Rechargeable Aqueous Zinc-ion Batteries Research Articles

Machine-Learning-Assisted Development of Gel Polymer Electrolytes for Protecting Zn Metal Anodes from the Corrosion of Water Molecules.

Rechargeable aqueous zinc-ion batteries (RAZIBs) offer low cost, high energy density, and safety but struggle with anode corrosion and dendrite formation. Gel polymer electrolytes (GPEs) with both high mechanical properties and excellent electrochemical properties are a powerful tool to aid the practical application of RAZIBs. In this work, guided by a machine learning (ML) model constructed based on experimental data, polyacrylamide (PAM) with a highly entangled structure was chosen to prepare GPEs for obtaining high-performance RAZIBs. By controlling the swelling degree of the PAM, the obtained GPEs effectively suppressed the growth of Zn dendrites and alleviated the corrosion of Zn metal caused by water molecules, thus improving the cycling lifespan of the Zn anode. These results indicate that using ML models based on experimental data can effectively help screen battery materials, while highly entangled PAMs are excellent GPEs capable of balancing mechanical and electrochemical properties.

Improved rate and cycling capability of V2O5@MoS2 nanocomposites as an advanced cathode material for rechargeable aqueous zinc-ion batteries

Owing to the benefits of higher energy density, reliable safety, and eco-friendliness, rechargeable aqueous zinc (Zn)-ion batteries (RAZIBs) are employed in energy storage applications. Nevertheless, the enhancement of potential cathodes is hindered by low reversibility and sluggish Zn-ion diffusion kinetics, causing deficient rate capability and modest cycling performance. Vanadic anhydride (V2O5) provides a potential in RAZIBs from its layered structure and superior capacity. Herein, molybdenum disulfide (MoS2) was combined into the V2O5 to form V2O5@MoS2 nanocomposites (NCs) via a simple hydrothermal method. The V2O5@MoS2 NCs enable Zn ions to migrate effectively between layers and stabilize volume changes during the insertion/extraction process. Moreover, the presence of MoS2 as a mediator in the framework produces additional defects, which leads to an enhanced storage area for Zn ions. The optimized V2O5@MoS2–2 NCs exhibited a cycling capacity of 230.74 mA h g−1 at 0.5 A g−1, superior rate performance (73.59 mA h g−1 at 30 A g−1), and excellent long-term cycling stability (108.16 mA h g−1 at 10 A g−1 over 6000 cycles), surpassing those of V2O5@MoS2–1, V2O5@MoS2–3, V2O5, and MoS2 counterparts. Such fascinating properties reveal that the proposed composite materials as a progressive cathode for RAZIBs.

Boosting Zn2+ Intercalation in Manganese Oxides for Aqueous Zinc Ion Batteries via Delocalizing the d-electrons Spin States of Mn Site

Rechargeable aqueous zinc-ion batteries (AZIBs) have received increasing attention on account of their eco-friendliness and low cost. However, the limited capacity and poor rate properties of cathodes remain a major challenge due to the low electrochemical reactivity of cathode materials and sluggish Zn2+ transport kinetics. Herein, we design a 1,5-naphthalenediamine (NAPD) pre-intercalate potassium manganese dioxide (KMO-NAPD) with high capacity and rate capability for AZIBs. The introduction of NAPD can delocalize the d-electrons spin states of the Mn site and activate the reactivity of KMO-NAPD for Zn2+ intercalation. Moreover, the interaction between intercalated Zn2+ and KMO-NAPD is weakened due to the decreased electrostatic interaction force, which promotes the diffusion of Zn2+. Consequently, the KMO-NAPD cathode exhibits high specific capacity (237 mAh g−1 at 1 A g−1) satisfying rate capability (129 mAh g−1 at 4 A g−1), and excellent cycling stability (85% capacity retention after 1000 cycles). Furthermore, the fabricated AZIBs based on the KMO-NAPD exhibit a high energy density of 294.3 Wh kg−1 and a peak power density of 8.6 kW kg−1. This study opens up a new path for the development of high-energy organic-inorganic hybrid cathode materials with modulated electronic structures for advanced AZIBs.

Ethylene Glycol-Choline Chloride Based Hydrated Deep Eutectic Electrolytes Enabled High-Performance Zinc-Ion Battery.

Aqueous rechargeable zinc-ion batteries (ARZIBs) are considered as an emerging energy storage technology owing to their low cost, inherent safety, and reasonable energy density. However, significant challenges associated with electrodes, and aqueous electrolytes restrict their rapid development. Herein, ethylene glycol-choline chloride (Eg-ChCl) based hydrated deep-eutectic electrolytes (HDEEs) are proposed for RZIBs. Also, a novel V10O24·nH2O@rGO composite is prepared and investigated in combination with HDEEs. The formulated HDEEs, particularly the composition of 1ml of EG, 0.5g of ChCl, 4ml of H2O, and 2M ZnTFS (1-0.5-4-2 HDEE), not only exhibit the lowest viscosity, highest Zn2+ conductivity (20.38mScm-1), and the highest zinc (Zn) transference number (t+ = 0.937), but also provide a wide electrochemical stability window (>3.2V vs ZnǁZn2+) and enabledendrite-free Zn stripping/plating cycling over 1000 hours. The resulting ZnǁV10O24·nH2O@rGO cellwith 1-0.5-4-2 HDEE manifests high reversible capacity of ≈365mAhg-1 at 0.1Ag-1, high rate-performance (delivered ≈365/223mAhg-1 at 0.1/10mAg-1) and enhanced cycling performance (≈63.10% capacity retention in the 4000th cycle at 10Ag-1). Furthermore, 1-0.5-4-2 HDEE support feasible Zn-ion storage performance across a wide temperature range (0-80°C) FInally, a ZnǁV10O24·nH2O@rGO pouch-cell prototype fabricated with 1-0.5-4-2 HDEE demonstrates good flexibility, safety, and durability.

Lean-water hydrogel electrolyte with improved ion conductivity for dendrite-free zinc-Ion batteries

Although rechargeable aqueous zinc-ion batteries (ZIBs) are regarded as promising energy storage devices, the uncontrollable Zn dendrite and undesirable side reactions severely limit their practical applications. Herein, an anionic hydrogel electrolyte PAM/SA with 3D porous structures is developed by integrating sodium alginate (SA) and polyacrylamide (PAM) networks for highly reversible Zn plating/stripping. Mechanically enhanced and lean-water PAM/SA hydrogel with anionic chains for constructing ionic channels and molecular lubrication films, which facilitate Zn2+ migration for a high ionic conductivity (5.4 S m−1) and Zn2+ transference number (0.86) even under lean-water conditions (about 60%). Based on the experimental and theoretical analysis, the SA chain with strong coordination ability endows PAM/SA with improved desolvation kinetics and the ability to regulate the electric field intensity at the electrode/electrolyte interface, which is beneficial for suppressing side reactions and facilitating directional Zn deposition. Subsequently, the symmetric Zn//Zn cell based on PAM/SA hydrogel electrolyte delivers stable cycles for over 1800 h. The assembled Zn//V2O5 battery based on PAM/SA reveals a high specific capacity and a long cycle life. This work provides a new insight for developing hydrogel electrolytes with high ionic conductivity and lean-water properties toward stable Zn anode

Rational Design of an In‐Situ Polymer‐Inorganic Hybrid Solid Electrolyte Interphase for Realising Stable Zn Metal Anode under Harsh Conditions

AbstractThe in‐depth understanding of the composition‐property‐performance relationship of solid electrolyte interphase (SEI) is the basis of developing a reliable SEI to stablize the Zn anode‐electrolyte interface, but it remains unclear in rechargeable aqueous zinc ion batteries. Herein, a well‐designed electrolyte based on 2 M Zn(CF3SO3)2‐0.2 M acrylamide‐0.2 M ZnSO4 is proposed. A robust polymer (polyacrylamide)‐inorganic (Zn4SO4(OH)6.xH2O) hybrid SEI is in situ constructed on Zn anodes through controllable polymerization of acrylamide and coprecipitation of SO42− with Zn2+ and OH−. For the first time, the underlying SEI composition‐property‐performance relationship is systematically investigated and correlated. The results showed that the polymer‐inorganic hybrid SEI, which integrates the high modulus of the inorganic component with the high toughness of the polymer ingredient, can realize high reversibility and long‐term interfacial stability, even under ultrahigh areal current density and capacity (30 mA cm−2~30 mAh cm−2). The resultant Zn||NH4V4O10 cell also exhibits excellent cycling stability. This work will provide a guidance for the rational design of SEI layers in rechargeable aqueous zinc ion batteries.

Solvothermal Guided V2O5 Microspherical Nanoparticles Constructing High-Performance Aqueous Zinc-Ion Batteries.

Rechargeable aqueous zinc-ion batteries have attracted a lot of attention owing to their cost effectiveness and plentiful resources, but less research has been conducted on the aspect of high volumetric energy density, which is crucial to the space available for the batteries in practical applications. In this work, highly crystalline V2O5 microspheres were self-assembled from one-dimensional V2O5 nanorod structures by a template-free solvothermal method, which were used as cathode materials for zinc-ion batteries with high performance, enabling fast ion transport, outstanding cycle stability and excellent rate capability, as well as a significant increase in tap density. Specifically, the V2O5 microspheres achieve a reversible specific capacity of 414.7 mAh g-1 at 0.1 A g-1, and show a long-term cycling stability retaining 76.5% after 3000 cycles at 2 A g-1. This work provides an efficient route for the synthesis of three-dimensional materials with stable structures, excellent electrochemical performance and high tap density.

A Pyrophosphate Bifunctional Cathode with Inductive Effect for High-Voltage and Self-Charging Zinc Ion Battery.

With the growing demand for new energy storage devices, rechargeable aqueous zinc ion batteries (ZIBs) have attracted widespread attention due to their low cost and high safety. Among the cathode materials for ZIBs, polyanionic-based cathode materials with high voltage, high stability, and low cost have great potential. In this paper, tetragonal Na2VOP2O7 was prepared using a simple sol-gel method. The discharge platform voltage amounted to 1.8 V and had good rate and cycle performance due to the inductive effect of pyrophosphate. Then, a protective layer of Zn-hydroxyapatite (ZnHAP) modification was applied to the cathode surface, which can inhibit the hydrolysis of vanadium ions. The capacity was enhanced by 19% after modification and the capacity retention after 100 cycles was also higher. Interestingly, the Na2VOP2O7 cathode also possesses a self-charging effect, recovering to 48% of its initial capacity with an open-circuit voltage (OCV) of 1.1 V within a certain period, and light exposure can reduce the self-charging time by 83%. These beneficial results indicate that the pyrophosphate bifunctional cathode with inductive effect has a great potential to construct high-voltage and multifunctional zinc ion battery.

Achieving Long-Cycle-Life Zinc-Ion Batteries through a Zincophilic Prussian Blue Analogue Interphase.

The practical application of rechargeable aqueous zinc-ion batteries (ZIBs) has been severely hindered by detrimental dendrite growth, uncontrollable hydrogen evolution, and unfavorable side reactions occurring at the Zn metal anode. Here, we applied a Prussian blue analogue (PBA) material K2Zn3(Fe(CN)6)2 as an artificial solid electrolyte interphase (SEI), by which the plentiful -C≡N- ligands at the surface and the large channels in the open framework structure can operate as a highly zincophilic moderator and ion sieve, inducing fast and uniform nucleation and deposition of Zn. Additionally, the dense interface effectively prevents water molecules from approaching the Zn surface, thereby inhibiting the hydrogen-evolution-resultant side reactions and corrosion. The highly reversible Zn plating/stripping is evidenced by an elevated Coulombic efficiency of 99.87% over 600 cycles in a Zn/Cu cell and a prolonged lifetime of 860 h at 5 mA cm-2, 2 mAh cm-2 in a Zn/Zn symmetric cell. Furthermore, the PBA-coated Zn anode ensures the excellent rate and cycling performance of an α-MnO2/Zn full cell. This work provides a simple and effective solution for the improvement of the Zn anode, advancing the commercialization of aqueous ZIBs.

Rational Design of an In-Situ Polymer-Inorganic Hybrid Solid Electrolyte Interphase for Realising Stable Zn Metal Anode under Harsh Conditions.

The in-depth understanding of the composition-property-performance relationship of solid electrolyte interphase (SEI) is the basis of developing a reliable SEI to stablize the Zn anode-electrolyte interface, but it remains unclear in rechargeable aqueous zinc ion batteries. Herein, a well-designed electrolyte based on 2 M Zn(CF3SO3)2-0.2 M acrylamide-0.2 M ZnSO4 is proposed. A robust polymer (polyacrylamide)-inorganic (Zn4SO4(OH)6.xH2O) hybrid SEI is in situ constructed on Zn anodes through controllable polymerization of acrylamide and coprecipitation of SO4 2- with Zn2+ and OH-. For the first time, the underlying SEI composition-property-performance relationship is systematically investigated and correlated. The results showed that the polymer-inorganic hybrid SEI, which integrates the high modulus of the inorganic component with the high toughness of the polymer ingredient, can realize high reversibility and long-term interfacial stability, even under ultrahigh areal current density and capacity (30 mA cm-2~30 mAh cm-2). The resultant Zn||NH4V4O10 cell also exhibits excellent cycling stability. This work will provide a guidance for the rational design of SEI layers in rechargeable aqueous zinc ion batteries.

Heterojunction tunnelled vanadium-based cathode materials for high-performance aqueous zinc ion batteries

Rechargeable aqueous zinc ion batteries (ZIBs) have emerged as a promising alternative to lithium-ion batteries due to their inherent safety, abundant availability, environmental friendliness and cost-effectiveness. However, the cathodes in ZIBs encounter challenges such as structural instability, low capacity, and sluggish kinetics. In this study, we constructed BiVO4@VO2 (BVO@VO) heterojunction cathode material with bismuth vanadate and vanadium dioxide phases for ZIBs, which demonstrate significant advancements in both aqueous and quasi-solid-state ZIBs. Benefitting from the heterojunction structure, the materials present a high capacity of 262 mAh g−1 at 0.1 A g−1, superb cyclic stability with 96% capacity retention after 1000 cycles at 2 A g−1, and outstanding rate property with a specific capacity of 218 mAh g−1 even at a high rate of 5.0 A g−1. Furthermore, the flexible quasi-solid-state ZIBs incorporating the BVO@VO cathode demonstrate prolonged cyclic life performance with a remarkable specific capacity of 234 mAh g−1 over 100 cycles at a current density of 0.1 A g−1. This study potentially paves the way for the utilization of heterointerface-enhanced zinc ion diffusion for vanadium-based materials in ZIBs, thereby providing a new approach for the design and investigation of high-performance zinc-ion systems.

Fabricating composites of multicomponent active substances embedded in carbon matrix for enhancing structural stability and redox kinetics of cathode in aqueous zinc-ion batteries

Rechargeable aqueous zinc-ion batteries (ZIBs) are recognized as a potential candidate for large-scale energy storage due to its high-security and low-expense aspects. However, the poor structural stability and sluggish redox kinetics of cathode material lead to the serious capacity fading and bad rate performances, which hinders its practical applications. Herein, a novel one-step pyrolysis strategy is conducted for fabricating the composites of multicomponent active substances (including WO3, Bi and Bi2O3) embedded in amorphous N-doped carbon matrix (BWO@C) using polydopamine-coated Bi2WO6 micro-flowers as the precursors. The amorphous nitrogen-doped carbon endows BWO@C composite to possess more active-sites and higher electrical conductivity for rapid electrons/ions transport, and meanwhile the active substances could be effectively utilized even undergoing thousands of charge/discharge cycles. Therefore, the resulting BWO@C as cathode for aqueous ZIBs exhibits satisfying rate performances as well as outstanding cycling stability. This work provides a simple and efficient pathway for designing the cathode materials with high conductivity and high structural stability to achieve remarkable performances and long life-span of aqueous ZIBs.

CoNi hexacyanoferrate nanoparticles anchored on carbon nanotubes as superior cathode materials for rechargeable aqueous zinc-ion batteries

Prussian blue analogues (PBAs) have attracted growing interest as competitive cathode materials for aqueous zinc-ion batteries (AZIBs). However, their low conductivity and easy structural collapse often lead to poor reversible capacity and cyclability. Herein, cobalt‑nickel hexacyanoferrate (CoNiHCF), a CoNi-Prussian blue analogue, are designed as AZIBs cathode materials for the first time, in which highly uniform CoNiHCF nanocubes are in-situ decorated on carbon nanotubes (CNTs) via a simple co-precipitation method. The resulted CoNiHCF/CNTs composite displays superior zinc ion storage performance, with a great reversible capacity of 124.9 mAh g−1 at the current density of 50 mA g−1, and a high capacity retention of 81.8 % at 3000 mA g−1 for 1000 cycles, which are remarkably superior to those of CoHCF, NiHCF and CoNiHCF. The excellent Zn2+ storage properties of CoNiHCF/CNTs can be ascribed to the bimetallic synergistic effect of Co and Ni as well as the introduction of conductive CNTs skeleton. This study offers a straightforward and efficient method for promoting the application of PBAs-based cathodes in AZIBs.

The Compatibility of COFs Cathode and Optimized Electrolyte for Ultra-Long Lifetime Rechargeable Aqueous Zinc-Ion Battery.

Rechargeable aqueous zinc-ion batteries (RAZIBs) are attractive due to their affordability, safety, and eco-friendliness. However, their potential is limited by the lack of high-capacity cathodes and compatible electrolytes needed for reliable performance. Herein, we have presented a compatibility strategy for the development of a durable and long-lasting RAZIBs. The covalent organic frameworks (COFs) based on anthraquinone (DAAQ-COF) is created and utilized as the cathode, with zinc metal serving as the anode. The electrolyte is made up of an aqueous solution containing zinc salts at various concentrations. The COF cathode has been designed to be endowed with a rich array of redox-active groups, enhancing its electrochemical properties. Meanwhile, the electrolyte is formulated using triflate anions, which have exhibited superiority over sulfate anions. This strategy lead to the development of an optimized COF cathode with fast charging capability, high Coulombic efficiency (nearly 100 %) and long-term cyclability (retention rate of nearly 100 % at 1 A g-1 after 10000 cycles). Moreover, through experimental analysis, a co-insertion mechanism involving Zn2+ and H+ in this cathode is discovered for the first time. These findings represent a promising path for the advancement of organic cathode materials in high-performance and sustainable RAZIBs.

Dual-Parasitic Effect Enables Highly Reversible Zn Metal Anode for Ultralong 25,000 Cycles Aqueous Zinc-Ion Batteries.

The use of electrolyte additives is an efficient approach to mitigating undesirable side reactions and dendrites. However, the existing electrolyte additives do not effectively regulate both the chaotic diffusion of Zn2+ and the decomposition of H2O simultaneously. Herein, a dual-parasitic method is introduced to address the aforementioned issues by incorporating 1-ethyl-3-methylimidazolium trifluoromethanesulfonate ([EMIm]OTf) as cosolvent into the Zn(OTf)2 electrolyte. Specifically, the OTf- anion is parasitic in the solvent sheath of Zn2+ to decrease the number of active H2O. Additionally, the EMIm+ cation can construct an electrostatic shield layer and a hybrid organic/inorganic solid electrolyte interface layer to optimize the deposition behavior of Zn2+. This results in a Zn anode with a reversible cycle life of 3000 h, the longest cycle life of full cells (25,000 cycles), and an extremely high initial capacity (4.5 mA h cm-2), providing a promising electrolyte solution for practical applications of rechargeable aqueous zinc-ion batteries.

Achieving Dendrite-Free Zinc Metal Anodes via Molecule Anchoring and lon-Transport pumping.

The potential for scale-up application has been acknowledged by researchers for rechargeable aqueous zinc-ion batteries (ZIBs). Nonetheless, the progress of the development is significantly impeded due to the instability of the interface between the zinc anode and electrolyte. Herein, efficient and environmentally benign valine (Val) were introduced as aqueous electrolyte additive to stabilize the electrode/electrolyte interface (EEI) via functional groups in additive molecules, thus achieving reversible dendrite-free zinc anode. The amino groups present in Val molecules have a strong ability to adsorb on the surface of zinc metal, enabling the construction of anchored molecular layer on the surface of zinc anodes. The strongly polar carboxyl groups in Val molecules can act as ion-transport pumps to capture zinc ions in the double electrical layer (DEL) through coordination chemistry. Therefore, this reconstructed EEI could modulate the zinc ion flux and simultaneously suppress side reactions and dendritic growth of Zn. Consequently, a long stable cycling up to 1400 h at a high current density of 20 mA cm-2 is achieved. Additionally, Zn//V2O5 full cell with Val additive exhibit enhanced cyclability, retaining 77% capacity after 3000 cycles, displaying significant potential in promoting the commercialization of ZIBs.

Polypyrrole pre-intercalation engineering-induced NH4+ removal in tunnel ammonium vanadate toward high-performance zinc ion batteries

Ammonium vanadate with stable bi-layered structure and superior mass-specific capacity have emerged as competitive cathode materials for aqueous rechargeable zinc-ion batteries (AZIBs). Nevertheless, fragile NH…O bonds and too strong electrostatic interaction by virtue of excessive NH4+ will lead to sluggish Zn2+ ion mobility, further largely affects the electro-chemical performance of ammonium vanadate in AZIBs. The present work incorporates polypyrrole (PPy) to partially replace NH4+ in NH4V4O10 (NVO), resulting in the significantly enlarged interlayers (from 10.1 to 11.9 Å), remarkable electronic conductivity, increased oxygen vacancies and reinforced layered structure. The partial removal of NH4+ will alleviate the irreversible deammoniation to protect the laminate structures from collapse during ion insertion/extraction. The expanded interlayer spacing and the increased oxygen vacancies by the virtue of the introduction of polypyrrole improve the ionic diffusion, enabling exceptional rate performance of NH4V4O10. As expected, the resulting polypyrrole intercalated ammonium vanadate (NVOY) presents a superior discharge capacity of 431.9 mAh g−1 at 0.5 A g−1 and remarkable cycling stability of 219.1 mAh g−1 at 20 A g−1 with 78 % capacity retention after 1500 cycles. The in-situ electrochemical impedance spectroscopy (EIS), in-situ X-ray diffraction (XRD), ex-situ X-ray photoelectron spectroscopy (XPS) and ex-situ high resolution transmission electron microscopy (HR-TEM) analysis investigate a highly reversible intercalation Zn-storage mechanism, and the enhanced the redox kinetics are related to the combined effect of interlayer regulation, high electronic conductivity and oxygen defect engineering by partial substitution NH4+ of PPy incorporation.

Gyroid Liquid Crystals as Quasi-Solid-State Electrolytes Toward Ultrastable Zinc Batteries.

The potential for optimizing ion transport through triply periodic minimal surface (TPMS) structures renders promising electrochemical applications. In this study, as a proof-of-concept, we extend the inherent efficiency and mathematical beauty of TPMS structures to fabricate liquid-crystalline electrolytes with high ionic conductivity and superior structural stability for aqueous rechargeable zinc-ion batteries. The specific topological configuration of the liquid-crystalline electrolytes, featuring a Gyroid geometry, enables the formation of a continuous ion conduction pathway enriched with confined water. This, in turn, promotes the smooth transport of charge carriers and contributes to high ionic conductivity. Meanwhile, the quasi-solid hydrophobic phase assembled by hydrophobic alkyl chains exhibits notable rigidity and toughness, enabling uniform and compact dendrite-free Zn deposition. These merits synergistically enhance the overall performance of the corresponding full batteries. This work highlights the distinctive role of TPMS structures in developing high-performance, liquid-crystalline electrolytes, which can provide a viable route for the rational design of next-generation quasi-solid-state electrolytes.

Trifunctional Rb+-Intercalation Enhancing the Electrochemical Cyclability of Ammonium Vanadate Cathode for Aqueous Zinc Ion Batteries.

Rechargeable aqueous zinc-ion batteries (AZIBs) have been highly desired due to their low cost, intrinsic safety, environmental friendliness, and great potential in large-scale power storage systems. However, their practical applications are impeded by unstable long-term electrochemical performances induced by microstructure degradation of the cathode material, hydrogen evolution reaction in the electrolyte, and dendritic growth on the zinc anode upon cycling. In this work, rubidium cations (Rb+) are introduced to synthesize an Rb+-preintercalated NH4V4O10 (NVO-Rb) composite. The contribution of Rb+ ions as pillars in V-O interlayers to facilitating Zn2+ storage is investigated first, and then the influences of partial Rb+ ions from the NVO-Rb cathode on the aqueous electrolyte and zinc anode are specially inspected from different viewpoints. Based on a series of characterization results, it is comprehensively elucidated that the partial Rb+ ions into the electrolyte suppress the generation of byproducts on the cathode and regulate the dendrite growth on the zinc anode, thus effectively promoting the long-term electrochemical performances of NVO-based AZIBs. The assembled Zn∥Zn(CF3SO3)2∥NVO-Rb cell can exhibit a high specific capacity and optimized Zn2+ diffusion kinetics, especially an improved electrochemical cyclability with a capacity retention of 87.6% at 5 A g-1 over 10000 cycles. This study enlightens the multiple roles of cation-preintercalation in the layered structure material and provides a feasible strategy for the development of high-performance aqueous batteries.

Constructing a rapid ion-transport anode interface protective layer for zinc ion batteries to suppress solvation and improve surface electronic structure

Rechargeable Aqueous Zinc-Ion Batteries (AZIBs) have attracted significant attention in recent years due to their high energy density, safety, and cost-effectiveness. However, despite these advantages, AZIBs face challenges such as anode side reactions, passivation, corrosion, hydrogen evolution, and the growth of zinc dendrites, which hinder their widespread use. To address these issues, this study involves the creation of a zinc-affinitive coating using a WSe2/ZIF composite on zinc foils. The amorphous WSe2 protective layer, formed through electrochemical induction as ZnSe, enhances the anode's zinc affinity, accelerates Zn2+ transfer at the interface, and effectively inhibits zinc dendrite growth. Additionally, the coating improves electrolyte wettability, reducing interface resistance. Compared to pure zinc, anodes with a WSe2/ZIF protective layer exhibit excellent performance in both symmetric cells and full-cell systems using MXene/MnO2 as the cathode. Symmetric cells can cycle for over 1000 h at a current density of 5 mA/cm2, and the full cell maintains a capacity retention of 91.4 % after 2000 charge-discharge cycles. This interface engineering strategy, supported by density functional theory calculations, provides a strong foundation for practical applications.