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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]

Tetrahydrofurfuryl alcohol (THFA), a cost-effective electrolyte additive, is employed innovatively to optimize both the cathode and anode, thereby enhancing the performance of zinc-based batteries significantly. [Display omitted] Aqueous zinc-ion batteries (AZIBs) are highly regarded for their affordability, stability, safety, and eco-friendliness. Nevertheless, their practical application is hindered by severe side reactions and the formation of zinc (Zn) dendrites on the Zn metal anode surface. In this study, we employ tetrahydrofuran alcohol (THFA), an efficient and cost-effective alcohol ether electrolyte, to mitigate these issues and achieve ultralong-life AZIBs. Theoretical calculations and experimental findings demonstrate that THFA acts as both a hydrogen bonding donor and acceptor, effectively anchoring H 2 O molecules through dual-site hydrogen bonding. This mechanism restricts the activity of free water molecules. Moreover, the two oxygen (O) atoms in THFA serve as dual solvation sites, enhancing the desolvation kinetics of [Zn(H 2 O) 6 ]2+ and improving the deposition dynamics of Zn2+ ions. As a result, even trace amounts of THFA significantly suppress adverse reactions and the formation of Zn dendrites, enabling highly reversible Zn metal anodes for ultralong-life AZIBs. Specifically, a Zn-based symmetric cell containing 2 % THFA achieves an ultralong cycle life of 8,800 h at 0.5 mA cm−2/0.5 mAh cm−2, while a Zn//VO 2 full cell containing 2 % THFA maintains a remarkable 80.03 % capacity retention rate at 5 A g−1 over 2,000 cycles. This study presents a practical strategy to develop dendrite-free, cost-effective, and highly efficient aqueous energy storage systems by leveraging alcohol ether compounds with dual-site hydrogen bonding capabilities. [ABSTRACT FROM AUTHOR]

The low-cost small molecule nicotinamide serves as an electrolyte additive for aqueous zinc-ion batteries. Only 1 wt% of nicotinamide enables Zn||Zn symmetric cells to have an ultra-long lifespan of over 9700h at 1 mA cm−2, expanding nearly 808 times compared to that without nicotinamide. This work is remarkable among state-of-the-art novel aqueous zinc-ion batteries. [Display omitted] Aqueous zinc-ion batteries (AZIBs) have recently been paid great attention due to their robust safety features, high theoretical capacity, and eco-friendliness, yet their practical application is hindered by the serious dendrite formation and side reactions of Zn metal anode during cycling. Herein, a low-cost small molecule, nicotinamide (NIC), is proposed as an electrolyte additive to effectively regulate the Zn interface, achieving a highly reversible and stable zinc anode without dendrites. NIC molecules not only modify the Zn2+ solvation structure but also preferentially adsorb on the Zn surface than solvated H 2 O to protect the Zn anode and provide numerous nucleation sites for Zn2+ to homogenize Zn deposition. Consequently, the addition of 1 wt% NIC enables Zn||Zn symmetric cells an ultra-long lifespan of over 9700 h at 1 mA cm−2, which expands nearly 808 times compared to that without NIC. The advantages of NIC additives are further demonstrated in NaVO||Zn full cells, which exhibit exceptional capacity retention of 90.3 % after 1000 cycles with a high Coulombic efficiency of 99.9 % at 1 A/g, while the cell operates for only 42 cycles without NIC additive. This strategy presents a promising approach to solving the anode problem, fostering advancements in practical AZIBs. [ABSTRACT FROM AUTHOR]

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 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]

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]

Aqueous Zn ion batteries are appealing systems owing to their safety, low cost, and environmental friendliness; however, their practical applicability is impeded by the growth of Zn dendrites and side reactions. Herein, a dual‐functional electrolyte additive, namely acetylacetone (AT) is utilized for the simultaneous regulation of the solventized structure and anode–electrolyte interface (AEI) to achieve a durable, dendrite‐free Zn anode. Theoretical calculations and experimental characterizations reveal that the AT molecule can be adsorbed onto Zn metal surface to reconstruct the AEI and allow for the primordial desolvation of [Zn(H2O)6]2+ at locations away from the surface of the Zn anode during deposition, which is attributed to the strong polarity of the carbonyl functional group. In addition, the two carbonyls of AT can replace two H2O molecules in the primary solventized structure of Zn2+ to reduce the number of active H2O molecules, efficiently suppressing Zn dendrite growth and detrimental reactions. As a proof of concept, a Zn//Cu cell is constructed in ZnSO4 containing 3 vol.% AT electrolyte, delivering stable cycling over 1800 cycles while maintaining a high Coulombic efficiency of 99.74%. This study provides a practical approach for inhibiting dendrite growth and side reactions by harnessing carbonyl chemistry. [ABSTRACT FROM AUTHOR]

Uncontrolled growth of Zn dendrites is the main reason for the short‐circuit failure of aqueous Zn‐ion batteries. Using electrolyte additives to manipulate the crystal growth is one of the most convenient strategies to mitigate the dendrite issue. However, most additives would be unstable during cycling due to the structural reconstruction of the deposition layer. Herein, it is proposed to use 1‐butyl‐3‐methylimidazolium cation (BMIm+ ion) as an electrolyte additive, which could steadily induce the preferential growth of (002) plane and inhibit the formation of Zn dendrites. Specifically, BMIm+ ion will be preferentially adsorbed on (100) and (101) planes of Zn anodes, forcing Zn2+ ion to deposit on the (002) plane, thus inducing the preferential growth of the (002) plane and forming a flat and compact deposition layer. As a result, the Zn anode cycles for 1000 h at10 mA cm−2 and 10 mAh cm−2 as well as a high Coulombic efficiency of 99.8%. Meanwhile, the NH4V4O10||Zn pouch cell can operate stably for 240 cycles at 0.4 A g−1. The BMIm+ ion additive keeps a stable effect on the structural reconstruction of the Zn anode during the prolonged cycling. [ABSTRACT FROM AUTHOR]

The uncontrollable dendrite growth, hydrogen evolution, and other side‐reactions, originating from the zinc anode, have severely restricted the practical application of aqueous zinc–ion batteries (ZIBs). To address these challenges, a stable solid‐electrolyte‐interface (SEI) layer is constructed through introducing sericin molecules as an electrolyte additive to modulate the Zn nucleation and overpotential of hydrogen evolution. This SEI layer increases the nucleation overpotential during Zn plating, leading to the finer‐grained, dense, and uniform Zn deposition. Meanwhile, the lower unoccupied molecular orbital molecules in SEI layer have a higher reduction potential than H2O, inhibiting hydrogen production, and subsequently suppressing the Zn dendritic and interfacial side‐reactions. Consequently, the Zn|Zn symmetric cells with sericin additives exhibit an extremely prolonged cycling lifetime of 4446 h compared with to bare Zn electrode of 53 h at 1.0 mA cm−2/1.0 mAh cm−2, and a high average Coulombic efficiency of 99.29% under a high cumulative plated capacity of 1.0 Ah cm−2 tested in Zn|Cu cells. Moreover, the assembled full cells using Na2V6O16·3H2O cathodes endure 2000 cycles with high capacity retention of 81.7% at 5.0 A g−1. This study sheds new light on modulating the process of Zn nucleation and overpotential of H2 evolution for durable Zn anode design. [ABSTRACT FROM AUTHOR]

"Tip effect" triggered by uneven zinc deposition accelerates the growth of Zn dendrites. The unfavorable interfacial activity gradient aggravates zinc deposition at the tips, which is the root cause of zinc dendrites. This study reports an interfacial local activation strategy to reconfigure the interfacial activity gradient of zinc anode to promote more stable operation of zinc batteries. A locally activated zinc anode (Zn-ILA) is proposed as the proof-of-concept zinc anode by constructing high-active microchannels to induce preferential zinc deposition, while the remaining low-active region is accompanied by zinc epitaxial growth, thus achieving bottom-up zinc deposition at the anode interface. A fabrication method based on nanosecond pulsed laser is used to modify the zinc anode by creating high-active microchannels through thermal impingement. Additionally, low-active regions covered by dense ZnO nanoparticles are also formed due to the plasma effect. The laser-induced cross-scale oxide layers help improve the corrosion resistance at the full zinc anode interface. The proposed interfacial local activation strategy enables ordered selective deposition at the Zn-ILA interface owing to the activity gradient, as well as stabilizes the long-term operation of symmetric and full cells. The effectiveness of Zn-ILA is also validated in large-area pouch batteries, showing great potential for large-scale energy storage systems. [Display omitted] • An interfacial local activation strategy has been proposed to promote stable zinc anodes. • A gradient active interface has been developed to tailor the patterns of selective zinc deposition. • Corrosion resistance and charge transfer kinetics of the Zn-ILA electrode can be synergistically enhanced. • The optimized Zn-ILA electrode enables outstanding cycling stability in both coin and pouch cells. [ABSTRACT FROM AUTHOR]

• 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]

Metallic zinc (Zn) has been considered to be an ideal anode material for aqueous batteries, but is impeded by the growth of Zn dendrites and its side reactions with an aqueous electrolyte. Here, it is reported that an artificial protective layer filled with novel 2D Zn2+ adsorbed Sb3P2O143− (denoted as Zn‐Sb3P2O14) nanosheets provide an effective route to mitigate the above challenging problems. The Zn‐Sb3P2O14 protection layer not only avoids the direct contact with the aqueous electrolyte to suppress the side reactions but also allows for Zn‐ions to pass through the protection layer rapidly. Moreover, the 2D Sb3P2O143− skeleton with negative charge also confines the 2D diffusion of Zn‐ion along the lateral surface of Zn anode, resulting in a uniform electron‐deposition. This unique protection layer not only enables dendrite‐free Zn plating/stripping with an average Coulombic efficiency of 99.2% for 200 cycles, but also sustains the symmetric Zn||Zn cell over 1300 h at 1 mA cm−2 and 1 mAh cm−2 as well as for 450 h at 10 mA cm−2 and 10 mAh cm−2. Such advantages bring high reversibility to full Zn batteries with MnO2 cathodes, which deliver a discharge capacity of 111.7 mAh g−1 after 1000 cycles. [ABSTRACT FROM AUTHOR]

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]

Aqueous zinc metal batteries (AZMBs) are regarded as competitive candidates for next‐generation energy storage owing to their low cost, high performance, high safety, and high environmental friendliness. However, serious issues, including Zn dendrites, chemical corrosion, H2 evolution, and sluggish Zn2+ diffusion kinetics, have largely impeded the commercial application of AZMBs. To understand these issues in depth and identify countermeasures, comprehensive analyses of AZMBs have continuously been developed. In this review, a detailed overview of the analytical techniques used to study AZMBs, including characterization methods, simulations, and theoretical calculations is presented, which provides a comprehensive toolbox for further research. Conventional characterization methods that provide preliminary information are first summarized. Various in situ techniques, including visualization and spectral characterization, are then discussed. These advanced real‐time monitoring techniques contribute to a deeper understanding of the battery failure mechanism. Simulations and theoretical calculations are then presented in detail, enabling an in‐depth investigation of the mechanism at the atomic level. Theoretical analyses can not only explore the mechanism in more detail, but also play a key role in guiding research and predicting future directions. Finally, the challenges and perspective of comprehensive analyses of AZMBs are discussed. [ABSTRACT FROM AUTHOR]

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]

Aqueous Zn-based batteries (AZBs) have attracted great attention due to their high safety, low cost, and environmental friendliness. However, the Zn anode suffers from problems such as the formation of Zn dendrites. And there are only few active cathode materials which can allow the insertion/extraction of Zn2+ ions. Thereinto, Prussian blue analogs (PBAs) are promising active cathode materials for AZBs, having high operation voltage but poor electrochemical stability. Herein, K 2 Zn 3 [Fe(CN) 6 ] 2 (KZnHCF) particles with cubic morphology are prepared for AZBs, and the electrochemical stability is improved by simply adjusting the composition of the electrolyte solvent in the battery system. Electrochemical tests indicate that the electrolyte with ethanol (EA) as solvent can promote the uniform deposition of zinc, thereby inhibiting the growth of Zn dendrites. Furthermore, ex-situ XRD results prove that the structural damage of KZnHCF during charging-discharge process is greatly alleviated when EA is used as the electrolyte solvent. Nonetheless, using pure EA as electrolyte solvent exposes the batteries to potential safety hazards, and compared with the Zn/KZnHCF batteries with H 2 O as solvent, the specific capacities of the batteries with EA as solvent are lower. Hence, the mixed electrolytes with different volume ratios (H 2 O/EA-1:1, H 2 O/EA-1:2, H 2 O/EA-2:1) are applied. It's obvious that not only the growth of zinc dendrites is suppressed, but also the electrochemical performances of the batteries are further improved. Overall, a dendrite-free and high-performance Zn/KZnHCF battery is obtained by using a mixed electrolyte solvent (H 2 O/EA-1:1), presenting average specific capacities of 50.0, 49.0, 46.3, and 43.2 mAh g−1 at current densities of 50, 100, 150, and 200 mA g−1, and remaining a specific capacity of 29.1 mAh g−1 at a current density of 200 mA g−1 after 500 cycles. • A dendrite-free and high-performance Zn/KZnHCF battery is created. • The inhibition effect of ethanol on the growth of Zn dendrites is clarified. • The effect of different electrolyte solvents is investigated by ex-situ XRD tests. • As-prepared Zn/KZnHCF batteries are superior to the reported aqueous zinc batteries. [ABSTRACT FROM AUTHOR]

The issue of Zn dendrites has been limiting the further application of aqueous Zn ion batteries. In this work, the three-dimensional trench interface on the surface of the Zn foil is constructed by a simple etching method to buffer the formation of the Zn dendrite. Importantly, the relationship between stripping/plating behavior and dendrite formation, especially stripping behavior, is systematically analyzed using Ex-situ scanning electron microscope and finite element method. The low current density interface designed by etching a three-dimensional trench structure plays a key role in controlling the formation of the Zn dendrite. Therefore, the resultant Zn anode can be stably cycled up to 1800h at the current density of 1 mA cm−2 in the symmetric cell and displays a discharge capacity of 120.1 mAh g−1 after 1000 cycles at a current density of 1 A g−1 in a full cell. This strategy affords a generic approach for large-scale applications of metal anodes in aqueous systems. •The low current density interface is designed by the etched Zn foil. •The effects of stripping/plating behavior on the dendrite formation are analyzed. •The resultant Zn anode displays superior electrochemical performance in the cell. [ABSTRACT FROM AUTHOR]

Zinc anode is promising for various aqueous batteries due to its low cost and high theoretical specific capacity. However, poor cycling stability caused by dendritic growth seriously hampered its widespread application. Herein, we demonstrate that by using an anion-exchange membrane, quaternary ammonia poly (N -methyl-piperidine- co - p -terphenyl) (QAPPT), as the separator, the damage from short circuits can be completely prevented. More details reveal that when approaching the QAPPT membrane, Zn dendrites perform a bending growth rather than pierce through it, which helps achieve a superior cycling stability without any short. The bending growth can be ascribed to a variation of electrolyte concentration at the electrode/membrane interface where Zn electrodeposited at a very low rate in the direction perpendicular to the membrane. By using QAPPT membrane, an ultra-stable Ni–Zn full cell is then realized. This finding may pave a facile way to solve the problems associated with dendrites for diverse alkaline Zn-based batteries. Image 1 • A highly base-stable anion-exchange membrane was employed as battery separator. • The separator exhibits zincate ion-conducting property. • The unique electrode/electrolyte interface prevents the short caused by dendrites. • Providing a practical strategy for rechargeable alkaline Zn-based batteries. [ABSTRACT FROM AUTHOR]