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Aqueous Zn‐ion batteries (AZIBs) are promising energy storage systems due to their low cost, excellent safety, and environmental friendliness. However, challenges like uncontrollable dendrite growth and side reactions during battery operation limit their commercialization. Addressing these issues requires regulating ion deposition behavior at the anode/electrolyte interface. The electrostatic shielding effect, which leverages the interplay between electric potential and ionic motion, provides a unique mechanism to inhibit zinc dendrites and side reactions effectively. Despite significant progress in understanding electrostatic shielding in AZIBs, a comprehensive summary of its effects is still lacking. This paper first reviews the primary challenges in AZIBs and then describes how the electrostatic shielding effect can optimize their performance. Existing strategies for achieving electrostatic shielding through anode structure optimization and electrolyte optimization‐are classified and analyzed. Finally, the review summarizes current electrostatic shielding strategies for stabilizing zinc anodes, identifies existing challenges, and discusses the future potential, and for this approach in AZIBs. [ABSTRACT FROM AUTHOR]

Three dimensional (3D) framework structure is one of the most effective ways to achieve uniform zinc deposition and thus inhibit the Zn dendrites growth in working Zn metallic anode. A major challenge facing for the most commonly used 3D zincophilic hosts is that the zincophilic layer tends to peel off during repeatedly cycling, making it less stable. Herein, for the first time, a hetero‐superlattice Zn/ZnLi (HS−Zn/ZnLi) anode containing periodic arrangements of metallic Zn phase and zincophilic ZnLi phase at the nanoscale, is well designed and fabricated via electrochemical lithiation method. Based on binding energy and stripping energy calculation, and the operando optical observation of plating/stripping behaviors, the zincophilic ZnLi sites with a strong Zn adsorption ability in the interior of the 3D ZnLi framework structure can effectively guide uniform Zn nucleation and dendrite‐free zinc deposition, which significantly improves the cycling stability of the HS−Zn/ZnLi alloy (over 2800 h without a short‐circuit at 2 mA cm−2). More importantly, this strategy can be extended to HS−Zn/ZnNa and HS−Zn/ZnK anodes that are similar to the HS−Zn/ZnLi microstructure, also displaying significantly enhanced cycling performances in AZIBs. This study can provide a novel strategy to develop the dendrite‐free metal anodes with stable cycling performance. [ABSTRACT FROM AUTHOR]

Uncontrollable growth of Zn dendrites, irreversible dissolution of cathode material and solidification of aqueous electrolyte at low temperatures severely restrict the development of aqueous Zn‐ion batteries. In this work, 2,2,2‐trifluoroethanol (TFEA) with a volume fraction of 50% as a highly compatible polar‐solvent is introduced to 1.3 M Zn(CF3SO3)2 aqueous electrolyte, achieving stable high‐performance Zn‐ion batteries. Massive theoretical calculations and characterization analysis demonstrate that TFEA weakens the tip effect of Zn anode and restrains the growth of Zn dendrites due to electrostatic adsorption and coordinate with H2O to disrupt the hydrogen bonding network in water. Furthermore, TFEA increases the wettability of the cathode and alleviates the dissolution of V2O5, thus improving the capacity of the full battery. Based on those positive effects of TFEA on Zn anode, V2O5 cathode, and aqueous electrolyte, the Zn//Zn symmetric cell delivers a long cycle‐life of 782 h at 5 mA cm−2 and 2 mA h cm−2. The full battery still declares an initial capacity of 116.78 mA h g−1, and persists 87.73% capacity in 2000 cycles at −25 °C. This work presents an effective strategy for fully compatible co‐solvent to promote the stability of Zn anode, V2O5 cathode and aqueous electrolyte for high‐performance Zn‐ion batteries. [ABSTRACT FROM AUTHOR]

To construct an efficient regulating layer for Zn anodes that can simultaneously address the issues of dendritic growth and side reactions is highly demanded for stable zinc metal batteries (ZMBs). Herein, we fabricate a hydrogen‐bonded organic framework (HOF) enriched with zincophilic sites as a multifunctional layer to regulate Zn anodes with controlled spatial ion flux and stable interfacial chemistry (MA‐BTA@Zn). The framework with abundant H‐bonds helps capture H2O and remove the solvated shells on [Zn(H2O)6]2+, leading to suppressed side reactions. The HOF layer also helps form electrolyte‐philic surfaces and expose Zn (002) crystal planes which benefit for rapid conduction and uniform deposition of Zn2+, and weakened sides reactions. Additionally, the electrochemically active zincophilic sites (C=O, −NH2 and triazine groups) favor the targeted guidance and penetration of Zn2+ and provide advantageous sites for uniform Zn deposition. High Young's modulus of the HOF layer further contributes to a high interfacial flexibility and stability against Zn plating‐associated stress. The MA‐BTA@Zn symmetric cells thereby obtain a substantially extended battery life over 1000 h at 4 mA cm−2. The MA‐BTA@Zn||Cu half‐cell demonstrates a highly reversible Zn stripping/plating process over 1500 cycles with impressive average Coulombic efficiency (CE) of 99.5 % at 10 mA cm−2. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous zinc (Zn) ion batteries (AZIBs) using low-cost and safe Zn metal anodes are considered promising candidates for future grid-scale energy storage systems, but the Zn dendrite problem severely hinders the further prospects of AZIBs. Regulating Zn depositing behaviors toward horizontal alignment is highly effective and thus has received huge attention. However, such a strategy is usually based on previous substrate engineering, which requires complex preparation or expensive equipment. Therefore, it is essential to develop a novel solution that can realize horizontally aligned Zn flake deposition via easy operation and low cost. Herein, we report an ultrathin and robust Kevlar membrane as the interlayer to mechanically suppress Zn dendrite growth. Compared to the randomly distributed flaky dendrites in the control group, the deposited Zn sheets would grow into parallel alignment with the existence of such interlayer. As the dendrites are effectively suppressed, Zn∥Cu asymmetric, Zn∥Zn symmetric, and Zn∥MnO2 full batteries using Kevlar interlayer deliver significantly improved cycling stabilities. Furthermore, the Zn∥MnO2 pouch cell using a Kevlar interlayer delivers stable cycling performance and shows stable operation during multi-angle folding. We believe this work provides a new possibility for regulating Zn deposition from a crystallographic perspective. [ABSTRACT FROM AUTHOR]

Owing to the intrinsically high safety, low cost, natural abundance, and high energy density of Zn metal, aqueous Zn ion batteries (AZIBs) have become a promising candidate for large‐scale energy conversion and storage. However, the practical application of AZIBs is hampered by the severe Zn dendrites growth and the poor low‐temperature performance due to the elevated freezing point of aqueous electrolyte. Herein, the study proposes a new kind of room‐temperature liquid Zn salt, which is called Zn coordinated ionic liquid (i.e., (EMIM)5Zn(OTF)7), for all‐temperature AZIBs. The aqueous electrolyte containing 0.261 mol kg−1 (EMIM)5Zn(OTF)7 in Ethylene Glycol (EG) / H2O (6:4) exhibits ultralow freezing point below −100 °C. The liquid Zn salt and EG molecules not only modulate the solvation structure of Zn2+ ion, reducing the coordinated H2O in the first solvation sheath, but also suppresses the parasitic side reaction. As a proof of concept, Zn || Zn symmetric cells and Zn || PANI full cells with the designed electrolyte achieve improved cycling stability and can operate under wide temperature (from −40 to 60 °C). Even with high Zn utilization ratio of 40%, long cycle life over 70 times with capacity retention of 80% is achieved. [ABSTRACT FROM AUTHOR]

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Aqueous rechargeable zinc‐sulfur (Zn‐S) batteries are a promising, cost‐effective, and high‐capacity energy storage technology. Still, they are challenged by the poor reversibility of S cathodes, sluggish redox kinetics, low S utilization, and unsatisfactory areal capacity. This work develops a facile strategy to achieve an appealing high‐areal‐capacity (above 5 mAh cm−2) Zn‐S battery by molecular‐level regulation between S and high‐electrical‐conductivity tellurium (Te). The incorporation of Te as a dopant allows for manipulation of the Zn‐S electrochemistry, resulting in accelerated redox conversion, and enhanced S utilization. Meanwhile, accompanied by the S‐ZnS conversion, Te is converted to zinc telluride during the discharge process, as revealed by ex‐situ characterizations. This additional redox reaction contributes to the S cathode's total excellent discharge capacity. With this unique cathode structure design, the carbon‐confined TeS cathode (denoted as Te1S7/C) delivers a high reversible capacity of 1335.0 mAh g−1 at 0.1 A g−1 with a mass loading of 4.22 mg cm−2, corresponding to a remarkable areal capacity of 5.64 mAh cm−2. Notably, a hybrid electrolyte design uplifts discharge plateau, reduces overpotential, suppresses Zn dendrites growth, and extends the calendar life of Zn‐Te1S7 batteries. This study provides a rational S cathode structure to realize high‐capacity Zn‐S batteries for practical applications. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries (AZIBs) suffer from rampant Zn dendrites growth, corrosion and sluggish transport kinetics, all of which have a serious impact on their performance and practical applications. Therefore, porous carbon nanofibers (BTO@PCNFs) loaded with BaTiO3 nanoparticles (BTO NPs) are constructed as a multifunctional interlayer for stabilizing the Zn anodes. Owing to the synergistic effect of BTO NPs and 3D porous carbon framework, this interlayer can achieve uniform electric field distribution, accelerate Zn2+ migration, and promote ion flux homogenization, thus leading to uniform Zn deposition. Meanwhile, the BTO@PCNFs interlayer demonstrates excellent anti‐corrosion effect, which can effectively prevent the side reactions. Benefiting from the synergistic effect of interlayers, the BTO@PCNFs multifunctional interlayers achieve a comprehensive optimization of the Zn anodes. The BTO@PCNFs‐Zn electrode exhibits lower nucleation overpotential (33.5 mV) at 0.5 mA cm−2. The Zn//Zn symmetrical cell with BTO@PCNFs interlayer exhibits ultra‐low overpotential (14 mV) and ultra‐long cycle life (5250 h at 0.5 mA cm−2). Even at high current density (30 mA cm−2), the BTO@PCNFs‐Zn electrode can be stably cycled for more than 830 h, achieving an ultra‐high cumulative capacity of 12 450 mAh cm−2. The multifunctional interlayers can provide a reference for the design of high‐performance Zn anodes. [ABSTRACT FROM AUTHOR]

The drawbacks of poor electronic conductivity and structural instability during the cycling process limit the electrochemical property of vanadium‐based cathode materials for aqueous zinc‐ion batteries. In addition, continuous growth and accumulation of zinc dendrites can puncture the separator and cause an internal short circuit in the battery. In this work, a unique multidimensional nanocomposite is designed by a facile freeze‐drying method with subsequent calcination, consisting of V2O3 nanosheets and single‐walled carbon nanohorns (SWCNHs) crosslinked together and wrapped by reduced graphene oxide (rGO). The multidimensional structure can largely enhance the structural stability and electronic conductivity of the electrode material. Besides, additive Na2SO4 in the ZnSO4 aqueous electrolyte not only prevents the dissolution of cathode materials but also suppresses the Zn dendrite growth. After considering the influence of additive concentration on ionic conductivity and electrostatic force for electrolyte, V2O3@SWCNHs@rGO electrode delivers a high initial discharge capacity of 422 mAh g−1 at 0.2 A g−1 and a high discharge capacity of 283 mAh g−1 after 1000 cycles at 5 A g−1 in 2 m ZnSO4 + 2 m Na2SO4 electrolyte. Experimental techniques reveal that the electrochemical reaction mechanism can be expressed as the reversible phase transformation between V2O5 and V2O3 with Zn3(VO4)2. [ABSTRACT FROM AUTHOR]

Severe dendrite growth on Zn anodes poses a significant challenge to the development of Zn‐based batteries. An effective strategy for inhibiting the formation of Zn dendrites involves electrode modification. In this study, hollow nitrogen‐doped carbon spheres (HNCS) are synthesized and used as electrodes to regulate Zn deposition in Zn‐based flow batteries. The electrochemical performance of HNCS reveals that the pyrrole nitrogen of HNCS changes the electrode surface state. Therefore, HNCS can inhibit the hydrogen evolution reaction and achieve uniform Zn deposition. HNCS can effectively inhibit dendrite growth and improve the reversibility of the Zn plating/stripping process to regulate the reversibility of Zn‐based batteries. The zinc‐bromine redox flow battery assembled with HNCS significantly reduces the hydrogen evolution reaction and exhibits a coulombic efficiency of 90 % and energy efficiency of 73 % at a current density of 60 mA cm−2. Similarly, an alkaline zinc‐iron flow battery can maintain high Coulombic efficiency and energy efficiency of 83 %. [ABSTRACT FROM AUTHOR]

The practical realization of aqueous zinc-ion batteries relies crucially on effective interphases governing Zn electrodeposition chemistry. In this study, an innovative solution by introducing an ultrathin (≈2 μm) biomass membrane as an intimate artificial interface, functioning as nature's ion-regulation skin to protect zinc metal anodes is proposed. Capitalizing on the inherent properties of natural reed membrane, including multiscale ion transport tunnels, abundant -OH groups, and remarkable mechanical integrity, the reed membrane demonstrates efficacy in regulating uniform and rapid Zn2+ transport, promoting desolvation, and governing Zn (002) plane electrodeposition. Importantly, a unique in situ electrochemical Zn-O bond formation mechanism between the reed membrane and Zn electrode upon cycling is elucidated, resulting in a robustly adhered interface covering on the zinc anode surface, ultimately ensuring remarkable dendrite-free and highly reversible Zn anodes. Consequently, the approach achieves a prolonged cycle life for over 1450 h at 3 mA cm-2/1.5 mAh cm-2 in symmetric Zn//Zn cells. Moreover, exceptional cyclic performance (88.95%, 4000 cycles) is obtained in active carbon-based cells with an active mass loading of 5.8 mg cm-2. The approach offers a cost-effective and environmentally friendly strategy for achieving stable and reversible zinc anodes for aqueous batteries. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries (AZIBs) suffer from rampant Zn dendrites growth, corrosion and sluggish transport kinetics, all of which have a serious impact on their performance and practical applications. Therefore, porous carbon nanofibers (BTO@PCNFs) loaded with BaTiO3 nanoparticles (BTO NPs) are constructed as a multifunctional interlayer for stabilizing the Zn anodes. Owing to the synergistic effect of BTO NPs and 3D porous carbon framework, this interlayer can achieve uniform electric field distribution, accelerate Zn2+ migration, and promote ion flux homogenization, thus leading to uniform Zn deposition. Meanwhile, the BTO@PCNFs interlayer demonstrates excellent anti‐corrosion effect, which can effectively prevent the side reactions. Benefiting from the synergistic effect of interlayers, the BTO@PCNFs multifunctional interlayers achieve a comprehensive optimization of the Zn anodes. The BTO@PCNFs‐Zn electrode exhibits lower nucleation overpotential (33.5 mV) at 0.5 mA cm−2. The Zn//Zn symmetrical cell with BTO@PCNFs interlayer exhibits ultra‐low overpotential (14 mV) and ultra‐long cycle life (5250 h at 0.5 mA cm−2). Even at high current density (30 mA cm−2), the BTO@PCNFs‐Zn electrode can be stably cycled for more than 830 h, achieving an ultra‐high cumulative capacity of 12 450 mAh cm−2. The multifunctional interlayers can provide a reference for the design of high‐performance Zn anodes.

Highlights Digital holography can realize the in situ observation of electrode/electrolyte interface and provide dynamic evolution information of the liquid phase of electrode, which is both efficient and effective in investing the interficial electrochemical mechanism and screening electrolyte additives. Thioacetamide electrolyte additive effectively enhances the electrochemical performance of Zn anode by regulating the interficial ion flux to induce dendrite-free Zn deposition and constructing adsorption molecule layers to inhibit side reactions.

The practical implementation of aqueous zinc‐iodine batteries (ZIBs) is hindered by the rampant Zn dendrites growth, parasite corrosion, and polyiodide shuttling. In this work, ionic liquid EMIM[OAc] is employed as an all‐round solution to mitigate challenges on both the Zn anode and the iodine cathode side. First, the EMIM+ embedded lean‐water inner Helmholtz plane (IHP) and inert solvation sheath modulated by OAc− effectively repels H2O molecules away from the Zn anode surface. The preferential adsorption of EMIM+ on Zn metal facilitates uniform Zn nucleation via a steric hindrance effect. Second, EMIM+ can reduce the polyiodide shuttling by hindering the iodine dissolution and forming an EMIM+‐I3− dominated phase. These effects holistically enhance the cycle life, which is manifested by both Zn || Zn symmetric cells and Zn‐I2 full cells. ZIBs with EAc deliver a capacity decay rate of merely 0.01 ‰ per cycle after over 18,000 cycles at 4 A g−1, and lower self‐discharge and better calendar life than the ZIBs without ionic liquid EAc additive. [ABSTRACT FROM AUTHOR]

With the increasing demand for low‐cost and high‐safety portable batteries, aqueous zinc‐ion batteries (ZIBs) have been regarded as a potential alternative to the lithium‐ion batteries, bringing about extensive research dedicated in the exploration of high‐performance and highly reversible ZIBs. Although separators are generally considered as non‐active components in conventional research on ZIBs, advanced separators designs seem to offer effective solutions to the majority of issues within ZIBs system. These issues encompass concerns related to the zinc anode, cathode, and electrolyte. Initially, we delve into the origins and implications of various inherent problems within the ZIBs system. Subsequently, we present the latest research advancements in addressing these challenges through separators engineering. This includes a comprehensive, detailed exploration of various strategies, coupled with instances of advanced characterizations to provide a more profound insight into the mechanisms that influence the separators. Finally, we undertake a multi‐criteria evaluation, based on application standards for diverse substrate separators, while proposing guiding principles for the optimal design of separators in zinc batteries. This review aims to furnish valuable guidance for the future development of advanced separators, thereby nurturing progress in the field of ZIBs. [ABSTRACT FROM AUTHOR]

Highlights: Digital holography can realize the in situ observation of electrode/electrolyte interface and provide dynamic evolution information of the liquid phase of electrode, which is both efficient and effective in investing the interficial electrochemical mechanism and screening electrolyte additives. Thioacetamide electrolyte additive effectively enhances the electrochemical performance of Zn anode by regulating the interficial ion flux to induce dendrite-free Zn deposition and constructing adsorption molecule layers to inhibit side reactions.Zinc ion batteries are considered as potential energy storage devices due to their advantages of low-cost, high-safety, and high theoretical capacity. However, dendrite growth and chemical corrosion occurring on Zn anode limit their commercialization. These problems can be tackled through the optimization of the electrolyte. However, the screening of electrolyte additives using normal electrochemical methods is time-consuming and labor-intensive. Herein, a fast and simple method based on the digital holography is developed. It can realize the in situ monitoring of electrode/electrolyte interface and provide direct information concerning ion concentration evolution of the diffusion layer. It is effective and time-saving in estimating the homogeneity of the deposition layer and predicting the tendency of dendrite growth, thus able to value the applicability of electrolyte additives. The feasibility of this method is further validated by the forecast and evaluation of thioacetamide additive. Based on systematic characterization, it is proved that the introduction of thioacetamide can not only regulate the interficial ion flux to induce dendrite-free Zn deposition, but also construct adsorption molecule layers to inhibit side reactions of Zn anode. Being easy to operate, capable of in situ observation, and able to endure harsh conditions, digital holography method will be a promising approach for the interfacial investigation of other battery systems. [ABSTRACT FROM AUTHOR]

The implementation of aqueous zinc ion batteries (AZBs) is hindered by the notorious Zn dendrite growth and side reactions on Zn anodes. Herein, a novel strategy is introduced to overcome these hurdles by designing a self‐adapting soft polymeric composite interface (SAP). Unlike conventional methods relying on passive coating process, the approach leverages dynamic in situ electrochemical bonding via Zn─O interactions formed during cycling, ensuring intimate contact between the SAP interface and Zn electrode. The SAP interface boasts a robust network of hydrogen bonding and electrostatic interactions, which not only promotes the desolvation of Zn2+ and the repulsion of SO42−, facilitating uniform and rapid Zn2+ migration while effectively suppressing parasitic reactions; but also exhibits remarkable self‐adapting and self‐healing capabilities, enabling the interface to accommodate volume changes and repair mechanical failures over prolonged cycling. Consequently, highly reversible Zn electrodes are achieved with SAP, showcasing 3300 h at 1 mA cm−2/0.5 mAh cm−2 and 350 h at 20 mA cm−2/10 mAh cm−2 in the symmetric cells. The advantages of the SAP interface are further verified when paired with high mass loading LiMn2O4 cathodes in AZBs. The versatile SAP interface offers insights into advanced interface design for efficient and durable AZBs. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries (ZIBs) have been regarded as a promising candidate for the next‐generation energy‐storage devices due to their intrinsic safety, low cost, resource abundance, and environmental friendliness. Nevertheless, the commercial applications of ZIBs have been largely plagued by the instability of the Zn anodes. Interfacial engineering arises as a straightforward and effective method to address the instability issues for the development of high‐performance ZIBs. In this review, a comprehensive overview of recent progress and perspective in interfacial engineering techniques to stabilize Zn anodes in ZIBs is presented. With emphasis on the critical issues regarding the instability problems, including Zn dendrites, hydrogen evolution reaction (HER), corrosion and passivation, the major effects and the underlying mechanisms are analyzed, and the corresponding interfacial engineering strategies as well as analytical technologies are summarized. The existing challenges and opportunities in interfacial engineering are also prospected for the future development of high‐performance ZIBs. [ABSTRACT FROM AUTHOR]

Because of their high safety, low cost, and high volumetric specific capacity, zinc-ion batteries (ZIBs) are considered promising next-generation energy storage devices, especially given their high potential for large-scale energy storage. Despite these advantages, many problems remain for ZIBs—such as Zn dendrite growth, hydrogen evolution, and Zn anode corrosion—which significantly reduce the coulomb efficiency and reversibility of the battery and limit its cycle lifespan, resulting in much uncertainty in terms of its practical applications. Numerous electrolyte additives have been proposed in recent years to solve the aforementioned problems. This review focuses on electrolyte additives and discusses the different substances employed as additives to overcome the problems by altering the Zn ^2+ solvation structure, creating a protective layer at the anode–electrolyte interface, and modulating the Zn ^2+ distribution to be even and Zn deposition to be uniform. On the basis of the review, the possible research strategies, future directions of electrolyte additive development, and the existing problems to be solved are also described.

[Display omitted] • Cycling performance of Zn electrodes is enhanced via adding lactose. • Regulating Zn electrode/electrolyte interface by lactose contributes to uniform Zn deposition, as well as higher CE. • The zinc ion electrodeposition process is effectively regulated by lactose's dynamic regulatory interface. The practical utilization of rechargeable aqueous zinc metal batteries (AZMBs) has been constrained by the formation of zinc dendrites and other associated issues. This article introduces lactose, a compound rich in hydroxyl groups, as an electrolyte additive into the aqueous solution of the electrolyte with the objective of suppressing the harmful growth of zinc dendrites. The lactose additive, with its strong zincophilicity, robust intermolecular hydrogen bonding, and a large number of exposed high electronegativity hydroxyl groups, enables lactose to effectively modulate the electrode/electrolyte interface in a dynamic manner, thereby achieving the stability and reversibility of the zinc anode. The findings presented in this work demonstrate the uniform deposition and stripping of zinc in a 2 M ZnSO 4 electrolyte with the addition of lactose, thereby enhancing the cycling performance of Zn||Zn batteries. The alteration of the zinc ion environment on the surface of the zinc electrode, in conjunction with the dynamic modulation of the Gouy-Chapman-Stern (GCS) layer by lactose, increases the nucleation overpotential, thereby facilitating to a uniform deposition morphology in lieu of the formation of large-scale dendrites. Furthermore, the formation of hydrogen bonds serves to prevent the occurrence of side reactions. These factors act in concert to enhance the electrochemical performance of AZMBs. The addition of lactose to the electrolyte has resulted in a significant enhancement in the Coulombic efficiency of the card-type Zn||Cu asymmetric battery, reaching 99.7 %. The biodegradability of lactose and the sustainability of its source make this research conducive to the development of environmentally friendly battery electrolyte additives. [ABSTRACT FROM AUTHOR]

This work reports a novel 3D printed grid reservoir-integrated mesoporous carbon coordinated silicon oxycarbide hybrid composite (3DP-MPC-SiOC) to establish the zincophile interphase for controlling the dendrite formation. The customized 3D printed grid patterned structure inhibits Zn dendrite growth and achieves long-term stability with reduced voltage polarization due to homogeneous electric field distribution. The hybrid composite consisting of SiOC interpenetrated within carbon constructs a high zinc nucleation interphase, hence promoting uniform Zn 2+ deposition and enhancing ionic diffusion with dendrite-free growth and a reduced nucleation energy barrier. As a result, the 3DP-MPC-SiOC@Zn symmetrical cell affords a highly reversible Zn plating/stripping and dendrite-free structure over 198 h with an ultra-low voltage polarization. These inspiring performances endow the 3DP anode with a 3DP-VO cathode as a full battery, which shows a retention capacity of 78.8 mAh g -1 (Coulombic efficiency: 94.04%) at 0.1 A g -1 and a large energy density of 41 Wh kg -1 at a power density of 1.2 W kg -1 (based on the total mass of electrode) after 120 cycles. This newly developed 3D printing of hybrid composite as an electrode is straightforward and scalable and provides a novel concept for realizing dendrite-free and stable rechargeable Zn-ion batteries., (© 2024 Wiley‐VCH GmbH.)

• Aqueous rechargeable batteries with low-cost hybrid electrolytes can effectively improve the output voltage and alleviate the zinc dendrites. • The full cells assembled with potassium zinc hexacyanoferrate (KZnHCF) cathodes and zinc foil anodes reach an output voltage of 1.92 V and an energy density of 107.6 Wh kg−1. • The hybrid electrolyte contributes to the uniform deposition/stripping and suppress the zinc dendrites. The energy density of aqueous reachable batteries (ARBs) is limited by the output voltage in the aqueous electrolyte. Herein, low-cost aqueous hybrid electrolytes composed of ZnSO 4 and K 2 SO 4 dual salts effectively improve the output voltage and suppress the zinc dendrites. The aqueous full cells assembled with potassium zinc hexacyanoferrate (KZnHCF) cathodes and zinc foil anodes reach an output voltage of 1.92 V and an energy density of 107.6 Wh kg−1. It is demonstrated the reversible insertion/extraction of K+ at the cathodes and uniform zinc deposition/striping at the anode in hybrid electrolyte via a series in-situ and ex-situ investigation. The dual salt electrolyte can not only satisfy the reversible capacitive dominated process at the cathodes but also suppress the zinc dendrite. Density functional theory (DFT) calculation demonstrates the K+ preferential intercalation mechanism of KZnHCF in hybrid electrolyte and the inhibition effect of K+ insertion on Zn2+ insertion. This strategy presents a promising approach for development of high performance and low-cost aqueous electrolyte. [ABSTRACT FROM AUTHOR]

Aqueous zinc-ion batteries (AZIBs) have emerged as one of the most promising energy storage technologies due to their high safety and cost-effectiveness. However, several challenges associated with the Zn metal anode, such as dendrite growth, corrosion, and hydrogen evolution reaction (HER), have hindered further applications of AZIBs. Herein, maltose (MT) is used as a functional electrolyte additive to protect the Zn metal electrode during the interface deposition process. The additive can effectively affect the interface of Zn metal, suppressing HER and corrosion reactions. Moreover, it facilitates the uniform deposition of Zn by inducing Zn 2+ to form a stable (100) crystal plane. As a result, the symmetric cell exhibited stable cycling performance for 2000 h at a current density of 2 mA cm -2 , and the Zn||NH 4 V 4 O 10 full cell maintained steady cycling for 1000 cycles at 2 A g -1 . This study provides an approach to achieve uniform Zn deposition through additives.

Aqueous zinc-ion batteries (AZIBs) have emerged as one of the most promising candidates for next-generation energy storage devices due to their outstanding safety, cost-effectiveness, and environmental friendliness. However, the practical application of zinc metal anodes (ZMAs) faces significant challenges, such as dendrite growth, hydrogen evolution reaction, corrosion, and passivation. Fortunately, the rapid rise of nanomaterials has inspired solutions for addressing these issues associated with ZMAs. Nanomaterials with unique structural features and multifunctionality can be employed to modify ZMAs, effectively enhancing their interfacial stability and cycling reversibility. Herein, an overview of the failure mechanisms of ZMAs is presented, and the latest research progress of nanomaterials in protecting ZMAs is comprehensively summarized, including electrode structures, interfacial layers, electrolytes, and separators. Finally, a brief summary and optimistic perspective are given on the development of nanomaterials for ZMAs. This review provides a valuable reference for the rational design of efficient ZMAs and the promotion of large-scale application of AZIBs.

The highly reversible plating/stripping of Zn is plagued by dendrite growth and side reactions on metallic Zn anodes, retarding the commercial application of aqueous Zn-ion batteries. Herein, a distinctive nano dual-phase diamond (NDPD) comprised of an amorphous-crystalline heterostructure is developed to regulate Zn deposition and mechanically block dendrite growth. The rich amorphous-crystalline heterointerfaces in the NDPD endow modified Zn anodes with enhanced Zn affinity and result in homogeneous nucleation. In addition, the unparalleled hardness of the NDPD effectively overcomes the high growth stress of dendrites and mechanically impedes their proliferation. Moreover, the hydrophobic surfaces of the NDPD facilitate the desolvation of hydrate Zn 2+ and prevent water-mediated side reactions. Consequently, the Zn@NDPD presents an ultrastable lifespan exceeding 3200 h at 5 mA cm -2 and 1 mAh cm -2 . The practical application potential of Zn@NDPD is further demonstrated in full cells. This work exhibits the great significance of a chemical-mechanical synergistic anode modification strategy in constructing high-performance aqueous Zn-ion batteries.

Zinc metal suffers from violent and long-lasting water-induced side reactions and uncontrollable dendritic Zn growth, which seriously reduce the coulombic efficiency (CE) and lifespan of aqueous zinc-metal batteries (AZMBs). To suppress the corresponding harmful effects of the highly active water, a stable zirconium-based metal-organic framework with water catchers decorated inside its sub-nano channels is used to protect Zn-metal. Water catchers within narrow channels can constantly trap water molecules from the solvated Zn-ions and facilitate step-by-step desolvation/dehydration, thereby promoting the formation of an aggregative electrolyte configuration, which consequently eliminates water-induced corrosion and side reactions. More importantly, the functionalized sub-nano channels also act as ion rectifiers and promote fast but even Zn-ions transport, thereby leading to a dendrite-free Zn metal. As a result, the protected Zn metal demonstrates an unprecedented cycling stability of more than 10 000 h and an ultra-high average CE of 99.92% during 4000 cycles. More inspiringly, a practical NH 4 V 4 O 10 //Zn pouch-cell is fabricated and delivers a capacity of 98 mAh (under high cathode mass loading of 25.7 mg cm -2 ) and preserves 86.2% capacity retention after 150 cycles. This new strategy in promoting highly reversible Zn metal anodes would spur the practical utilization of AZMBs., (© 2024 Wiley‐VCH GmbH.)

The drawbacks of poor electronic conductivity and structural instability during the cycling process limit the electrochemical property of vanadium-based cathode materials for aqueous zinc-ion batteries. In addition, continuous growth and accumulation of zinc dendrites can puncture the separator and cause an internal short circuit in the battery. In this work, a unique multidimensional nanocomposite is designed by a facile freeze-drying method with subsequent calcination, consisting of V 2 O 3 nanosheets and single-walled carbon nanohorns (SWCNHs) crosslinked together and wrapped by reduced graphene oxide (rGO). The multidimensional structure can largely enhance the structural stability and electronic conductivity of the electrode material. Besides, additive Na 2 SO 4 in the ZnSO 4 aqueous electrolyte not only prevents the dissolution of cathode materials but also suppresses the Zn dendrite growth. After considering the influence of additive concentration on ionic conductivity and electrostatic force for electrolyte, V 2 O 3 @SWCNHs@rGO electrode delivers a high initial discharge capacity of 422 mAh g -1 at 0.2 A g -1 and a high discharge capacity of 283 mAh g -1 after 1000 cycles at 5 A g -1 in 2 m ZnSO 4 + 2 m Na 2 SO 4 electrolyte. Experimental techniques reveal that the electrochemical reaction mechanism can be expressed as the reversible phase transformation between V 2 O 5 and V 2 O 3 with Zn 3 (VO 4 ) 2 ., (© 2023 Wiley‐VCH GmbH.)

Zinc-ion batteries, known for safety and efficiency, are a hotspot in electrochemical energy storage field. Nonetheless, the emergence of dendrites on zinc anodes during electrochemical cycles can lead to capacity attenuation and even failure, particularly under low temperatures. In this study, we develop a novel dendrite-free and low-temperature resistant Zn(ClO 4) 2 /Li 2 SO 4 /Dimethyl sulfoxide (DMSO) hybrid electrolyte by using DMSO as a hydrogen bond acceptor and solvation regulator. Our research demonstrates that, by reducing the desolvation energy barrier of the Zn2+ solvation sheath and the nucleation overpotential of Zn deposition, DMSO effectively inhibits zinc dendrites and side reactions. Furthermore, DMSO disrupts hydrogen bonding between water molecules, preventing electrolyte freezing at low temperatures. As a result, at 0.5 mA cm−2, the Zn||Zn symmetric device using this hybrid electrolyte exhibits consistent operation for over 4000 h even at -25 °C, featuring a minimal deposition/dissolution overpotential of approximately 0.045 mV. Additionally, at -20 °C, the Zn||Zn(ClO 4) 2 -Li 2 SO 4 -DMSO||LiFePO 4 battery demonstrates stable cycling for over 600 cycles at 0.6 C (1 C = 170 mA g − 1), delivering a capacity of 103 mA h g−1. [ABSTRACT FROM AUTHOR]

The inherent safety and high energy density of aqueous Zn-ion batteries (AZIBs), coupled with the abundant reserves of Zn, make them an ideal candidate for the following generation of energy storage devices. Nevertheless, the growth of dendrites and water decomposition seriously hinder the commercialization of AZIBs. This work proposes depositing a thin polydimethylsiloxane (PDMS) layer on the Zn surface through a simple vapor method (PDMS@Zn) to address the above challenges. Significantly, the presence of this PDMS layer degrades the resistance of nucleation, optimizes the crystal orientation of Zn2+ deposition, isolates and protects Zn anode, and restricts the flow of Zn2+, improving the kinetics of Zn2+ deposition and homogenizes Zn2+ stripping/plating. The assembled PDMS@Zn symmetrical batteries exhibit 25 mV low voltage hysteresis for 1500 h cycles at 1 mA cm−2, 0.5 mA h cm−2, and the full-cell with an ultra-long cycle life of 2500 cycles. • The PDMS layer is prepared on Zn metal using a one-step vapor deposition method. • The PDMS layer presents an excellent desolvation effect. • The hydrophobic PDMS layer isolates the Zn anode and inhibits water decomposition. • The gap structure of the layer limits Zn2+ flux and facilitates Zn2+ a uniform deposition. [ABSTRACT FROM AUTHOR]

Zinc-iodine batteries have the potential to offer high energy-density aqueous energy storage, but their lifetime is limited by the rampant dendrite growth and the concurrent parasite side reactions on the Zn anode, as well as the shuttling of polyiodides. Herein, a cation-conduction dominated hydrogel electrolyte is designed to holistically enhance the stability of both zinc anode and iodine cathode. In this hydrogel electrolyte, anions are covalently anchored on hydrogel chains, and the major mobile ions in the electrolyte are restricted to be Zn 2+ . Specifically, such a cation-conductive electrolyte results in a high zinc ion transference number (0.81) within the hydrogel and guides epitaxial Zn nucleation. Furthermore, the optimized Zn 2+ solvation structure and the reconstructed hydrogen bond networks on hydrogel chains contribute to the reduced desolvation barrier and suppressed corrosion side reactions. On the iodine cathode side, the electrostatic repulsion between negative sulfonate groups and polyiodides hinders the loss of the iodine active material. This all-round electrolyte design renders zinc-iodine batteries with high reversibility, low self-discharge, and long lifespan., (© 2024 Wiley‐VCH GmbH.)

Metallic Zn is considered as a promising anode material because of its abundance, eco-friendliness, and high theoretical capacity. However, the uncontrolled dendrite growth and side reactions restrict its further practical application. Herein, we proposed a β-cyclodextrin-modified multiwalled carbon nanotube (CD-MWCNT) layer for Zn metal anodes. The obtained CD-MWCNT layer with high affinity to Zn can significantly reduce the transfer barrier of Zn 2+ at the electrode/electrolyte interface, facilitating the uniform deposition of Zn 2+ and suppressing water-caused side reactions. Consequently, the Zn||Zn symmetric cell assembled with CD-MWCNT shows a significantly enhanced cycling durability, maintaining a cycling life exceeding 1000 h even under a high current density of 5 mA cm -2 . Furthermore, the full battery equipped with a V 2 O 5 cathode displays an unparalleled long life. This work unveils a promising avenue toward the achievement of high-performance Zn metal anodes.

Atomic-scale inorganic carbon nanomaterials (ICN) with rich surface polarity and low lattice mismatch for zinc is proposed as a green and effective electrolyte additive to regulate the Zn deposition behavior, rending dendrite-free and side reactions-free Zn metal anodes. [Display omitted] • A multifunctional electrolyte additive of ICN is developed for Zn-ion batteries. • The high surface polarity of ICN mitigates the water-induced side reactions. • The low lattice mismatch with Zn(0 0 2) nanosheets guides parallel Zn deposition. • The full battery harvests excellent cycling performance under practical conditions. The renaissance of aqueous zinc-ion batteries (ZIBs) is impeded by the disordered Zn deposition and notorious water attack at the Zn-electrolyte interface. Electrolyte additive engineering plays a vital role in tuning the electrode–electrolyte interface chemistry to stabilize Zn anode but its long-term performance at high plating/stripping rates and capacities remains a challenge. Herein, we demonstrate highly reversible Zn anodes by employing the atomic-scale inorganic carbon nanomaterials (ICN) as a multifunctional electrolyte additive into the common ZnSO 4 solution to regulate the Zn deposition behaviors. The ICN with rich surface polar groups modulates the primary Zn2+ solvation structure to avoid the side reactions, and preferentially absorbs on the Zn anode surface to build a passivated-protect interface to suppress Zn corrosion and dendrite growth. More importantly, its low lattice mismatch with zinc navigates the preferred Zn (0 0 2) deposition to induce smooth and dense Zn plating morphology, fundamentally eradicating the Zn dendrite issues and further Zn corrosion. Consequently, the electrolyte containing ICN additive endows the symmetric Zn cells with fabulous cumulative capacity (3500 mAh cm−2), decent Coulombic efficiency (99.69 %) at 10 mA cm−2, and excellent stability of 800 cycles with only 0.022 % capacity decay per cycle in the Zn||VO X battery under practical conditions of limited Zn supply, high-loading cathode and lean electrolyte. This work presents an effective strategy to advance the practical applications of rechargeable aqueous zinc batteries. [ABSTRACT FROM AUTHOR]

Rampant dendrite growth, electrode passivation and severe corrosion originate from the uncontrolled ions migration behavior of Zn 2+ , SO 4 2- , and H + , which are largely compromising the aqueous zinc ion batteries (AZIBs) performance. Exploring the ultimate strategy to eliminate all the Zn anode issues is challenging but urgent at present. Herein, a fluorinated separator interface (PVDF@GF) is constructed simply by grafting the polyvinylidene difluoride (PVDF) on the GF surface to realize high-performance AZIBs. Experimental and theoretical studies reveal that the strong interaction between C─F bonds in the PVDF and Zn 2+ ions enables evenly redistributed Zn 2+ ions concentration at the electrode interface and accelerates the Zn transportation kinetics, leading to homogeneous and fast Zn deposition. Furthermore, the electronegative separator interface can spontaneously repel the SO 4 2- and anchor H + ions to alleviate the passivation and corrosion. Accordingly, the Zn|Zn symmetric cell with PVDF@GF harvests a superior cycling stability of 500 h at 10 mAh cm -2 , and the Zn|VOX full cell delivers 76.8% capacity retention after 1000 cycles at 2 A g -1 . This work offers an all-round solution and provides new insights for the design of advanced separators with ionic sieve function toward stable and reversible Zn metal anode chemistry., (© 2023 Wiley-VCH GmbH.)