锁甲基纤维素改善锌电池负极

No abstract available

No abstract available

No abstract available

No abstract available

To address interfacial challenges of the zinc anode in aqueous zinc‐ion batteries (AZIBs), including dendrite growth and by‐product formation, a carbon microspheres/carboxymethyl cellulose (CMC) composite coating (CCZn) is developed on the zinc foil. The composite coating achieves effective regulation of zinc deposition behavior through the synergistic effect of carbon microspheres and CMC. Specifically, the abundant oxygen‐containing functional groups in the coating can form coordination bonds with the zinc substrate to enhance the mechanical stability of the anode. The CMC molecular chains fix the carbon microspheres through a hydrogen bond network to build a 3D stable framework, enabling rapid ion transport. Meanwhile, the rich carboxylate groups in the coating can promote the desolvation process of Zn(H 2 O) 6 2+ , accelerating the kinetics of the zinc ion deposition process. In addition, the presence of the coating can cover the original surface defects of raw Zn (RZn), thereby uniformizing the electric field distribution on the electrode surface to inhibit dendrite growth. Consequently, the CCZn symmetric cell exhibits a cycle life 18 times longer than the RZn cell at 0.8 and 0.8 mAh cm −2 , highlighting its exceptional cycling durability. This work provides a novel interfacial engineering strategy to address zinc deposition challenges in AZIBs.

Aqueous Zn‐ion batteries (AZIBs) show great potential in new energy storage devices due to low cost, inherent safety, and environmental friendliness. However, the severe dendrites and side reactions on the anode greatly constrain their practical application. Herein, a novel colloidal electrolyte composed of ZnSO4 and sodium carboxymethyl cellulose (CMC‐Na) has been developed for inhibiting dendrite growth on Zn anode. Molecular dynamics (MD) simulation confirms that CMC‐Na alters the electric double layer (EDL) structure of Zn anode surface to reduce the content of water and SO42− and inhibit side reactions. More importantly, an organic/inorganic hybrid solid electrolyte interface (SEI) layer is in situ constructed during the cycling, which enables ultrastable Zn plating/stripping (> 2000 h) under high current density (5 mA cm−2, 5 mAh cm−2) and high coulombic efficiency (99.8%) for more than 1000 cycles. Meanwhile, zinc‐ion hybrid capacitors (ZIHCs) with the colloidal electrolyte exhibit a favorable capacitance retention of 97% after 15000 cycles at the current density of 2 A g−1. Even at a high current density of 5 A g−1, it still has a capacitance retention of 96% after 30000 cycles. This study presents a novel electrolyte strategy for the formation of ultrastable electrode‐electrolyte interfaces in AZIBs.

Aqueous zinc‐ion batteries (ZIBs) are emerging as promising contenders for large‐scale energy storage owing to their intrinsic safety, cost‐effectiveness, and environmental sustainability. However, their practical application remains constrained by persistent issues at the Zn metal anode, including dendritic growth, interfacial passivation, and poor cycling stability. This study introduced a novel biopolymer‐based interfacial engineering strategy utilizing carboxymethyl cellulose (CMC), a zincophilic, water‐soluble, and sustainable biopolymer. A uniform CMC coating is applied via a scalable spray‐coating process and subsequently converted into a conductive carbonaceous interlayer through laser‐assisted carbonization, yielding a functional c‐CMC/Zn anode. This layer effectively suppresses dendrite formation, enhances Zn2+ ion transport, and improves the overall electrochemical stability of the Zn anode. Symmetric cell tests demonstrate exceptional cycling performance, with stable operation exceeding 3600 h at 2.0 mA cm−2 and an areal capacity of 2.0 mAh cm−2. When integrated into full‐cell architectures with V2O5cathodes, the c‐CMC/Zn║V2O5 device achieves a high specific capacity of 319 mAh g−1 at 0.2 A g−1 and retains 77% of its capacity over 1000 cycles at 1.0 A g−1. This work underscores the potential of laser‐carbonised biopolymer coatings as a versatile and scalable solution to the longstanding challenges of Zn anode instability in aqueous ZIB systems.

Featured by inherent advantages of low cost and high safety, zinc‐ion energy storage devices have emerged as a pivotal focus in the field of energy storage research. However, their large‐scale application is hindered by critical challenges: the instability of zinc anodes, which are plagued by dendritic growth and severe detrimental interfacial side reactions. In this study, by utilizing the inherent reducibility of the Zn anode and adding sodium carboxymethyl cellulose (CMC‐Na) as an electrolyte additive, we have prepared in situ cross‐linked CMC‐Na/polyacrylamide (PAM) hydrogel electrolytes to improve the stability of the Zn anode. The proposed synergistic optimization strategy effectively suppresses interfacial side reactions triggered by active water molecules. Moreover, this dual‐strategy intervention mitigates anode corrosion and dendrite growth through cooperative regulatory mechanisms. Consequently, the symmetric cells assembled with the in situ‐formed hydrogel electrolyte deliver stable cycling performance for 1000 h at a current density of 1 mA cm −2 . For the hybrid capacitor integrated with the CMC‐Na/PAM hydrogel electrolyte, it maintains efficient operation over 10,000 cycles even at a high current density of 10 mA cm −2 . This study demonstrates the superior efficacy of the integrated dual optimization strategies, offering a practical pathway for the advancement of high‐performance zinc‐ion hybrid capacitors.

Currently, the zinc anode faces significant challenges such as dendrite growth, corrosion, and hydrogen evolution, which severely limit the practical applications of aqueous zinc-ion batteries. To address these issues, this study designed a zinc anode (denoted as CG@Zn) coated with a gel composed of carboxymethyl cellulose sodium (CMC) and glucose. This coating featured dual functionalities: it regulated the directional transport of Zn2+ ions and constrained the electrochemical activity of interfacial water molecules, effectively inhibiting the growth of zinc dendrites and significantly reducing the occurrence of corrosion and hydrogen evolution side reactions. Benefiting from these advantages, CG@Zn exhibited excellent electrochemical performance. Under testing conditions of 5 mA cm-2/1 mAh cm-2, the symmetric battery assembled with CG@Zn demonstrated over 1000 h of stable cycling, achieving a cycle life five times that of bare zinc electrodes. Furthermore, the full cell configuration of CG@Zn//NaV3O8·1.5H2O with a matching zinc sulfate electrolyte maintained a capacity retention of 67.1 % after 15,000 cycles at 10 A g-1, significantly outperforming the rapid capacity decay observed in bare zinc batteries under the same conditions. Therefore, this study successfully developed an effective bifunctional gel coating for zinc anodes using CMC and glucose, paving the way for the development of safe and eco-friendly aqueous zinc-ion batteries.

Aqueous zinc‐ion batteries (AZIBs) have garnered significant interest for their potential in large‐scale energy storage, attributed to their high safety and low cost. Nonetheless, issues such as limited cycling lifespan and low coulombic efficiency (CE) associated with dendrite formation and uncontrollable side reactions on the Zn metal anode pose challenges that restrict their practical applications. Herein, a dielectric filler‐assisted artificial hybrid interphase is constructed on the Zn anode surface to address the challenges faced by the Zn anode in aqueous electrolytes. TiO2 nanoparticles with special dielectric properties promote the solvation process and carboxymethyl cellulose (CMC) acts as a physical barrier for suppressing the adverse reactions and blocking the dendrite. Consequently, a symmetric cell using a modified zinc anode achieves a prolonged cycle life of over 2500 h at 1 and 1 mAh cm−2. Furthermore, the full cell with a vanadium‐based cathode delivers excellent electrochemical performance (over 600 cycles at 1 A g−1). This research offers an efficient and scalable approach to enhance the performance of Zn metal anodes.

Zinc powder has attracted attention as a promising anode material for aqueous zinc-ion batteries (AZIBs) due to its excellent tunability and scalability. However, its practical application is limited by poor cycling stability, primarily caused by nonuniform reactions during repeated Zn plating and stripping processes. To address this issue, the binder plays a crucial role in maintaining the structural integrity of the anode components throughout cycling. Despite its importance, the influence of binder chemistry on electrochemical performance in ZIBs remains underexplored. In this study, we investigate the effects of two representative binders—polyvinylidene fluoride (PVDF) and the eco-friendly carboxymethyl cellulose sodium (CMC)—on the electrochemical behavior, cycling performance, and structural stability of AZIB anodes. PVDF, a conventional binder widely used in ZIBs, suffers from weak adhesion, requires the use of toxic organic solvent N-methyl-2-pyrrolidone (NMP), and exhibits poor electrolyte wettability, leading to delayed activation and capacity loss during early cycles. Additionally, its fluorinated polymer structure raises environmental concerns, limiting its suitability for next-generation sustainable energy storage systems. To overcome these limitations, we applied CMC as a hydrophilic and environmentally benign binder for the Zn anode. CMC provides strong adhesion and contains carboxylate functional groups that interact with Zn 2+ ions, promoting uniform Zn deposition. However, when used alone, CMC is susceptible to dissolution in aqueous electrolytes, compromising structural stability. To mitigate this, a crosslinked hydrophilic binder was introduced. The crosslinked binder simultaneously offers hydrophilicity, mechanical robustness, and environmental compatibility. As a result, the electrodes maintained structural integrity even under high mass loading and exhibited enhanced electrochemical performance. This study highlights the significance of binder design incorporating functional groups capable of regulating interfacial reactions in ZIBs. We present a simple and effective strategy for fabricating long-life, high-loading Zn powder anodes, thereby contributing a foundational approach toward the commercialization of zinc-based energy storage systems. These findings underscore the potential of cost-effective, stable, and eco-friendly energy storage technologies.

Aqueous zinc–iodine batteries (AZIBs) possess significant potential for energy storage owing to their high theoretical capacity and remarkable cycling stability. Nevertheless, their practical deployment is severely constrained by a shortened life resulting from uncontrollable parasitic reactions and poor temperature adaptability. Herein, we design a multifunctional dual‐network hydrogel electrolyte PHEAA‐CMC‐ Zn(CF 3 SO 3 ) 2 (HCZ) composed of rigid carboxymethyl cellulose (CMC) and flexible poly (N‐hydroxyethyl acrylamide) (PHEAA) featuring abundant dynamic intra/intermolecular hydrogen bonds. Intriguingly, the rich hydrophilic groups in the electrolyte form hydrogen bonds with water molecules, effectively regulating water‐induced side reactions at the electrode–electrolyte interfaces and enabling excellent temperature tolerance across a wide range from −30°C to 50°C. Moreover, the polar amide groups and oxygen‐containing functionalities within the hydrogel can coordinate with Zn 2+ to promote Zn 2+ migration at the anode, while simultaneously providing electrostatic adsorption of polyiodide species to mitigate the shuttle effect at the cathode. Therefore, Zn‖Zn symmetric cells equipped with this engineered electrolyte exhibit prolonged cycling stability exceeding 3000 h at both 20 and −30°C. Moreover, AZIBs with this hydrogel deliver long‐term cycling durability over 20 000 cycles at −30°C and 30 000 cycles at 50°C. This electrolyte provides new insights for AZIBs capable of stable operation across broad temperature.

Transient batteries are expected to lessen the inherent environmental impact of traditional batteries that rely on toxic and critical raw materials. This work presents the bottom-up design of a fully transient Zn-ion battery (ZIB) made of nontoxic and earth-abundant elements, including a novel hydrogel electrolyte prepared by cross-linking agarose and carboxymethyl cellulose. Facilitated by a high ionic conductivity and a high positive zinc-ion species transference number, the optimized hydrogel electrolyte enables stable cycling of the Zn anode with a lifespan extending over 8500 h for 0.25 mA cm-2 - 0.25 mAh cm-2 . On pairing with a biocompatible organic polydopamine-based cathode, the full cell ZIB delivers a capacity of 196 mAh g-1 after 1000 cycles at a current density of 0.5 A g-1 and a capacity of 110 mAh g-1 after 10 000 cycles at a current density of 1 A g-1 . A transient ZIB with a biodegradable agarose casing displays an open circuit voltage of 1.123 V and provides a specific capacity of 157 mAh g-1 after 200 cycles at a current density of 50 mA g-1 . After completing its service life, the battery can disintegrate under composting conditions.

No abstract available

Polymer electrolytes with high mechanical stability and versatility are increasingly critical for flexible wearable electronics. This study introduces a method for incorporating montmorillonite (MMT) into a carboxymethyl cellulose (CMC) and polyvinyl alcohol (PVA) matrix to develop a high-performance nanostructured composite electrolyte. This approach aims to establish robust nanoscale interfacial interactions between montmorillonite nanosheets and the polymer matrix. The well-developed pore structure within the system and the abundant active sites on the MMT nanosheets contribute to the ionic conductivity of the composite electrolyte, which achieves 23.96 ± 0.25 mS cm-1 at room temperature and expands the voltage window to 2.4 V. The assembled Zn || Zn symmetric cells demonstrate reversible stripping/plating over 1500 h at 1 mA cm-2 current density. Density Functional Theory (DFT) calculations reveal that Zn2+ preferentially binds with the polymer, regulating its solvation effect with water and suppressing the formation of zinc dendrite. The electrolyte shows excellent adaptability and versatility with various electrodes. For instance, flexible zinc-ion hybrid capacitors (FZHC) retain 88.6 % capacity after 90,000 cycles at 10 A g-1 and maintain normal function under harsh conditions such as cutting, bending, and pressing. This electrolyte holds significant potential for flexible energy storage applications.

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.

No abstract available

Replacing zinc foil with Zn micropowders (ZnMPs) enhances manufacturing compatibility for Zn‐metal batteries but imposes challenges like uncontrolled Zn deposition and accelerated structural degradation, typically resulting in a short cycle life of < 50 cycles. Herein, we synthesize a multifunctional bottle‐brush polycationic binder based on naturally abundant and mechanically robust chitin, which enables exceptional long‐term Zn plating/stripping reversibility, averaging 99.5% Coulombic efficiency over 300 cycles. The design rationales are experimentally validated as follows: diverse functional groups integrated onto the chitin backbone provide multiple supramolecular interactions ensuring ZnMP electrodes’ spatial uniformity and structural robustness; Zn2+‐carboxylate coordination simultaneously enhances the binder's mechanical strength (~1.2 MPa), toughness (~8.6 MJ m−3) and ionic conductivity (an 87% increase, reaching 1.72 × 10−5 S cm−1) upon swelling; while synergistic dynamic electrostatic interactions and hydrogen bonding permit rapid self‐recovery of the electrodes during cycling. This work underscores the promise of supramolecular engineering for binders targeting aggressive electrode chemistries.

Maintaining a steady affinity between gallium‐based liquid metals (LM) and polymer binders, particularly under continuous mechanical deformation, such as extrusion‐based 3D printing or plating/stripping of Zinc ion (Zn2+), is very challenging. Here, an LM‐initialized polyacrylamide‐hemicellulose/EGaIn microdroplets hydrogel is used as a multifunctional ink to 3D‐print self‐standing scaffolds and anode hosts for Zn‐ion batteries. The LM microdroplets initiate acrylamide polymerization without additional initiators and cross‐linkers, forming a double‐covalent hydrogen‐bonded network. The hydrogel acts as a framework for stress dissipation, enabling recovery from structural damage due to the cyclic plating/stripping of Zn2+. The LM‐microdroplet‐initialized polymerization with hemicelluloses can facilitate the production of 3D printable inks for energy storage devices.

Aqueous zinc (Zn)-ion batteries are considered very promising in grid-scale energy storage systems. However, the dendrite, corrosion, and H2 evolution issues of Zn anode have restricted their further applications. Herein, to solve these issues, a hydrophilic layer, consisting of a covalent organic polymer (COP) and carboxylmethyl cellulose (CMC), is designed to in situ construct a multifunctional quasi-gel (COP-CMC/QG) interface between Zn metal and the electrolyte. The COP-CMC/QG interface can significantly improve the rechargeability of the Zn anode through enhancing Zn2+ transport kinetics, guiding uniform nucleation, and suppressing Zn corrosion and H2 evolution. As a result, the COP-CMC-Zn anode exhibits a reduced overpotential (12 mV at 0.25 mA cm-2), prolonged cycle life (over 4000 h at 0.25 mA cm-2 and 2000 h at 5 mA cm-2 in symmetrical cells), and elevated full-cell (Zn/MnO2) performance. This work provides an efficient approach to achieve long-life Zn metal anodes and paves the way toward high-performance Zn-based and other metal-ion batteries.

Zinc (Zn) metal has attracted considerable attention because of its natural abundance and stability in aqueous environments compared with lithium/sodium metal anodes. Moreover, Zn metal as anode showed a high theoretical capacity (820 mAh g−1), high energy per volume (5855 mA cm−3), and low operational potential (–0.78 V vs SHE) in electrochemical systems. However, Zn metal suffers from dendrite growth and poor plating/stripping reversibility, resulting from inhomogeneous Zn ion flux and contamination by generally used glass fiber membranes (GFs) as separators. Although studies to inhibit dendritic Zn growth have been conducted, dendritic Zn remains still a major problem during long-term cycling under practical rate and capacity conditions. In this context, it is essential to investigate Zn deposition behavior from initial nucleation to Zn growth morphologies after long-term cycling. Among the problematic factors pointed out by researchers, the irregular pore distribution of GFs causes uneven Zn ion flux. Moreover, the detached fibers after cycling contaminate the Zn anode surface, resulting in nonuniform Zn deposition and trapping of Zn metal in the separator. To stabilize Zn metal anodes, introducing a protective layer can be an effective strategy to construct ion channels with abundant functional groups for high affinity with Zn metaland protect from direct contact with GFs. Organic polymers are suitable candidates for construction of protective layer which tolerates the volume changes of Zn metal and exhibit good chemical compatibility with Zn metal. Polysaccharides are favorable for use as gel polymers, separators, and binders owing to their cost-effectiveness and good electrochemical properties. Besides, they contain various oxygen-containing groups, resulting in relatively high ionic conductivity. However, it is not sufficient to fabricate membranes for the stabilization of Zn metal using polysaccharide alone because of insufficient ion conductive properties. This problem can be solved by blending polymers with high ionic conductivities such as poly(ethylene oxide) (PEO), poly(vinylidene difluoride), and poly(vinyl chloride). Notably, PEO has mainly been used in gel polymer electrolytes. The hydroxyl groups of PEO can facilitate the transport of metal ions and ether linkages can enhance the affinity with cations, resulting high ionic conductivity. In this study, we designed a functional protective layer by blending polysaccharide and PEO and investigated Zn deposition behavior from the formation of initial nucleation to Zn growth process after long-term cycling. The protective layer, fabricated by a one-pot method, featured highly dispersed blending polymers by phase separation and contained uniformly distributed oxygen-containing functional groups. Moreover, we demonstrated that the protective layer induced the formation of regular Zn nucleation sites and smooth Zn deposition after long-term cycling under the realistic conditions required for high-energy metal battery systems. Using the Zn||Cu and Zn||Zn cells stabilized by the protective layer under low capacity (0.1 mAh cm−2), we confirmed that homogeneous initial Zn deposition patterns were induced by ex situ SEM images of Cu and Zn electrodes. Subsequently, smooth and dense Zn growth was confirmed under fast Zn plating/stripping conditions, indicating that protective layer can induce basal plane (002) dominant deposition to mitigate dendrite formation and protect physically and chemically from GFs. Based on the morphological Zn deposition behavior, we successfully fabricated a functional protective layer and significantly enhanced the electrochemical performance of Zn metal battery systems. The Zn||Cu cells with a functional protective layer showed significantly increased long-term cycling above 3850 cycles (more than 160 days) at high rate and capacity condition (2 mA cm−2 and 1 mAh cm−2). In addition, the durability of protective layer was confirmed by a high-rate test (at 10 mA cm−2). These results are consistent with those of the Zn||Zn symmetric cell tests under harsh conditions of 5 mA cm−2 and 5 mAh cm−2. Furthermore, full cell with the protective layer using vanadium disulfides as the cathode exhibited enhanced cyclability over 1000 cycles with 87 % capacity retention compared to the bare full cell that short-circuited at the 340th cycle. Our work demonstrated that there are two important factors affecting the durability of Zn anodes: (i) Zn metal surface should be protected by a smooth and dense layer with high affinity to Zn metal and ions and (ii) physical and chemical contamination from GFs. Figure 1

Aqueous Zn ion batteries (ZIBs) are one of the most promising battery chemistries for grid‐scale renewable energy storage. However, their application is limited by issues such as Zn dendrite formation and undesirable side reactions that can occur in the presence of excess free water molecules and ions. In this study, a nanocellulose‐carboxymethylcellulose (CMC) hydrogel electrolyte is demonstrated that features stable cycling performance and high Zn2+ conductivity (26 mS cm−1), which is attributed to the material's strong mechanical strength (≈70 MPa) and water‐bonding ability. With this electrolyte, the Zn‐metal anode shows exceptional cycling stability at an ultra‐high rate, with the ability to sustain a current density as high as 80 mA cm−2 for more than 3500 cycles and a cumulative capacity of 17.6 Ah cm−2 (40 mA cm−2). Additionally, side reactions, such as hydrogen evolution and surface passivation, are substantially reduced due to the strong water‐bonding capacity of the CMC. Full Zn||MnO2 batteries fabricated with this electrolyte demonstrate excellent high‐rate performance and long‐term cycling stability (>500 cycles at 8C). These results suggest the cellulose‐CMC electrolyte as a promising low‐cost, easy‐to‐fabricate, and sustainable aqueous‐based electrolyte for ZIBs with excellent electrochemical performance that can help pave the way toward grid‐scale energy storage for renewable energy sources.

Aqueous zinc (Zn)‐based structural batteries capable of both electrochemical energy storage and mechanical load‐bearing capabilities are attractive for next‐generation energy storage for future electric vehicles due to their eco‐friendliness, non‐toxic, and safe nature. However, parasitic free water activities plague aqueous Zn‐based batteries, detrimental to the electrochemical performance and longevity of the cell. Developing polymer gel electrolytes is a notable potential solution, but they usually have poor electrode interfacial interactions and inadequate mechanical properties. This article introduces a novel non‐fibrous highly amorphous cellulose polymer electrolyte “Cellyte” for aqueous structural Zn‐based batteries. Cellyte exhibits a high strength of ≈24 MPa and Young's modulus of ≈380 MPa, along with the ability to suppress parasitic water activity. The symmetric Zn||Cellyte||Zn cell therefore demonstrates excellent cycling stability of over ≈3000 h. Cellyte can also serve as the binder for the structural cathode material, creating a continuous polymer electrolyte–cathode interface, thereby increasing mechanical robustness and decreasing interfacial resistances of the battery, allowing the structural Zn||Cellyte||LMO‐CF battery to achieve high electrochemical performance with excellent cycling stability over 1200 h with ≈91.5% capacity retention. This provides a pathway to design mechanically robust, electrochemically performing, and safe structural batteries.

No abstract available

Zinc‐based batteries are emerging as promising alternatives to mainstream technologies due to their superior safety, cost‐effectiveness, and abundance of raw materials. However, zinc anodes, exhibit insufficient cycle life and low utilization in aqueous electrolytes, mainly owing to shape change and passivation. While nanostructuring of Zn anodes has been explored for Zn‐Ni rechargeable alkaline batteries, no explicit electrochemical studies have elucidated how nanostructures, fabricated in the oxidized state, are reduced during the initial formation step, yielding elemental Zn. In this work, a hydrothermal synthesis of freestanding electrodes is proposed, based on vertically aligned ZnO nanorods grown directly on carbon cloth (CC) (ZnO/CC). ZnO nanostructuring mitigates passivation, while the carbon cloth fiber network confines soluble Zn(II) intermediates, hindering diffusion into the electrolyte bulk. Moreover, the CC substrate provides optimal electronic contact to the active material, and acts as a built‐in current collector. This work investigates the evolution of ZnO/CC during the first electrochemical reduction cycle, with emphasis on morphochemical nanostructure changes rather than establishing a benchmark anode. Electrochemical measurements are combined with advanced characterization techniques, high‐resolution transmission electron microscopy (HRTEM), and X‐ray absorption hyperspectral imaging via scanning transmission X‐ray microscopy (STXM) and ptychography at the Zn L‐edge. This multimodal approach offers unprecedented insights into the ZnO‐to‐Zn reduction to guide future Zn‐ion anode design.

Aqueous zinc-ion batteries are attracting extensive attention due to the long-term service life and credible safety as well as the superior price performance between the low cost of manufacture and high energy density. The fabrication of inexpensive, high-performance flexible solid-state zinc-ion batteries, thus, are urgently need for the blooming wearable electronics. Herein, as a proof-of-concept study of waste into wealth, cellulose flakes derived from waste pomelo peel are utilized as the substrate for electrodes and hydrogel electrolytes into a flexible rocking-chair zinc-ion battery. The unique sandwich-type structure holding the flake-like cellulose substrate and linear carbon nanotubes endows the flexible cathode and anode with fast ion and electron transportation. The obtained cellulose-based hydrogel electrolytes on account of special affinity with aqueous ZnSO4 electrolyte output an excellent ionic conductivity. The assembled flexible rocking-chair zinc-ion battery benefitting from the synergistic effect of sandwich-type electrodes and cellulose-based hydrogel electrolytes demonstrates outstanding electrochemical performance and mechanical properties. This work not only puts up an effective roadmap for flexible battery devices, but also reveals the great potential of waste biomass materials in energy storage applications.

Sustainable and cheaper energy storage devices are the key to the global decarbonizing initiative. The alarming consequences of mining metals like lithium are surmountable by transitioning towards alternatives like zinc-based energy storage and using greener components in the battery architecture. This work explores bacterial cellulose, a proven sustainable biomaterial made through microbial fermentation, as an electrode and electrolyte for a zinc ion battery. Combined with the simplicity and scalability of the preparation method for bacterial cellulose, we designed a tri-layer electrode with V 2 O 5 and nano-fibrillated hydrogel electrolyte for an all-solid-state zinc ion battery. The CNT-cellulose-based large-surface scaffolds encapsulating V 2 O 5 facilitate the manufacturing of inexpensive electrodes exhibiting a high capacity of 200 mAh g -1 at 4 A g -1 after 500 cycles with excellent stability. On the other hand, the hydrogel electrolyte offers a high ionic conductivity of 41 mS cm -1 at 30°C. The hydrogel is designed by a facile solvent exchange approach, where glycerol substitutes the free water molecules and settles between cellulose nanofibers. Owing to its bigger molecular size and ability to form hydrogen bonds with the cellulose fibers, a highly stable BC-based gel could be developed that regulates ion transport and extends the potential window compared to conventional hydrogels. Utilizing differential scanning calorimetry (DSC) to determine a eutectic phase of the water-glycerol mixture, we were also able to expand the operating temperature up to -40°C and investigate the performance of these zinc-ion batteries at sub-zero temperatures.

No abstract available

Aqueous zinc-ion batteries (ZIBs) offer a safe and cost-effective solution for stationary energy storage, but achieving long-term cycling at high areal loadings and low C-rates remains challenging. Here, we present a polyaniline-based ZIB with a unique 3D interconnected sponge-like carbon nanotube (CNT) host that provides high porosity, mechanical resilience, and robust conductivity. This architecture supports active material loading up to 6 mg cm–2, enabling stable cycling at practical current densities. With a dimethyl sulfoxide electrolyte additive, the cell retains 70% capacity over ∼6,000 cycles at 0.68C, highlighting its outstanding long-term stability at low rates. It also maintains ∼9,000 cycles at 6.8C, demonstrating high-rate capability. To demonstrate scalability, we implemented a solvent-free dry electrode process using CNT chunks and polytetrafluoroethylene binder, achieving a high areal loading of 7.9 mg cm–2 and delivering 140 mAh g–1 at 0.5 C. These results represent a significant step toward durable, high-loading, and scalable ZIBs for grid-level energy storage applications.

No abstract available

The unstable electrolyte-anode interface, plagued by parasitic side reactions and uncontrollable dendrite growth, severely hampers the practical implementation of aqueous zinc-ion batteries. To address these challenges, we developed a regenerated cellulose-based artificial interphase with synergistically optimized structure and surface chemistry on the Zn anode (RC@Zn), using a facile molecular chain rearrangement strategy. This RC interphase features a drastically increased amorphous region and more exposed active hydroxyl groups, facilitating rapid Zn2+ diffusion and homogeneous Zn2+ interface distribution, thereby enabling dendrite-free Zn deposition. Additionally, the compact texture and abundant negatively charged surface of the RC interphase effectively shield water molecules and harmful anions, completely preventing H2 evolution and Zn corrosion. The superior mechanical strength and adhesion of the RC interphase also accommodate the substantial volume changes of Zn anodes even under deep cycling conditions. Consequently, the RC@Zn electrode demonstrates an outstanding cycling lifespan of over 8000 hours at a high current density of 10 mA cm-2. Significantly, the electrode maintains stable cycling even at a 90% depth of discharge and ensures stable operation of full cells with a low negative/positive capacity ratio of 1.6. This study provides new solution to construct highly stable and deep cycling Zn metal anodes through interface engineering.

No abstract available

No abstract available

No abstract available

No abstract available

Zinc-air batteries (ZABs) have become an ideal energy storage option for wearable devices due to their high theoretical energy density and low cost. However, the evaporation and leakage of liquid electrolytes limit their long-term stability. In this study, a novel dual-network gel electrolyte (PANa-SiO2-CMC) was synthesized through the synergistic effect of sodium polyacrylate (PANa), nano-silica (SiO2) and carboxymethyl cellulose (CMC), and it was applied to flexible ZAB. This material exhibits outstanding comprehensive performance: superior mechanical properties (with tensile strength of 3.62 MPa and elongation of 1865.01 %), high ionic conductivity (276.51 mS·cm-1), and excellent electrolyte retention ability (83.24 %). The flexible ZAB assembled based on this electrolyte demonstrates excellent electrochemical performance: the open-circuit voltage is stably maintained at approximately 1.4 V, the capacity reaches 760.61 mAh·g-1, and it can maintain stable voltage output after 160 h cycling tests and under different bending angles, fully demonstrating its applicability in wearable devices. Through molecular dynamics (MD) simulation, the rapid diffusion mechanism of OH- in the PANa-SiO2-CMC system was further revealed, providing an important theoretical basis for the design of electrolytes for high-performance ZABs.

No abstract available

Moderate-concentration ZnCl 2 (15 m) was found to be effective for suppressing the dissolution of vanadate cathode, which was more stable and had 4 times higher ionic conductivity than 30 m “water-in-salt” electrolyte. K 0.486 V 2 O 5 with huge interlayer space of ~ 0.95 nm was chosen for the first time to assemble aqueous Zn ion batteries, giving rise to excellent rate performance and high energy and power densities. A novel sodium carboxymethyl cellulose-15 m ZnCl 2 hydrogel electrolyte with high ionic conductivity of 10.08 mS cm −1 was designed, enabling a bendable Zn ion battery with outstanding resistance to temperature and pressure. Vanadium-based cathodes have attracted great interest in aqueous zinc ion batteries (AZIBs) due to their large capacities, good rate performance and facile synthesis in large scale. However, their practical application is greatly hampered by vanadium dissolution issue in conventional dilute electrolytes. Herein, taking a new potassium vanadate K 0.486 V 2 O 5 (KVO) cathode with large interlayer spacing (~ 0.95 nm) and high capacity as an example, we propose that the cycle life of vanadates can be greatly upgraded in AZIBs by regulating the concentration of ZnCl 2 electrolyte, but with no need to approach “water-in-salt” threshold. With the optimized moderate concentration of 15 m ZnCl 2 electrolyte, the KVO exhibits the best cycling stability with ~ 95.02% capacity retention after 1400 cycles. We further design a novel sodium carboxymethyl cellulose (CMC)-moderate concentration ZnCl 2 gel electrolyte with high ionic conductivity of 10.08 mS cm −1 for the first time and assemble a quasi-solid-state AZIB. This device is bendable with remarkable energy density (268.2 Wh kg −1 ), excellent stability (97.35% after 2800 cycles), low self-discharge rate, and good environmental (temperature, pressure) suitability, and is capable of powering small electronics. The device also exhibits good electrochemical performance with high KVO mass loading (5 and 10 mg cm −2 ). Our work sheds light on the feasibility of using moderately concentrated electrolyte to address the stability issue of aqueous soluble electrode materials.

Significance The anode of aqueous zinc-ion batteries suffers from zinc dendrites and parasitic reactions, while the cathode faces vertical deposition of the intermediate product. Inspired by wood, this work introduces an anisotropic hydrogel electrolyte (Aniso-CMC), which possesses oriented architecture. Compared to conventional hydrogel electrolytes, the Aniso-CMC achieves significantly enhanced modulus and ionic conductivity along the longitudinal direction, therefore proving effectiveness in inhibiting vertical deposition of electrochemical products at the electrode/electrolyte interface while mitigating electrochemical polarization. Accordingly, the zinc stripping/plating reversibility can be considerably improved, and the assembled quasi-solid-state Zn//MnO2 battery realizes excellent cycling stability and substantial volumetric energy density. The research results could aid in the future development of hydrogel electrolytes and aqueous batteries.

No abstract available

A quick and simple HCl treatment is designed to suppress the formation of Zn dendrites on Zn metal anodes. This special microgroove structure homogenizes the electric field on the surface of the Zn plate, giving rise to more uniform Zn deposition.

In this study, bacterial cellulose-polyelectrolyte complex (BC/PEC) composite hydrogels were prepared for an electrode separator. First, the poly(sodium 4-styrenesulfonate)/poly(dimethyl diallyl ammonium chloride) hydrogel was prepared using NaCl as a shielding agent and a dialysis tube to control the formation of the PEC hydrogel. BC was incorporated into the supporting skeleton. The 3D BC sponge was prepared by using an alkali swollen BC gel, followed by freeze–thaw cycles to develop the porous framework. The BC backbone was then cross-linked with glutaraldehyde (GA) under acidic conditions to obtain cross-linked BC (BC-GA), resulting in the improved dimensional stability of the BC skeleton in an alkali medium. Subsequently, the PEC was introduced into the BC-GA pores, resulting in the BC-GA/PEC composite hydrogel with improved mechanical and dimensional properties and thermal stability. Electrolyte permeability tests with 6 M KOH showed that BC/PEC had lower permeability (approximately 2 × 10–2 cm2/min) compared to BC and BC-GA (1.0–1.5 × 10–1 cm2/min) compared to the ionic conductivity of BC-GA/PEC with values of 30.9–55.9 mS/cm. The charge–discharge cycling performance of BC-GA/PEC hydrogels as a zinc battery separator was evaluated using plating/stripping tests, revealing that the zinc anode surface exhibited less corrosion and slower dendrite growth. This phenomenon was due to the decrease in Zn2+ crossover by either repulsion or attraction forces between Zn2+ and BC-GA/PEC hydrogels, making them an alternative for electrode separators in place of liquid electrolyte separators.

Aqueous zinc metal batteries (ZMBs) are expected to be used in grid-scale storage systems due to their superior intrinsic safety and lower manufacturing cost of zinc anodes. However, the uncontrolled...

The zinc dendrite growth generally relies upon a "positive-feedback" mode, where the fast-grown tips receive higher current densities and ion fluxes. In this study, a self-limiting polyacrylamide (PAM) hydrogel that presents negative feedback to dendrite growth is developed. The monomers are purposefully polymerized at the dendrite tips, then the hydrogel reduces the local current density and ion flux by limiting zinc ion diffusion with abundant functional groups. As a consequence, the accumulation at the dendrite tips is restricted, and the (002) facets-oriented deposition is achieved. Moreover, the refined porous structure of the gel enhances Coulombic Efficiency by reducing water activity. Due to the synergistic effects, the zinc anodes perform an ultralong lifetime of 5100 h at 0.5 mA cm-2 and 1500 h at 5 mA cm-2 , which are among the best records for PAM-based gel electrolytes. Further, the hydrogel significantly prolongs the lifespan of zinc-ion batteries and capacitors by dozens of times. The developed in situ hydrogel presents a feasible and cost-effective way to commercialize zinc anodes and provides inspiration for future research on dendrite suppression using the negative-feedback mechanism.

Regarded as one of the popular cathode materials in aqueous zinc ion batteries (ZIBs), VS2 has unsatisfied cycling stability and relatively low capacity owing to its poor conductivity and low mechanical properties. To this regard, compositing VS2 with high‐conductive 2D transition metal carbide (MXene) has been an effective method recently. However, the Zn dendrite on the anode electrode derived from the uncontrollable sluggish migration of solvated Zn2+/H2O ions seriously threatens the application safety of ZIB batteries. To effectively regulate the diffusion of zinc ions, in this work a conductive polymeric electrolyte of sulfonated polyaniline (SPANI) is added in the electrolyte solution. Under the Zn2+/SPANI interactions confirmed by X‐ray diffraction, Raman, and zeta potential experiments, the Zn2+/H2O combination is weakened, and the deposition rate of Zn2+ is increased evaluated by the galvanostatic intermittent titration technique. Theoretical simulation shows that the electrostatic shielding by SPANI combining Zn2‐ at the zinc/electrolyte interface has important contribution to the significant suppression of Zn dendrite. Accordingly, the fabricated VS2@MXene||ZnSO4+SPANI||Zn battery shows high capacity (368.0 mAh g‐1 at 0.1 A g‐1), which remains 96% after 5000 cyclic charge–discharge operations. This work develops an available strategic idea for suppressing growth of metallic dendrites to improve the ZIB performances.

Aqueous zinc-metal batteries (AZMBs) are a promising solution for safe and sustainable energy storage, yet zinc anode instability remains a key challenge. Electrolyte additives are widely employed to enhance performance by suppressing the hydrogen evolution reaction (HER) and slowing charge transfer kinetics. However, their benefits typically peak at an optimal concentration and diminish beyond that point—a behavior that remains poorly understood. Here, we show that this optimal performance arises from a delicate balance between solvent reorganization kinetics, charge transfer rates, and suppression of parasitic reactions. Using temperature-dependent studies and model additives across commonly used zinc electrolytes—ZnCl₂, ZnSO₄, and Zn(OTf)₂—we find that most additives stabilize zinc deposition by reducing the exchange current density ( i 0,Dep ), resulting in a peak in coulombic efficiency (CE) at a specific i 0,Dep . Contrary to conventional expectations, we demonstrate that reducing i 0,Dep beyond this optimal point does not further improve performance. Instead, it introduces mass transport limitations, increases HER activity—quantified using electrochemical mass spectrometry (ECMS)—and promotes dendritic growth. While the Sands’ model predicts dendrite formation at high i 0,Dep , it does not fully account for the electrolyte-additive interactions that become significant at low i 0,Dep . We propose a refined mechanistic framework that extends beyond classical models, offering new insight into the counterintuitive decline in performance observed at excessive additive concentrations.

Aqueous zinc‐ion batteries are promising for flexible energy storage; however, water‐related issues such as electrolyte decomposition, dendrite growth, and anode corrosion impede practical application. Although hydrogel electrolytes can suppress water activity and guide zinc‐ion transport to inhibit dendrites, achieving high strength, high conductivity, and low temperature tolerance together remains challenging. Inspired by natural cryoprotection, a competitive interaction strategy using natural proline is present to enhance the polyvinyl alcohol (PVA)/ZnSO 4 hydrogel electrolyte. The hydrogel is physically crosslinked by PVA crystallites and stabilized by noncovalent interactions among PVA, Zn 2+ , and proline, showing 0.9 MPa tensile strength and 403% elongation. Proline's zwitterionic groups compete with water molecules in zinc‐ion solvation, with a higher binding energy of 222.15 kcal/mol compared to 100.42 for water, enabling uniform Zn deposition and dendrite suppression. Zn||MnO 2 cells with this hydrogel retained 61% capacity after 200 cycles at 0.5 C, much better than the 32% with a liquid electrolyte. Proline also breaks the hydrogen bonding network of water, lowering the freezing point of the hydrogel to −27°C and maintaining 1.95 mS/cm conductivity at −20°C. The hydrogel allows flexible pouch cells to operate reliably under deformation and freezing conditions, demonstrating great potential for wearable energy storage. image

No abstract available

The reversible cycling lifespan of zinc‐ion batteries is fundamentally compromised by the hydrogen evolution reaction (HER) and the growth of Zn dendrites induced by tips on 2D zinc metal anodes. Herein, a 3D zinc metal alloy anode to effectively mitigate dendrite growth and HER through dual regulation of the interface is presented. Experimental results confirm that the second component with strong H+ adsorption can efficiently inhibit Hads desorption diffusion, thereby suppressing HER. Moreover, the robust interaction between the in‐situ derived solid electrolyte interphase (SEI) layer and Zn2+ also enhances Zn2+ diffusion kinetics, reduces nucleation energy barriers, achieving dendrite‐free deposition of Zn2+. The as‐prepared 3D Zn‐W anodes achieve a lifespan of up to 2400 h with a coulombic efficiency of 99.23% achieved in symmetrical cells and can also exceed 200 h when operated at a depth of discharge as high as 91.46%. This work provides a simple and effective approach toward enhancing the safety and efficiency of zinc‐ion batteries while significantly improving Zn utilization efficiency.

The cycle life of aqueous zinc‐ion batteries (AZIBs) is hindered by the unstable Zn anode interface, causing uncontrolled dendrite growth and side reactions. Herein, for the first time, a hierarchical nanostructure‐engineered hydrogel interphase layer is developed via a facile and precisely controlled copolymerization‐induced microphase separation (CIMS) strategy, which enables multi‐level Zn2+‐buffering to stabilize the Zn anode interface: 1) The nanoconfinement effect, combined with the hydrophobicity ofmethylacryloyloxypropyl cage‐type polyhedral oligomeric silsesquioxane (MP‐POSS), facilitates [Zn(H2O)6]2+ desolvation while blocking water and SO42− penetration, achieving an optimal balance between enhanced Zn2+ transport and minimized side reactions; 2) CIMS between polar comonomers and MP‐POSS creates hierarchical molecular clusters within the hydrogel. These self‐assembled domains homogenize Zn2+ flux and reduce interfacial concentration polarization, realizing dendrite‐free Zn deposition. After modification, symmetric cells achieve exceptionally long lifespan exceeding 5500 h (1 mA cm−2) and 1500 h (10 mA cm−2). Asymmetric cell demonstrates an impressive Coulombic efficiency of 99.6% after 3600 cycles. MnO2 and V2O5 full cells retain 85.4% and 84.7% capacity retention after 1000 (1 A g−1) and 2000 (5 A g−1) cycles, respectively. This research unveils a novel multi‐level Zn2+‐buffering mechanism based on gel polymer hierarchical nanostructure engineering and provides a feasible strategy for advancing grid‐scale AZIBs.

Zn metal with high specific capacity and low redox potential is deemed to be an ideal anode material for aqueous zinc-ion batteries (ZIBs). However, the serious dendrite problems induced by the uneven deposition of zinc shorten the service life and hinder the development of ZIBs. According to the nucleation and growth mechanism, the charge distribution at the anode interface is the critical factor affecting the deposition morphology. Herein, CF4 plasma technology is applied for the first time to in situ modification of the Zn anode, and then, the uniform nanoscale ZnF2 particles are formed. Due to the excellent ionic conductivity and poor electronic conductivity of ZnF2, the ion and electron distribution at the anode interface is orderly regulated, thus guiding uniform and reversible deposition behavior and restraining the dendrite growth. As a result, the Zn@ZnF2-5 anode exhibits low nucleation overpotential (16 mV), long cycle life (2500 h at 1 mA cm-2 and 1 mA h cm-2), and excellent resistance to high current density (20 mA cm-2) and high discharge depth (16%). Meanwhile, the Zn@ZnF2-5|I2@AC full battery shows remarkable cycle stability (1000 cycles) with ∼10% discharge depth of the anode. The novel and practical CF4 plasma in situ modification strategy provides a new idea for the interface modification of zinc anode.

The advancement of anode‐free batteries (AFBs) presents a promising approach to enhance the energy density of secondary batteries. Nonetheless, a prevalent challenge associated with AFBs is the low Coulombic efficiency (CE), which arises from the surface inhomogeneity of the current collector. Conventional strategies load a variety of metalophile materials on its surface to enhance CE. However, without the solution of the intrinsic inhomogeneity of the current collector, the modification cannot be absolutely uniform, resulting in defect generation and even interface failures. Herein, anode‐free zinc metal batteries employing copper foil as a representative are used to eliminate the inhomogeneity of the oxide layer on the commercial copper foil surface while simultaneously adhering a homogenized thin chlorine (Cl) atomic layer with 100% conformal coverage (modified‐Cu) by a one‐step method. The homogenized Cl atomic layer exhibits a 3D diffusion for Zn atoms and induces dense growth of Zn (100) crystal plane, promoting reversible Zn plating/stripping. Additionally, the modified‐Cu||ZnxMnO2 anode‐free full battery exhibits superior cycling stability (500 cycles with 80% capacity retention). In addition to this, meter‐level modified‐Cu is produced in large quantities through a roll‐to‐roll system. This innovative strategy for constructing homogenized surfaces can promote the development of high‐energy‐density anode‐free metal batteries toward practical applications.

This work aims to deal with the challenges associated with designing complementary bifunctional electrocatalysts and a separator/membrane that enables rechargeable zinc-air batteries (RZABs) with nearly solid-state operability. This solid-state RZAB was accomplished by integrating a bifunctional electrocatalyst based on Ru-RuO2 interface nanoparticles supported on nitrogen-doped (N-doped) graphene (Ru-RuO2/NGr) and a dual-doped poly(acrylic acid) hydrogel (d-PAA) electrolyte soaked in KOH with sodium stannate additive. The catalyst shows enhanced activity and stability toward the two oxygen reactions, i.e., oxygen reduction and evolution reactions (ORR and OER), with a very low potential difference (ΔE) of 0.64 V. The computational insights bring out the electronic factors contributing to the enhanced catalytic activity of Ru-RuO2/NGr based on the charge density difference (CDD) between the interfaces. The disadvantages of the existing solid-state RZABs, such as their limited lifespan brought on by passivation, dendritic growth, corrosion, and shape change, have also been taken into account. The introduction of the stannate additive to the electrolyte induced an in situ Zn-anode modification, which subsequently improved the interfacial stability of the ZABs and, hence, the battery life cycles. The experimental observations reveal that, during the charging process, the Sn nanoparticles enable the homogeneous Zn deposition on the surface of the anode. Thus, the in situ Zn-anode surface modification assisted in achieving a high-rate cycle capability, viz., the homemade catalyst-based system exhibited continuous charge-discharge cycles for 20 h at a current density of 2.0 mA cm-2, with each cycle lasting for 5 min.

To address the issues of dendrite growth and zinc corrosion in rechargeable zinc‐air batteries, multifunctional glycine/valine additives are introduced into the electrolyte. By regulating the solvation shell structure and enhancing interfacial stability, these additives aim to protect the reversibility and stability of the zinc anode. Glycine/valine molecules inhibit the formation of the [Zn(H2O)6]2+ and Zn5(OH)8(OAc)2·2H2O by‐products at the interface by replacing active water molecules in a strong alkaline environment. Additionally, they form a hydrophobic electric double layer on the zinc metal surface, during the charge/discharge process, and construct an in situ solid electrolyte interface layer. This further suppresses the hydrogen evolution reaction and dendrite growth. The superior long‐term cycling stability of Zn||Zn cells, Zn||Cu, and zinc‐air full cells demonstrates the effectiveness of glycine/valine additives.

High-safety aqueous zinc (Zn) ion batteries confront hydrogen evolution reaction (HER) and dendrite growth of Zn anode, which can be well solved by electrolyte optimization and electrode modification. However, the simultaneously implementation of the electrolyte solvation structure and electrode/electrolyte interface regulation has been ignored and rarely investigated. In this work, inspired by shunt mechanism of hemicellulose in plant kingdom, xylan (XL) was designed and developed as a trace electrolyte additive (ZS@XL) to disperse in aqueous electrolyte and adsorb on Zn anode to simultaneously regulate solvation structure and electrode/electrolyte interface of Zn anode. XL-adsorbed layer can act as "shunt channels" to uniform ion flux and physical barrier to reduce the contact between active H2O and Zn metal, thus suppressing dendrite growth and HER. Meanwhile, high binding energy of XL with Zn2+ can destroy the solvation structure of Zn(H2O)62+ to decrease the number of active H2O and facilitate fast desolvation kinetics for the hindrance of HER. As a result, Zn anode with ZS@XL achieves excellent plating/stripping reversibility of 1400 cycles, long cycling life of 2800 h, as well as Zn-iodine (I2) full battery with ZS@XL exhibits excellent cycling performance of 16,000 cycles and practical application to power electric instruments. This work opens a novel route to simultaneously regulate electrolyte solvation structure and electrode/electrolyte interface of Zn anode by biomass materials.

The reversibility and stability of aqueous zinc-ion batteries (AZIBs) are largely limited by free-water-induced side reactions (e.g., hydrogen evolution and zinc corrosion) and negative zinc dendrite growth. To address these issues, we introduced triethyl 2-phosphonopropionate (Tp), a novel high-dipole-moment electrolyte additive. Tp effectively replaces free water in the electrolyte through strong ion-dipole interactions, altering the solvation structure and suppressing hydrogen evolution and zinc corrosion at the zinc anode. Additionally, the high binding energy between Tp and zinc foil ensures that Tp adheres firmly to the zinc anode surface, while the hydrophobic alkyl chains repel free water, modifying the interfacial structure of the zinc anode, promoting reversible zinc deposition, and effectively suppressing zinc dendrite growth. With these excellent properties, the optimal concentration of Tp enables a cycle time of over 770 h for 1 mA cm-2 and 1 mAh cm-2 symmetric cells, which is 7.7 times longer than that of pure electrolyte. Furthermore, the cycle number of Zn//Na2V6O16 full cells increased from 600 to 4000 cycles compared to pure electrolyte, with capacity retention improved from 70 % to 92 %. These results highlight the significance of high-dipole moment electrolyte additives, provide new insights into electrolyte modification strategies, and are expected to accelerate the commercialization of AZIBs for practical applications.

Reasonable regulation of iodine redox has gradually shown potential as a desirable cathodic reaction in zinc‐based batteries, but suffers from poor cyclic reversibility caused by uncontrollable side reactions. Also, the irregular growth of dendrites and unavoidable occurrences of hydrogen evolution reaction in H2O‐rich environment have become permanent topics in anodic zinc. Herein, a cross‐linked gel based on carboxymethyl chitosan is proposed and serves as an artificial electrolyte interphase for zinc anode (marked as Zn‐CMCS). Such a coating formed by crosslinking among a monodentate carboxyl group, a hydroxyl, an amino, and Zn2+ from adding solution closely adheres on the surface of the zinc foil with toughness, ductility, and ideal electrochemical kinetics. Additionally, its homogenized surface charge distribution provides a “flexible” substrate for zinc plating/stripping, resulting in a flat real‐time interface. While introducing I−/I0 conversion by matching adsorptive activated carbon on carbon fiber cloth (AC‐CFC) as cathode, the internal space restricted by CMCS gel enables the assembled Zn‐CMCS/AC‐CFC battery to exhibit a greatly improved reversibility under long‐cycling condition within 28 000 cycles (measured for more than 2 years) in a narrow operating voltage range of 0.23 V.

Aqueous zinc-ion batteries (ZIBs) have attracted extensive research as a promising energy storage system, whereas their practical applications are plagued by zinc dendrite and parasitic reaction issues-caused poor stability of zinc anodes. The currently used glass fiber separators are incapable of stabilizing zinc anodes and also impair the energy density of ZIBs due to their large thickness (e.g., 260-780 μm). Herein, we report defect-rich carbonaceous interface-synergized cellulose nanofiber (CNF) membranes as functional ultrathin separators for ZIBs, which effectively inhibit zinc dendrite growth and parasitic reactions to realize stable zinc anodes. A carbonaceous material with rich N, O and Zn heteroatom defects is synthesized by carbonizing ZIF-8 precursor and then served as the modification interface of CNF membranes to fabricate 28 μm-thick bilayer-structured separators. For the designed functional ultrathin separators, the nanoporous CNF membrane substrate homogenizes Zn2+ flux, and more importantly, the defect-rich carbonaceous interface not only provides abundant zincophilic sites to promote Zn2+ desolvation and uniform zinc deposition but also suppresses parasitic reactions on zinc anodes. As a result, zinc anodes coupled with the designed separators present superior electrochemical stability such as a 2600 h operation lifetime, ∼50 times longer than that of zinc anodes coupled with glass fiber separators. The availability of the proposed functional ultrathin separators is further verified in Zn//NaV3O8‧1.5 H2O ZIBs. This work provides new inspiration for designing advanced separators for high-performance ZIBs.

Recent advancements in hydrogel electrolytes for aqueous zinc‐ion batteries (AZIBs) have drawn considerable interest due to their soft nature, offering potential to overcome challenges including reversibility and flexibility. As the most abundant natural polymer, cellulose is ideal for AZIB hydrogel electrolytes due to rich hydroxyls with stable hydrogen‐bonded networks for water retention. However, conventional cellulose hydrogels suffer from low Zn2+ conductivity and insufficient mechanical robustness, usually requiring additional polymers to meet practical demands. This work reports a chemically neutral dissolution system combined with Keggin‐type polyoxometalate as a bifunctional crosslinker and electrolyte modulator. This approach results in ultra‐low solvation of Zn2+ in cellulose hydrogel, contributing to a wide 2.48 V electrochemical stability window. The high‐desolvation hydrogel exhibits balanced Zn2+ reaction stability and transport kinetics, effectively suppressing dendrite growth and parasitic reactions. The Zn electrode can be stably strapped/plated with this hydrogel for thousands of cycles with minimal Coulomb efficiency change. The hydrogel also shows excellent flexibility, with toughness of 1.5 MJ m−3 and elongation at break of 80%. Pouch cells assembled with this hydrogel demonstrate high mechanical flexibility and stability under deformations. This pioneering cellulose dissolution and crosslinking chemistry paves the way for practical application of flexible, durable AZIBs.

A novel polymer host from carboxymethyl cellulose (CMC)/poly(N-isopropylacrylamide) (PNiPAM) was developed for a high safety solid polymer electrolyte (SPE) in a zinc ion battery. Effects of the PNiPAM loading level in the range of 0–40% by weight ( wt%) on the chemical, mechanical, thermal, and morphological properties of the CMC/PNiPAMx films (where x is the wt% of PNiPAM) were symmetrically investigated. The obtained CMC/PNiPAMx films showed a high compatibility between the polymers. The CMC/PNiPAM20 blend showed the greatest tensile strength and modulus at 37.9 MPa and 2.1 GPa, respectively. Moreover, the thermal degradation of CMC was retarded by the addition of PNiPAM. Scanning electron microscopy images of CMC/PNiPAM20 revealed a porous structure that likely supported Zn2+ movement in the SPEs containing zinc triflate, resulting in the high Zn2+ ion transference number (0.56) and ionic conductivity (1.68 × 10–4 S cm−1). Interestingly, the presence of PNiPAM in the CMC/PNiPAMx blends showed a greater stability during charge–discharge cyclic tests, indicating the ability of PNiPAM to suppress dendrite formation from causing a short circuit. The developed CMC/PNiPAM20 based SPE is a promising material for high ionic conductivity and stability in a Zn ion battery.

With the development of flexible and wearable electronic devices, it is a new challenge for polymer hydrogel electrolytes to combine high mechanical flexibility and electrochemical performance into one membrane. In general, the high content of water in hydrogel electrolyte membranes always leads to poor mechanical strength, and limits their applications in flexible energy storage devices. In this work, based on the "salting out" phenomenon in Hofmeister effect, a kind of gelatin-based hydrogel electrolyte membrane is fabricated with high mechanical strength and ionic conductivity by soaking pre-gelated gelatin hydrogel in 2 m ZnSO4 aqueous. Among various gelatin-based electrolyte membranes, the gelatin-ZnSO4 electrolyte membrane delivers the "salting out" property of Hofmeister effect, which improves both the mechanical strength and electrochemical performance of gelatin-based electrolyte membranes. The breaking strength reaches 1.5 MPa. When applied to supercapacitors and zinc-ion batteries, it can sustain over 7500 and 9300 cycles for repeated charging and discharging processes. This study provides a very simple and universal method to prepare polymer hydrogel electrolytes with high strength, toughness, and stability, and its applications in flexible energy storage devices provide a new idea for the construction of secure and stable flexible and wearable electronic devices.

As an earth‐abundant and natural biopolymer, cellulose has received significant attention in aqueous zinc‐ion batteries (AZIBs) due to its inherent sustainability and non‐toxicity, aligning perfectly with the core advantages of AZIBs. Nevertheless, the practical implementation of cellulose‐based materials is limited by their intrinsically low ionic conductivity. Herein, we introduce a novel zincophilic artificial protective layer by strategically hybridizing hydroxypropyl cellulose (HPC) with zinc trifluoromethanesulfonate on a zinc metal anode (HZ@Zn). Characterization and calculations demonstrate that the multi‐hydroxyl architecture of HPC constructs hydrogen bond networks, whereas the Zn 2+ ‐coordinated HPC domains function as preferential nucleation sites for zinc deposition. These interactions collectively enhance ion transport and accelerate desolvation kinetics. Additionally, the hybrid layer's mechanical flexibility and interfacial adhesion ensure the integrity of the artificial protective layer during long cycling. Thanks to this synergistic effect, HZ@Zn shows exceptional electrochemical performance, including a low desolvation activation energy of 14.38 kJ mol −1 and ultra‐long cycling stability. Symmetric cells demonstrate exceptional longevity, exceeding 9,500 h at 0.5 mA cm −2 /0.25 mAh cm −2 , whereas HZ@Zn‖PANI full cells maintain 89.8% capacity retention after 4000 cycles at 5 A g −1 . This study establishes biopolymers as versatile platforms for effectively stabilizing the zinc metal anode.

Aqueous zinc‐ion batteries (AZIBs) offer promising prospects for large‐scale energy storage due to their inherent abundance and safety features. However, the growth of zinc dendrites remains a primary obstacle to the practical industrialization of AZIBs, especially under harsh conditions of high current densities and elevated temperatures. To address this issue, a Janus separator with an exceptionally ultrathin thickness of 29 µm is developed. This Janus separator features the bacterial cellulose (BC) layer on one side and Ag nanowires/bacterial cellulose (AgNWs/BC) layer on the other side. High zincophilic property and excellent electric/thermal conductivity of AgNWs make them ideal for serving as an ion pump to accelerate Zn2+ transport in the electrolyte, resulting in greatly improved Zn2+ conductivity, deposition of homogeneous Zn nuclei, and dendrite‐free Zn. Consequently, the Zn||Zn symmetrical cells with the Janus separator exhibit a stable cycle life of over 1000 h under 80 mA cm−2 and are sustained for over 600 h at 10 mA cm−2 under 50 °C. Further, the Janus separator enables excellent cycling stability in AZIBs, aqueous zinc‐ion capacitors (AZICs), and scaled‐up flexible soft‐packaged batteries. This study demonstrates the potential of functional separators in promoting the application of aqueous zinc batteries, particularly under harsh conditions.

Zinc (Zn) metal anode suffers from uncontrollable Zn dendrites and parasitic side reactions at the interface, which restrict the practical application of aqueous rechargeable zinc batteries (ARZBs). Herein, an amphoteric cellulose-based double-network is introduced as hydrogel electrolyte to overcome these obstacles. On one hand, the amphoteric groups build anion/cation transport channels to regulate electro-deposition behavior on Zn (002) crystal plane enabled by homogenizing Zn2+ ions flux. On the other hand, the strong bonding between negatively charged carboxyl groups and Zn2+ ions promote the desolvation process of [Zn(H2O)6]2+ to eliminate side reactions. Based on the above two functions, the hydrogel electrolyte enables an ultra-stable cycling with a cumulative capacity of 7 Ah cm-2 at 20 mA cm-2/20 mAh cm-2 for Zn||Zn cell. This work provides significant concepts for developing hydrogel electrolytes to realize stable anode for high-performance ARZBs.

A nano-Zn2SnO4 (ZTO)/cellulose acetate (CA) hybrid coating (CZ) was designed for Zn anodes via a DFT-guided synthesis. DFT calculations revealed ZTO's Zn2+-selectivity and low migration barriers, enabling dual ion-sieving and acceleration effects. The C═O groups in CA formed Lewis acid-base pairs with desolvated Zn2+ and ZTO, synergistically regulating ion flux. The CZ coating combined superior film-forming ability with high Zn affinity, suppressing side reactions while homogenizing Zn2+ deposition. As a result, CZ-Zn anodes achieved stable cycling for 3000 h at 5 mA cm-2. Full cells paired with NH4V4O10 cathodes exhibited extended cyclability and enhanced rate performance. This work provides a universal strategy for Zn anode protection through multifunctional hybrid coatings.

The severe hydrogen evolution reaction and parasitic side reaction on Zn anode are the key issues which hinder the development of aqueous Zn-based energy storage devices. Herein, a polyacrylamide/carboxylated cellulose nanofibers/betaine citrate supramolecular zwitterionic hydrogels with molecular slip effects are proposed for enhancing Zn2+ diffusion and protecting Zn anodes. Non-covalent interactions within supramolecular hydrogels forms the skeleton for molecular slip and the strong coordination of carboxyl and amino groups with Zn2+ further facilitates the rapid Zn2+ transfer. Additionally, anchoring carboxyl and amino groups at the anode promotes the uniform deposition of Zn2+and protects Zn anode. On the basis of molecular slip mechanism and anchoring effect in the supramolecular zwitterionic hydrogels, Zn||Zn symmetric batteries undergo 800 h of stable electroplating stripping at a depth of discharge of 80 %. Zn||Cu asymmetric batteries exhibit an impressive average coulombic efficiency of 99.4 % over a remarkable span of 900 cycles at a current density of 15 mA cm-2. Furthermore, Zn||NH4V4O10 batteries successfully undergo over 1,000 cycles at a current density of 0.5 A g-1. Intrinsic ion diffusion mechanism of supramolecular hydrogel electrolytes provides an original strategy for the application of high-performance Zn-based energy storage devices.

A sustainable dual cross-linked cellulose hydrogel with excellent mechanical strength was fabricated from aqueous alkali hydroxide/urea solution using a sequential chemical and physical cross-linking strategy. The hydrogel electrolyte effectively suppresses dendrites growth and side reactions to achieve a stable Zn anode (over 2000 h for Zn||Zn cell), which are proved by a multi-perspective and in-depth mechanism investigation. The hydrogel electrolyte is easily accessible and biodegradable, making the zinc batteries attractive in terms of scalability and sustainability. A sustainable dual cross-linked cellulose hydrogel with excellent mechanical strength was fabricated from aqueous alkali hydroxide/urea solution using a sequential chemical and physical cross-linking strategy. The hydrogel electrolyte effectively suppresses dendrites growth and side reactions to achieve a stable Zn anode (over 2000 h for Zn||Zn cell), which are proved by a multi-perspective and in-depth mechanism investigation. The hydrogel electrolyte is easily accessible and biodegradable, making the zinc batteries attractive in terms of scalability and sustainability. Aqueous rechargeable Zn-metal batteries (ARZBs) are considered one of the most promising candidates for grid-scale energy storage. However, their widespread commercial application is largely plagued by three major challenges: The uncontrollable Zn dendrites, notorious parasitic side reactions, and sluggish Zn2+ ion transfer. To address these issues, we design a sustainable dual cross-linked cellulose hydrogel electrolyte, which has excellent mechanical strength to inhibit dendrite formation, high Zn2+ ions binding capacity to suppress side reaction, and abundant porous structure to facilitate Zn2+ ions migration. Consequently, the Zn||Zn cell with the hydrogel electrolyte can cycle stably for more than 400 h under a high current density of 10 mA cm−2. Moreover, the hydrogel electrolyte also enables the Zn||polyaniline cell to achieve high-rate and long-term cycling performance (> 2000 cycles at 2000 mA g−1). Remarkably, the hydrogel electrolyte is easily accessible and biodegradable, making the ARZBs attractive in terms of scalability and sustainability.

Aqueous zinc batteries (AZBs) are considered one of the most promising candidates for grid‐scale energy storage. However, achieving a stable electrode–electrolyte interface remains a challenge for developing high‐performance AZBs. Herein, taking the Zn||phenazine (PNZ) system as a prototype, where the proton uptake/removal mechanism dominates in the cathode, a carboxylic acid‐functionalized cellulose hydrogel electrolyte is designed to simultaneously solve the issues at both the anode and cathode interfaces. Specifically, the hydrogel electrolyte can not only regulate Zn2+ ions at the Zn anode side but also supply H+ ions at the PNZ cathode side to avoid the unfavored deposition of zinc sulfate hydroxides. Benefiting from the unique one‐gel‐for‐two‐electrodes strategy, the dendrite‐free and side reaction‐suppressed aqueous Zn||PNZ cells are developed with a high specific capacity (311 mAh g−1, 99% utilization of the theoretical capacity) and a long cycle life (over 1500 cycles within 2 months). This study proposes a facile and low‐cost electrolyte strategy for stabilizing AZBs.

Notorious zinc dendrite growth and hydrogen precipitation reactions disrupt the galvanic/stripping process at the electrolyte/electrode interface, which seriously affects the cycling stability of zinc anodes in aqueous zinc ion batteries. To improve the stability and reversibility of zinc anodes, we report an artificial SEI consisting of hydrophobic carbon nanocrystals and highly conductive carbon nanotube networks. This interfacial hydrophobicity effectively excludes free water from the surface of the zinc anode, which prevents water erosion and reduces the interfacial side reactions, resulting in a significant improvement in the cycling stability and coulombic efficiency of Zn plating/stripping. Benefiting from the reversible proton storage and fast desolvation kinetic behavior of the CNC/CNT interlayer, the stable cycling time of Zn/Zn symmetric batteries exceeds 700 h even at a high current density of 5 mA cm-2. The assembled CNC/CNT@Zn‖V2O5 full cell maintains a high capacity of 101.1 mA h g-1 after 5000 cycles (1.0 mA g-1). This study opens up a new area for expanding the use of organic compounds in zinc anode protection and offers a promising strategy for accelerating the development of aqueous zinc-ion batteries.

Aqueous zinc-ion batteries (AZIBs), one of the most promising renewable energy storage devices, are largely impeded by the disreputable cycling stability in its large-scale application as a result of the undesirable Zn dendrites growth and the side reactions. In this context, a carboxylate (-COO-) anionic group functionalized cellulose nanofibrils separator (A-CNF) with nanoporous structure and ion-sieving effect is developed to realize a stable Zn anode without dendrites and by-products. An increased Zn2+ transference number and uniform Zn deposition can be achieved through the electrostatic adsorption between -COO- and Zn2+. More importantly, the synergistic effect between -COO- and hydroxyl group (-OH) in the cellulose nanofibrils separator inhibits the occurrence of side reactions caused by SO42- and free water molecules. As a result, the nanoporous separator consisting of carboxylated cellulose nanofibrils enables Zn anode with high stability and utilization, exhibiting a stable cycling life for 950 h in Zn//Zn cell and an admirable coulombic efficiency of 98.9 % after 300 cycles in Zn//Cu cell. The assembled Zn//MnO2 full cell with the nanoporous cellulose nanofibrils-based separator shows exceptional cyclability and capacity retention after 1000 cycles. This work provides a valuable and practical separator for high performance AZIBs, which might spur its practical application.

Uneven zinc (Zn) deposition typically leads to uncontrollable dendrite growth, which renders an unsatisfactory cycling stability and Coulombic efficiency (CE) of aqueous zinc ion batteries (ZIBs), restricting their practical application. In this work, a lightweight and flexible three-dimensional (3D) carbon nanofiber architecture with uniform Zn seeds (CNF-Zn) is prepared from bacterial cellulose (BC), a kind of biomass with low cost, environmental friendliness, and abundance, as a host for highly reversible Zn plating/stripping and construction of high-performance aqueous ZIBs. The as-prepared 3D CNF-Zn with a porous interconnected network significantly decreases the local current density, and the functional Zn seeds provide uniform nuclei to guide the uniform Zn deposition. Benefiting from the synergistic effect of Zn seeds and the 3D porous framework in the flexible CNF-Zn host, the electrochemical performance of the as-constructed ZIBs is significantly improved. This flexible 3D CNF-Zn host delivers a high and stable CE of 99.5% over 450 cycles, ensuring outstanding rate performance and a long cycle life of over 500 cycles at 4 A g-1 in the CNF-Zn@Zn//NaV3O8·1.5H2O full battery. More importantly, owing to the flexibility of the 3D CNF-Zn host, the as-assembled pouch cell shows outstanding mechanical flexibility and excellent energy storage performance. This strategy of producing readily accessible carbon from biomass can be employed to develop advanced functional nanomaterials for next-generation flexible energy storage devices.

Aqueous zinc‐iodine batteries (ZIBs) have attracted extensive attention due to their advantages of high theoretical specific capacity, abundant reserves, high safety, and low cost, while the Zn anodes are still suffering from dendrite growth, side reactions, and polyiodide corrosion, seriously affecting the service life of ZIBs. Herein, sulfonated cellulose acetate (SCA) nanofiber membrane with zincophilic‐hydrophobic property is constructed on the Zn anode as a protective layer by electrospinning to circumvent the above problems and achieve a stable Zn anode. Attributing to both the hydrophobicity and zincophilicity, the SCA nanofiber membrane not only reduces the activity of water but also promotes the Zn2+ desolvation. Moreover, negatively‐charged groups of the SCA nanofiber membrane cause electrostatic repulsion with polyiodide. Density functional theory calculations and COMSOL simulations further reveal that the SCA nanofiber membrane can tune the uniform 3D deposition behavior of Zn2+ by chemisorption and physical structure, respectively. The obtained ZIBs can achieve ultra‐long life span (> 13000 cycles) with high‐capacity retention (96.74%) and reversibility (average CE: 99.83%), demonstrating the reliability of our proposed strategy for achieving stable and high‐performance ZIBs.

Aqueous zinc ion batteries (AZIBs) hold enormous potential as novel energy devices in light of their high safety, reasonable cost, and eco‐economic. While their application on a wide scale is restricted by the notorious dendrite growth and side reactions at the Zn anode/electrolyte interface. Herin, a dynamic regulation of interfacial micro‐environment strategy is proposed, introducing a green and safe hydroxyethyl cellulose (HEC) electrolyte additive to build highly stable and reversible Zn anode. Experiment and calculation results demonstrate that HEC can preferentially adsorb on Zn anode surface and create an HEC‐rich transition layer in inner Helmholtz plane (IHP) during plating/stripping. This layer can shield the parasitic reactions induced by active water and facilitate Zn uniform deposition. Meanwhile, HEC can reconstruct the Zn 2+ solvation sheath in outer Helmholtz plane (OHP), which accelerates Zn 2+ desolvation kinetics. Consequently, the Zn//Zn cells containing HEC electrolyte additive cycle stably for 2300 h and over 350 h at 1 and 30 mA cm −2 , respectively. It also endows Zn anode with excellent reversibility, maintaining high Coulombic efficiency of 99.4% over 600 cycles. After 3000 cycles, the Zn//AC@MnO 2 full cell with HEC electrolyte additive continues to exhibit outstanding cycling performance, retaining 85.2% of its initial capacity.

Zinc (Zn) metal is considered a potential anode owing to its high theoretical capacity, safety, and low cost. However, the dendrites and corresponding side reactions in aqueous electrolytes hinder their further development in environmentally-friendly energy storage. Herein, ion-affiliative cellulose acetate (CA) coating with Zn(CF3 SO3 )2 is constructed on Zn anode (CAZ@Zn). Owing to the complexation effect between the polar ester group (CO) and Zn salt (Zn2+ ), the CAZ polymer coating enhances the hydrophilicity of the Zn anode and reduces the interfacial resistance, allowing the rapid Zn2+ diffusion and homogenizing the Zn deposition in an aqueous electrolyte to suppress zinc dendrite formation and growth. Therefore, the symmetric CAZ@Zn//CAZ@Zn battery achieves reversible plating/stripping over 2800 h at 1 mA cm-2 with 1 mAh cm-2 , about sevenfold higher than bare Zn. The full cell fabricated with an optimized Zn anode and the NH4 V4 O10 cathode achieves substantially stable performance, superior to that of bare Zn. This work provides a straightforward, effective, and scalable method to suppress the zinc dendrites and corresponding side reactions for aqueous Zn-ions batteries.

The uncontrolled dendrite growth and detrimental parasitic reactions of Zn anodes currently impede the large-scale implementation of aqueous zinc ion batteries. Here, we design a versatile quasi-solid-state polymer electrolyte with highly selective ion transport channels via molecular crosslinking of sodium polyacrylate, lithium magnesium silicate and cellulose nanofiber. The abundant negatively charged ionic channels modulate Zn2+ desolvation process and facilitate ion transport. Moreover, an in-situ formed Zn-Mg-Si medium-entropy alloy on Zn anode allows for an improved Zn nucleation kinetics and homogeneous Zn deposition. These combined advantages of the polymer electrolyte enable Zn anodes to achieve an average Coulombic efficiency of 99.7 % over 2400 cycles and highly reversible cycling up to 600 h with large depth of discharge of 85.6%. The resultant Zn | |V2O5 offers a stable long-term cycling performance and its pouch cell achieves a cycling capacity of 1.13 Ah at industrial-level loading mass of 31.3 mg. The dendrite growth and parasitic reactions on Zn anodes pose significant challenges for the application of aqueous zinc-ion batteries. Here, the authors report a versatile quasi solid-state polymer electrolyte engineered with abundant ion transport channels for enhanced zinc ion battery performance.

Aqueous zinc-ion batteries (AZIBs) are renowned for their exceptional safety and eco-friendly design, are being considered as a prospective option for emerging energy storage technologies. However, the selected Zn foil as the anode material in existing AZIBs encounters significant challenges, including dendrite formation due to uneven zinc deposition/stripping, and undesirable side reactions. These issues considerably degrade the lifespan and capacity of the battery, thereby impeding its practical application and commercialization. To address these problems, this research introduces a highly stable Zn@CNF anode for AZIBs by using carboxylated cellulose nanofibers (CNFs) as a protective coating. Under consistent testing conditions, the symmetric batteries of Zn@CNF maintain stable Zn deposition/stripping behavior for 500 h, while the unprotected Zn symmetric batteries fail after merely 100 h. Additionally, during full-cell evaluations, the Zn@CNF||MnO₂ batteries increase capacity compared to Zn||MnO₂ battery. This approach offers a practical way for developing highly stable Zn anodes.

Though considered as a highly promising energy storage technology, aqueous zinc-ion batteries (AZIBs) still face challenges such as poor cycling stability and low coulombic efficiency (CE) due to side reactions and dendrite growth on the Zn anode surface during electrochemical processes. To overcome the above issues, commercial cosmetic cotton (CP) was functionalized using polyvinylidene fluoride (PVDF) to fabricate a PVDF-CP composite separator. CP (the main component being cellulose) exhibits high porosity, excellent mechanical properties and low price, and the cheap PVDF plays bifunctional roles in stabilizing the Zn anode interface. The β-phase PVDF in the separator forms a uniform electronegative region, endowing the separator with outstanding functionality: it constructs Zn2+ transport channels and thus accelerates ion migration, as well as restricting the disordered diffusion of Zn2+, which effectively boosts Zn deposition kinetics. Furthermore, the PVDF-CP separator inherits PVDF's hydrophobicity and establishes a stable hydrophobic interface that can prevent water from accessing the Zn electrode, thereby significantly alleviating water-induced parasitic reactions. Consequently, the multifunctional synergistic effects of the PVDF-CP composite separator observably promote the electrochemical performance of AZIBs, and Zn∥Zn symmetric cells assembled with the PVDF-CP separator obtain a cycling lifespan of over 2810 h. Zn∥Cu asymmetric cells demonstrate 1000 reversible cycles with a high average CE of 99.0%, showcasing the stable Zn plating/stripping behavior. Besides, Zn∥NVO full cells exhibit exceptional cycling stability, retaining 88.0% capacity (155.0 mAh g-1) after 2300 cycles at 5 A g-1.

No abstract available