M Zn(CF₃SO₃)₂) to address these limitations. The specific capacity and cycle stability accompanying the stable high voltage of 1.39 V were significantly enhanced compared with those for the traditional electrolyte of 3 M Zn(CF₃SO₃)₂, benefiting from the suppressed vanadium dissolution. The cathode materials of MnVOPO₄·2H₂O achieved a high specific capacity of 152 mAh g⁻¹ at 0.2 A g⁻¹, with a retention rate of 86% after 100 cycles for AZMBs. A high energy density of 211.78 Wh kg⁻¹ was also achieved. This strategy could illuminate the significance of electrolyte modification and provide potential high-voltage cathode materials for AZMBs and other rechargeable batteries. Full article

Aqueous zinc ion batteries (AZIBs) have received a lot of attention in electrochemical energy storage systems for their low cost, environmental compatibility, and good safety. However, cathode materials still face poor material stability and conductivity, which cause poor reversibility and poor rate performance in AZIBs. Herein, a heterogeneous structure combined with cation pre-intercalation strategies was used to prepare a novel CaV₆O₁₆·3H₂O@Ni_0.24V₂O₅·nH₂O material (CaNiVO) for high-performance Zn storage. Excellent energy storage performance was achieved via the wide interlayer conductive network originating from the interlayer-embedded metal ions and heterointerfaces of the two-phase CaNiVO. Furthermore, this unique structure further showed excellent structural stability and led to fast electron/ion transport dynamics. Benefiting from the heterogeneous structure and cation pre-intercalation strategies, the CaNiVO electrodes showed an impressive specific capacity of 334.7 mAh g⁻¹ at 0.1 A g⁻¹ and a rate performance of 110.3 mAh g⁻¹ at 2 A g⁻¹. Therefore, this paper provides a feasible strategy for designing and optimizing cathode materials with superior Zn ion storage performance. Full article

Aqueous zinc−ion batteries (ZIBs) are widely recognized as highly promising energy storage devices because of their inherent characteristics, including superior safety, affordability, eco−friendliness, and various other benefits. However, the significant corrosion of the zinc metal anode, side reactions occurring between the anode and electrolyte, and the formation of zinc dendrites significantly hinder the practical utilization of ZIBs. Herein, we utilized an electrodeposition method to apply a unique hydrous molybdenum oxide (HMoO_x) layer onto the surface of the zinc metal anode, aiming to mitigate its corrosion and side reactions during the process of zinc deposition and stripping. In addition, the HMoO_x layer not only improved the hydrophilicity of the zinc anode, but also adjusted the migration of Zn²⁺, thus facilitating the uniform deposition of Zn²⁺ to reduce dendrite formation. A symmetrical cell with the HMoO_x−Zn anode displayed reduced−voltage hysteresis (80 mV at 2.5 mA/cm²) and outstanding cycle stability after 3000 cycles, surpassing the performance of the uncoated Zn anode. Moreover, the HMoO_x−Zn anode coupled with a γ−MnO₂ cathode created a considerably more stable rechargeable full battery compared to the bare Zn anode. The HMoO_x−Zn||γ−MnO₂ full cell also displayed excellent cycling stability with a charge/discharge−specific capacity of 129/133 mAh g⁻¹ after 300 cycles. In summary, this research offers a straightforward and advantageous approach that can significantly contribute to the future advancements in rechargeable ZIBs. Full article

The upcoming energy transition requires not only renewable energy sources but also novel electricity storage systems such as batteries. Despite Li-ion batteries being the main storage systems, other batteries have been proposed to fulfil the requirements on safety, costs, and resource availability. Moving away from lithium, materials such as sodium, magnesium, zinc, and calcium are being considered. Water-based electrolytes are known for their improved safety, environmentally friendliness, and affordability. The key, however, is how to utilize the negative metal electrode, as using water-based electrolytes with these metals becomes an issue with respect to oxidation and/or dendrite formation. This work studied magnesium, where we aimed to determine if it can be electrochemically deposited in aqueous solutions with alginate-based additives to protect the magnesium. In order to do so, atomic force microscopy was used to research the morphological structure of magnesium deposition at the local scale by using a probe—the tip of a cantilever—as the active electrode, during charging and discharging. The second goal of using the AFM probe technology for magnesium deposition and stripping was an extension of our previous study in which we investigated, for lithium, whether it is possible to measure ion current and perform nonfaradaic impedance measurements at the local scale. The work presented here shows that this is possible in a relatively simple way because, with magnesium, no dendrite formation occurs, which hinders the stripping process. Full article

Aqueous zinc metal batteries (AZMBs) are considered a promising candidate for grid-scale energy storage systems owing to their high capacity, high safety and low cost. However, Zn anodes suffer from notorious dendrite growth and undesirable surface corrosion, severely hindering the commercialization of AZMBs. Herein, a strategy for engineering a dense ZnO coating layer on Zn anodes using the atomic layer deposition (ALD) technique is developed, aiming to improve its long-term cycling stability with fewer Zn dendrites. The surface-modified Zn anode (ZnO@Zn) exhibits an excellent long-cycling life (680 h) and stable coulombic efficiency when being used in a symmetric cell. Moreover, the ZnO@Zn electrode shows a high stability with almost no capacity decay after 1100 cycles at 2C in a full cell using MnO₂ as the cathode. The ZnO coating is conducive to reducing corrosion and the generation of by-products, thus increasing the reversibility of Zn²⁺/Zn stripping/plating. Particularly, density functional theory (DFT) calculation results reveal that the ZnO coating layer could effectively lower the adsorption energy of the Zn(002) plane in ZnO@Zn, inducing the preferential deposition of Zn²⁺ towards the (002) crystal plane with fewer Zn dendrites. The surface ZnO coating protocol provides a promising approach to achieve a dendrite-free Zn anode for stable AZMBs. Full article