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The practical application of aqueous zinc ion batteries (AZIBs) is impeded by the instability of the Zn anode|electrolyte interface, including dendrite growth, hydrogen evolution reaction (HER), and corrosion. Herein, the periodical micro‐nano structure is constructed on the surface of Zn anode through picosecond laser lithography (PLL) technology. This micro‐nano surface structure is conductive to obtain hydrophobicity for diminishing direct contact between the electrolyte and Zn anode, enhancing the corrosion resistance of the Zn anode. Simultaneously, the low surface energy and reconstructed electric field are achieved through laser‐induced texture microstructure, leading to the oriented Zn2+ deposition along the (002) plane. As a result, the lower electrochemical polarization and long cycling stability of 1400 h for Zn||Zn symmetric cell is achieved at 4 mA cm−2 and 2 mAh cm−2. The average coulombic efficiency (CE) of the Zn||Cu cell is enhanced to 99.83% at 2 mA cm−2, while the Zn||MnO2 cell delivers a capacity retention of 68.7% after 600 cycles at 1 A g−1. Consequently, the advantages of micro‐nano structure can highlight the importance of surface structure design for the development of stable Zn anode. [ABSTRACT FROM AUTHOR]

Aqueous Zn metal batteries (ZMBs) are largely hampered by the poor stability of zinc (Zn) anode in aqueous electrolyte due to uncontrollable deposition behavior and parasitic reactions. Hence, a stable Glu@Zn anode via acid etching is developed that simultaneously exposes (002) plane and modifies exposed grain boundaries. The surface‐preferred (002) plane is achieved by minimizing its surface energy. And the exposed grain boundaries are also modified by decomposition products of acid etching, which can greatly reduce the adverse effects caused by highly active grain boundaries. These features favor Glu@Zn anode by accrediting a long‐term cycle lifespan exceeding 4400 h with a high average coulombic efficiency (CE) of 98.9%. Surprisingly, Glu@Zn anode can run for more than 250 h with 50% Zn utilization. The assembled Glu@Zn//NH4V4O10 full batteries deliver a specific capacity of 291.6 mAh g−1 after 400 cycles even at a low current density of 0.5 A g−1. It can also obtain a stable cycling performance up to 2000 cycles. To further verify its stability, a pouch cell is constructed that can preserve stable 400 cycles with 5 mAh. This study sheds light on surface energy regulation exposing preferred crystal plane to develop highly stable and reversible cycling aqueous ZMBs. [ABSTRACT FROM AUTHOR]

The development of aqueous zinc‐ion batteries (AZIBs) for large‐scale industrial applications is substantially constrained by the persistent issue of zinc anode corrosion. This study introduces fucoidan (FCD), a corrosion inhibitor, to effectively mitigate the corrosion‐related challenges in zinc metal anodes. FCD forms a robust, covalently bonded layer on the zinc surface at a low concentration of 25 mm through interactions between the lone pairs on its polar atoms and the d orbitals of zinc. This layer is ultrathin, which does not deteriorate ion transfer but effectively shields the zinc from corrosive electrolytes and promotes uniform zinc deposition, resulting in suppressed corrosion, passivation, and dendrite formation. Consequently, the Zn||Zn cells exhibit excellent reversibility, stably operating for 2700 h at 1 mA cm−2 under 1 mAh cm−2 and 400 h at 10 mA cm−2 under 10 mAh cm−2. Furthermore, a large‐sized Zn||I2 pouch cell with a high iodine loading of 2 g and a discharge capacity of ≈300 mAh is demonstrated, which shows minimal capacity degradation—<3% after 300 cycles—and maintains a high Coulombic efficiency of ≈99.5%. The corrosion inhibition strategy proposed in this study provides crucial insights for enhancing the durability and practicability of AZIBs. [ABSTRACT FROM AUTHOR]

Zinc metal is a high‐capacity and cost‐effective anode material for aqueous zinc‐ion batteries, but its development is impeded by dendrite growth and interfacial side reactions. In this study, a unique dipole molecule (DPM) layer is constructed on a zinc surface via an in situ etching‐growth strategy to regulate the surface electric field and ion distribution. Theoretical calculations and experiments confirm that the asymmetrical charge distribution within the DPM layer can significantly remodel the electric field of the Zn anode surface. The zincophilic DPM layer accelerates the migration of zinc ions through ordered ion channels. Electro‐ionic field regulation via the DPM layer achieves dendrite‐free deposition and reduces the formation of byproducts. The DPM‐Zn symmetrical cells exhibit ultralow voltage hysteresis (≈ 24.2 mV), highly reversible zinc plating/stripping behavior, and stable cycling over 1700 h at 1 mA cm−2. The DPM‐Zn||MnO2 full cells exhibited a higher specific capacity and cycle stability than the bare Zn anode. This work verifies the feasibility of electro‐ionic‐field synergistic regulation for robust Zn anodes and provides new insights into the interface design of metal anodes. [ABSTRACT FROM AUTHOR]

The incorporation of additives into aqueous electrolytes provides substantial opportunities to mitigate dendrite formation and side reactions on zinc anodes. However, there is a lack of an effective guideline for selecting suitable electrolyte additives based on critical performance‐limiting factors. Herein, the use of the acid dissociation constant (pKa) as an intrinsic descriptor for screening suitable organic proton donors is proposed to achieve highly reversible Zn||polyaniline (PANI) batteries. Experimental results and theoretical calculations reveal that L‐malic acid (L‐MA) with a low pKa can supply constant protons to effectively reduce the accumulation of nonconductive alkaline byproducts and address the deprotonation issue of the PANI cathode. Meanwhile, the deprotonated malate anions form bidentate coordination with Zn2+, thereby reconfiguring a water‐deficient solvation structure of hydrated Zn2+ and facilitating the formation of ZnCO3‐rich solid electrolyte interphase. Taking L‐MA as a demonstration, Zn||Zn symmetric cells can stably cycle for over 460 h at a high depth of discharge of 80%. Additionally, the L‐MA additive enables Zn||PANI full cells to retain 89% capacity after 5000 cycles. The screening principle of organic proton‐donors that can simultaneously stabilize Zn anode and cathode of aqueous batteries is highlighted here. [ABSTRACT FROM AUTHOR]

The main challenge for aqueous zinc‐ion capacitors is the low stability of zinc anode. In this study, a Prussian blue analog (PBA) has been coated on the surface of zinc foil to create an inorganic protective layer. This layer features a three‐dimensional open microporous structure, which not only endows it with excellent pseudocapacitive properties but also serves as an effective barrier against dendrite growth. The presence of PBA coating can increase the nucleation point of zinc ions and provide a low‐energy barrier for the rapid migration of zinc ions. Hence, the PBA@Zn ||PBA@Zn symmetric cell exhibits exceptional cycling stability, enduring over 1400 h of operation at a current density of 1 mA cm−2 and a capacity of 1 mAh cm−2. The PBA@Zn||AC capacitor demonstrated a discharge capacity of 46.23 mAh g−1 after 10 000 cycles at a current density of 1 A g−1, with a capacity retention of 92.41%, whereas the discharge capacity of Zn||AC capacitor is only 16.02 mAh g−1, with a capacity retention of 23.13%. The PBA@Zn||AC capacitor exhibited remarkable endurance and stability, retaining a substantial discharge capacity of 32.7 mAh g−1 after 10 000 cycles at 10 A g−1. Density Functional Theory (DFT) calculations also show that PBA has a strong interaction with Zn and exhibits superior zincophilic ability. This study reports industrially applicable low‐cost Prussian blue analogs as artificial interfacial protective layers for improving the cycling stability of zinc anode with a low‐energy barrier for rapid migration of zinc ions especially at high current density. [ABSTRACT FROM AUTHOR]

Zn dendrite growth and parasitic reactions at the interface of zinc anode/electrolyte in aqueous zinc batteries severely hinder its lifespan in application. Herein, the zinc anode is effectively stabilized by introducing trace amounts of 4‐aminobutane‐1‐phosphate (ABPA) into the ZnSO4 electrolyte. The ABPA adsorbs onto the surface of zinc anode and then further decomposes to a high conductive organic/inorganic composite in situ SEI layer including amino, partial carbon chain, and zinc phosphate. In the SEI layer, the residual undecomposed carbon chain promotes the desolvation of Zn2+, the amino induces uniform Zn2+ plating and zinc phosphate facilitates the migration of Zn2+. Thus, this in situ SEI layer not only suppresses water‐related side reactions but also enhances the Zn2+ transport kinetics. As a result, Zn||Zn symmetric cell delivers an ultralong cycle life of over 13 000 cycles at 50 mA cm−2 and 1 mAh cm−2. A high average Coulombic efficiency of 99.72% is achieved in over 1000 cycles in Zn||Cu half‐cell. The Zn||I2 full cell delivers a high‐capacity retention of 91.42% after 40,000 cycles. Moreover, a 49 mAh Zn||I2 pouch cell maintains 80.28% capacity retention over 300 cycles and 61.22% after 1000 cycles. [ABSTRACT FROM AUTHOR]

Facilitating (002)‐textured zinc growth is crucial for achieving dendrite‐free zinc deposition in zinc‐ion batteries. Electrolyte engineering holds promise in directing zinc electrodeposition toward this desired orientation. However, despite the (002) plane's lower surface energy compared to other facets, it remains unclear why this plane does not dominate zinc crystal faces during electrodeposition under normal conditions. This knowledge gap underscores the need to better understand zinc electrodeposition behaviors and the influence of electrolyte compositions on its crystallographic texture. This study explores different tetraazamacrocycle derivatives as electrolyte additives. It reveals that achieving (002)‐textured zinc deposition is not solely dictated by thermodynamic equilibrium but also significantly influenced by interface dynamics. In typical ZnSO4 electrolytes, imbalanced kinetics among reduction, ion diffusion, and adatom diffusion processes lead to electroconvection and disorderly zinc accumulation, hindering proper zinc growth. In contrast, introducing specific tetraazamacrocycle derivative in the electrolyte regulates reduction rate, enhances limiting current density, and expedites adatom diffusion, mitigating hydrodynamic instability and dendrite growth. This regulation restores the thermodynamically favorable flat (002)‐textured zinc deposition, extending the zinc anode's lifespan to 1800 h at 5 mA cm−2 and 5 mAh cm−2, enabling the fabrication of a high‐performance zinc ion hybrid capacitor prototype capable of stable operation for 40 000 cycles. [ABSTRACT FROM AUTHOR]

[Display omitted] • The H 2 under organic acid regulates the reaction rate and protects the (0 0 2) crystal planes, initiating ultrathin SEI within 1 min. • The exposed (0 0 2) planes induce uniform deposition and enhance corrosion-resistance. • This SEI with organic groups exhibits excellent compatibility, low resistance and isolation of electrolyte/anode. • The ZAC1@Zn possesses practical application value due to the rapid preparation within 1 min and resistance to high current shock. Organic acid treatment can facilitate the in-situ formation of a solid electrolyte interface (SEI) on Zn foil protecting the anode from corrosion. However, the generation of hydrogen (H 2) during this process is inevitable, which is often considered detrimental to getting compact SEI. Herein, a H 2 film-assisted method is proposed under concentrated Amino-Trimethylene-Phosphonic-Acid to construct ultrathin and dense SEI within 1 min. Specifically, the (0 0 2) crystal planes survive from the etching process of 1 min due to the adhered H 2 , inducing uniform deposition and enhanced corrosion-resistance. Moreover, the H 2 can effectively regulate the reaction rate, leading to ultrathin SEI and initiating a morphology preservation behavior, which has been neglected by the previous reports. The quick-formed SEI has excellent compatibility, low resistance and effective isolation of electrolyte/anode, whose advantages work together with exposed (0 0 2) planes to get accustomed to high-current surge, leading to the ZAC1@Zn//ZAC1@Zn consistently cycling over 800 h at 15 mA cm−2 and 15 mAh cm−2, the ZAC1@Zn//Cu preserves high reversibility (CE 99.7 %), and the ZAC1@Zn//MVO exhibits notable capacity retention at 191.7 mAh/g after 1000 cycles. [ABSTRACT FROM AUTHOR]

Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety, cost‐effectiveness, and high capacity. However, the service life of zinc metal anodes is severely constrained by critical challenges, including dendrites, water‐induced hydrogen evolution, and passivation. In this study, a protective two‐dimensional metal–organic framework interphase is in situ constructed on the zinc anode surface with a novel gel vapor deposition method. The ultrathin interphase layer (~1 μm) is made of layer‐stacking 2D nanosheets with angstrom‐level pores of around 2.1 Å, which serves as an ion sieve to reject large solvent–ion pairs while homogenizes the transport of partially desolvated zinc ions, contributing to a uniform and highly reversible zinc deposition. With the shielding of the interphase layer, an ultra‐stable zinc plating/stripping is achieved in symmetric cells with cycling over 1000 h at 0.5 mA cm−2 and ~700 h at 1 mA cm−2, far exceeding that of the bare zinc anodes (250 and 70 h). Furthermore, as a proof‐of‐concept demonstration, the full cell paired with MnO2 cathode demonstrates improved rate performances and stable cycling (1200 cycles at 1 A g−1). This work provides fresh insights into interphase design to promote the performance of zinc metal anodes. [ABSTRACT FROM AUTHOR]

The research introduces trace amounts (0.1 mM) of 2-ethyl-1H-benzimidazole (EHB) into ZnSO 4 (ZS) electrolyte, regulating the nucleation overpotential of dendrite-free ZIBs. Under the influence of EHB additives, the modified electrolyte (ZS-EHB) nucleation overpotential increased from 53.0 mV to 74.2 mV. Therefore, in the ZS-EHB electrolyte, the inhibition efficiency exceeds 90%, and achieve ultra-long cycle of Zn||Zn batteries. [Display omitted] • Economical, trace, and efficient electrolyte additive EHB (0.1 mM) achieves dendrite-free zinc anode. • The strong zincophilic hydrophobic structure of EHB is effectively adsorbed on the zinc anode to regulate nucleation overpotential. • EHB achieves high reversibility of the zinc anode. Large-scale energy storage applications can greatly benefit from the low-cost and safe zinc metal anode. However, corrosion, side reactions and dendrite growth in water significantly inhibit the cycle life of zinc-ion batteries. Here, 2-ethyl-1H-benzimidazole (EHB), a strong zincophilic and hydrophobic structure, is introduced into the ZnSO 4 (ZS) electrolyte to adjust the nucleation overpotential in Zinc-ion batteries for the initial time. The strong zincophilic side of EHB firmly adheres to the zinc anode, while the hydrophobic end further protects the zinc anode from the influence of active water molecules due to steric effect. With the addition of EHB, the nucleation overpotential of the modified electrolyte (ZS-EHB) increases from 53.0 mV to 74.2 mV at 1 mA cm−2. Consequently, the inhibition efficiency of Zn anode in ZS-EHB electrolyte exceeds 90 %, and the lifespan of the symmetric Zn||Zn cells in ZS-HEB electrolyte reaches 6200 h at 5 mA cm−2 and over 2400 h at 8 mA cm−2, nearly 80-fold longer than that of the cells in ZS electrolyte. Furthermore, the designed Zn||α-MnO 2 cells can still deliver a consistent discharge capacity of 120.1 mAh g−1 even after 500 cycles. The research offers a promising route for creating zinc anode electrolyte additives. [ABSTRACT FROM AUTHOR]

The slow transport dynamics and poor dendritic growth significantly hinder the performance of zinc metal batteries. Here, a unique difunctional ion rectification strategy is developed using vacuum evaporation technology to design a coated separator for efficient ion transport. The highly conductive Cu‐coated separator acts as an ion redistributor, ensuring homogenized electric field distribution. The excellent znophilicity of the copper coating acts as an ion accelerator, promoting ion transport and facilitating face‐to‐face zinc deposition on the separator. Consequently, this synergy enables stable battery operation at high current densities (cumulative capacity up to 10 800 mAh cm−2 at 8 mA cm−2) and high depth of discharge (over 200 h at 94% DOD). The Cu‐coated separator exhibits a reversible plating/stripping life of over 2400 h with an average coulombic efficiency of 99.88%. Notably, the Cu‐coated separator significantly enhances the rate performance and cycle capacity of Zn||V6O13 and Zn||MnO2 full cells. This functional separator with a difunctional ion rectification strategy presents a promising solution to the challenge of zinc metal anodes. [ABSTRACT FROM AUTHOR]

Parasitic side reactions and dendrite growth on zinc anodes are formidable issues causing limited lifetime of aqueous zinc ion batteries (ZIBs). Herein, a spontaneous cascade optimization strategy is first proposed to regulate Zn2+ migration‐diffusion behavior. Specifically, PAPE@Zn layer with separation‐reconstruction properties is constructed in situ on Zn anode. In this layer, well‐soluble poly(ethylene oxide) (PEO) can spontaneously separation to bulk electrolyte and weaken the preferential coordination between H2O and Zn2+ to achieve primary optimization. Meanwhile, poor‐soluble polymerized‐4‐acryloylmorpholine (PACMO) is reconstructed on Zn anode as hydrophobic flower‐like arrays with abundant zincophilic sites, further guiding the de‐solvation and homogeneous diffusion of Zn2+ to achieve the secondary optimization. Cascade optimization effectively regulates Zn2+ migration‐diffusion behavior, dendrite growth and side reactions of Zn anode are negligible, and the stability is significantly improved. Consequently, symmetrical cells exhibit stability over 4000 h (1 mA cm−2). PAPE@Zn//NH4+−V2O5 full cells with a high current density of 15 A g−1 maintains 72.2 % capacity retention for 12000 cycles. Even better, the full cell demonstrates excellent performance of cumulative capacity of 2.33 Ah cm−2 at ultra‐low negative/positive (N/P) ratio of 0.6 and a high mass‐loading (~17 mg cm−2). The spontaneous cascade optimization strategy provides novel path to achieve high‐performance and practical ZIBs. [ABSTRACT FROM AUTHOR]

The catastrophic dendrite hyperplasia and parasitic reactions severely impede the future deployment of aqueous Zn‐ion batteries. Controlling zinc orientation growth is considered to be an effective method to overcome the aforementioned concerns, especially for regulating the (002) plane of deposited Zn. Unfortunately, Zn (002) texture is difficult to obtain stable cycling under high deposition capacity resulting from its large lattice distortion and nonuniform distribution in electric field. Herein, different from traditional cognition, a crystallization orientation regulation tactic is proposed to boost Zn (101) texture exposure and inhibit zinc dendrite proliferation during plating/stripping. Experimental results and theoretical calculations demonstrate the malate molecules preferentially adsorb on the Zn (002) facet, leading to the texture exposure of distinctive Zn (101) plane. Meanwhile, the −COOH and −OH groups of malate molecules exhibit strong adsorption on the Zn anode surface and chelate with Zn2+, achieving H2O‐poor electrical double layer. Very impressively, the multifunctional malate additive enlists zinc anode to survive for 600 h under a harsh condition of 15 mA cm−2/15 mAh cm−2. Moreover, the symmetric cell harvests highly‐reversible cycling life of 6600 h at 5 mA cm−2/1.25 mAh cm−2, remarkably outperforming the ZnSO4 electrolyte. The assembled Zn//MnO2 full cells also demonstrate prominent electrochemical reversibility. [ABSTRACT FROM AUTHOR]

Due to the presence of H2O within the solvated sheath of [Zn(H2O)6]2+ as well as reactive free water in the electrolyte bulk phase, the extended cycling of aqueous zinc‐ion batteries (AZIBs) is significantly affected by detrimental side reactions and the growth of Zn dendrites. This study significantly enhances the long‐term cycling stability of AZIBs by introducing a small amount of disodium malate (DM) into a 2 m ZnSO4 electrolyte solution. DM involvement in the solvation sheath of Zn2+ reduces the desolvation energy of Zn2+, thereby mitigating the corrosion and hydrogen evolution reaction (HER) of the negative electrode surface by [Zn(H2O)6]2+ ions. Additionally, DM adsorption on the zinc surface retards the reduction kinetics of Zn2+ at anode, promoting uniform distribution and predominant deposition on the flat (002) crystal plane, thus reducing dendrite formation. The assembled Zn||Zn symmetric cell exhibits stable cycling for over 500 h at 10 mA cm−2 and 5 mAh cm−2. The Zn||VO2 full cells with DM additive exhibits an ultralong cycling lifespan without capacity loss. [ABSTRACT FROM AUTHOR]

Ensuring effective and controlled zinc ion transportation is crucial for functionality of the solid electrolyte interphase (SEI) and overall performance in zinc‐based battery systems. Herein the first‐ever demonstration of incorporate cation‐π interactions are provided in the SEI to effectively facilitate uniform zinc ion flux. The artificial SEI design involves the immobilization of 4‐amino‐p‐terphenyl (TPA), a strong amphiphilic cation‐π interaction donor, as a monolayer onto a conductive poly(3,4‐ethylenedioxythiophene) (PEDOT) matrix, which enable the establishment of a robust network of cation‐π interactions. Through a carefully‐designed interfacial polymerization process, a high‐quality, large‐area, robust is achieved, thin polymeric TPA/PEDOT (TP) film for the use of artificial SEI. Consequently, this interphase exhibits exceptional cycling stability with low overpotential and enables high reversibility of Zn plating/stripping. Symmetrical cells with TP/Zn electrodes can be cycled for more than 3200 hours at 1 mA cm−2 and 1 mAh cm−2. And the asymmetric cells can cycle 3000 cycles stably with a high Coulomb efficiency of 99.78%. Also, under the extreme conditions of lean electrolyte and low N/P ratio, the battery with TP protective layer can still achieve ultra‐stable cycle. [ABSTRACT FROM AUTHOR]

The commercial utilization of Zn metal anodes with high plating capacity is significantly hindered by the uncontrolled growth of dendrites and associated side reactions. Herein, a robust artificial ion‐sieving MXene flake (MXF)‐coating layer, with abundant polar terminated groups, is constructed to regulate the interfacial Zn2+ deposition behavior. In particular, the fragmented MXF coupled with in situ generated quantum dots not only has strong Zn affinity to homogenize electric fields but also generates numerous zincophilic sites to reduce nucleation energy, thus securing a uniform dendrite‐free surface. Additionally, the porous coating layer with polar groups allows the downward diffusion of Zn2+ to achieve bottom‐up deposition and repels the excessive free water and anions to prevent parasitic reactions. The ion‐sieving effect of MXF is firmly verified in symmetric cells with high areal capacity of 10–40 mAh cm−2 (1.0 mA cm−2) and depth of discharge of 15%–60%. Therefore, the functional MXF‐coated anode manifests long‐term cycling with 2700 h of stable plating/stripping in Zn||Zn cell. Such rational design of MXF protective layer breaks new ground in developing high plating capacity zinc anodes for practical applications. [ABSTRACT FROM AUTHOR]

The feasibility of aqueous zinc‐ion batteries for large‐scale energy storage is hindered by the inherent challenges of Zn anode. Drawing inspiration from cellular mechanisms governing metal ion and nutrient transport, erythritol is introduced, a zincophilic additive, into the ZnSO4 electrolyte. This innovation stabilizes the Zn anode via chelation interactions between polysaccharides and Zn2+. Experimental tests in conjunction with theoretical calculation results verified that the erythritol additive can simultaneously regulate the solvation structure of hydrated Zn2+ and reconstruct the hydrogen bond network within the solution environment. Additionally, erythritol molecules preferentially adsorb onto the Zn anode, forming a dynamic protective layer. These modifications significantly mitigate undesirable side reactions, thus enhancing the Zn2+ transport and deposition behavior. Consequently, there is a notable increase in cumulative capacity, reaching 6000 mA h cm⁻2 at a current density of 5 mA cm−2. Specifically, a high average coulombic efficiency of 99.72% and long cycling stability of >500 cycles are obtained at 2 mA cm−2 and 1 mA h cm−2. Furthermore, full batteries comprised of MnO2 cathode and Zn anode in an erythritol‐containing electrolyte deliver superior capacity retention. This work provides a strategy to promote the performance of Zn anodes toward practical applications. [ABSTRACT FROM AUTHOR]

The carbon nanoparticles layer coated zinc anode with (1 0 3) crystal plane preferential oriented crystal structure (denoted as C@RZn) is prepared by a facile one-step vapor deposition method, and showed great potentials in extending lifespan and inhibiting dendrite growth. [Display omitted] • The C@RZn was prepared by a facile one-step vapor deposition method. • The C@RZn is combining crystallographic orientation and coating layer. • The C@RZn can guide the deposition of Zn2+ ions and inhibit the dendrite growth. • The C@RZn anode achieves a stable cycle life for more than 3000 h. • The MVO//C@RZn cell keep stable for 5000 cycles. Aqueous zinc ion batteries (ZIBs) have been considered promising energy storage systems due to their excellent electrochemical performance, environmental toxicity, high safety and low cost. However, uncontrolled dendrite growth and side reactions at the zinc anode have seriously hindered the development of ZIBs. Herein, we prepared the carbon nanoparticles layer coated zinc anode with (1 0 3) crystal plane preferential oriented crystal structure (denoted as C@RZn) by a facile one-step vapor deposition method. The preferential crystallographic orientation of (1 0 3) crystal plane promotes zinc deposition at a slight angle, effectively preventing the formation of Zn dendrites on the surface. In addition, the hydrophobic layer of carbon layer used as an inert physical barrier to prevent corrosion reaction and a buffer during volume changes, thus improving the reversibility of the zinc anode. As a result. the C@RZn anode achieves a stable cycle performance of more than 3000 h at 1 mA cm−2 with CE of 99.77 % at 5 mA cm−2. The full battery with C@RZn anode and Mn-doped V 6 O 13 (MVO) cathode show stability for 5000 cycles at the current density of 5 A g−1. This work provides a new approach for the design of multifunctional interfaces for Zn anode. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries represent a highly promising next‐generation electrochemical energy storage system because of their safety, environmental friendliness, resource abundance, and simple assembly conditions. However, the formation and growth of zinc dendrites on zinc anode seriously hinder the practical application of zinc‐ion batteries. Zincophilic design, which enables the uniform zinc nucleation/deposition, offers an effective solution to achieve dendrite‐free zinc anodes. Despite significant progress in the field of zincophilic design, the research in this field currently lacks clear analysis and guidance. This paper provides a comprehensive overview of the current research status of zincophilic design and the mechanism for dendrite‐free zinc anode from three aspects: construction of zinc anode zincophilic layers, addition of zincophilic additives in electrolyte, and construction of 3D zincophilic host. Moreover, the challenges facing the industrialization and commercialization of zinc‐ion batteries in the further are briefly discussed. [ABSTRACT FROM AUTHOR]

Aqueous battery with nonflammable and instinctive safe properties has received great attention. However, issues related to Zn anode such as side reactions and rampant dendrite growth hinder the long‐term circulation of AZMBs. Herein, an ultrathin(35 nm) MoO3 coating is deposited on the Zn anode by means of vacuum vapor deposition for the first time. Due to the peculiar layer structure of MoO3, insertion of Zn2+ in ZnxMoO3 acts as Zn2+ ion conductor, which regulates Zn2+ deposition in an ordered manner. Additionally, the MoO3 coating can also inhibit the hydrogen evolution and corrosion reactions at the interface. Therefore, both Zn//MoO3@Cu asymmetric battery and Zn symmetric battery cells manage to deliver satisfactory electrochemical performances. The symmetric cell assembled with MoO3@Zn shows a significant long cycle life of more than 1600 h at a current density of 2 mA cm−2. Meanwhile, the MoO3@Zn//Cu asymmetric cell exhibits an ultrahigh Zn deposition/stripping efficiency of 99.82% after a stable cycling of 650 h at 2 mA cm−2. This study proposes a concept of “zincophile Zn2+ conductor regulation” to dictate Zn electrodeposition and broadens novel design of vacuum evaporation for nano MoO3 modified Zn anodes. [ABSTRACT FROM AUTHOR]

Achieving reversible plating/stripping of zinc (Zn) anodes is crucial in aqueous Zn‐ion batteries (AZIBs). However, undesired dendrite growth and parasitic side reactions severely deteriorate battery lifespan. The construction of stable protective coating is an effective strategy to enhance anode stability. In this study, a multifunctional nanodiamond (ND) inorganic layer is designed and constructed on both Zn and Cu electrodes that can both effectively inhibit dendrite growth and suppress Zn anode corrosion. Experimental results and theoretical calculations demonstrate that this artificial protective layer, with ultra‐high surface energy, enables the controlled creation of abundant nucleation sites (in the order of 1012 cm−2) for the homogenization of ion flux and electric field on the anode. It is found that zinc ions preferentially adhere to the diamond surfaces with lower diffusion barriers, leading to uniform zinc deposition. A symmetric cell with the ND‐protected Zn (Zn‐ND) anode exhibits reversible plating/stripping behavior for an impressive duration of over 3600 h at 1 mA cm−2. Furthermore, the MnO2||Zn full battery retains 90% of its initial capacity after 3500 cycles at 2 A g−1, and assembled hybrid capacitor operates smoothly over 65 000 cycles at 10 A g−1. These results underscore the potential of this coating as a promising solution for achieving highly stable Zn anodes for aqueous batteries. [ABSTRACT FROM AUTHOR]

According to the first principle, the SDS anions are preferentially adsorbed on the (0 0 2) surface of the Zn anode, forming a protective layer which prevents the adsorption of free water molecules and modifies the electrode/electrolyte interface. The SDS additive significantly inhibits the contact of water molecules with the interface, reduces the generation of by-products, and effectively prevents the growth of dendrites. Consequently, with the assistance of SDS additives, the Zn||Zn symmetrical battery sustains a long cycle life for 2000h. [Display omitted] Aqueous zinc-ion batteries are emerging as powerful candidates for large-scale energy storage, due to their inherent high safety and high theoretical capacity. However, the inevitable hydrogen evolution and side effects of the deposition process limit their lifespan, which requires rational engineering of the interface between anode and aqueous electrolyte. In this paper, an anionic surfactant as electrolyte additive, sodium dodecyl sulfonate (SDS), is introduced to deliver highly reversible zinc metal batteries. Unlike traditional surfactants, the solvation structure is not affected by SDS, which tends to adsorb on the (0 0 2) crystal plane of Zn with the purpose of effectively limiting the water molecules adsorption. Attributed to the natural hydrophobic part of SDS, a dynamic electrostatic shielding layer and a unique hydrophobic interface are constructed on the anode. Assisted by the above merits, the adverse surface corrosion, hydrogen evolution and dendrite growth are significantly inhibited without the sacrifice in the deposition kinetics of Zn ions. As a result, the Zn||Zn symmetric batteries demonstrate an increased cycle life of 2000 h (1 mA cm−2, 1 mA h cm−2) with the presence of SDS additive. Such strategy provides a new avenue for the developing advanced electrolytes to be applied in aqueous energy storage systems. [ABSTRACT FROM AUTHOR]

The use of zinc (Zn) metal as an anode in aqueous batteries offers an eco‐friendly and cost‐effective energy storage solution. However, Zn dendrite formation severely restricts the cycle life of the battery toward practical application. Herein, a commercially hydrophilic polytetrafluoroethylene (PTFE) membrane is demonstrated as a separator to significantly extend the cycle life of the Zn metal anode. In contrast with the conventional fragile glass fiber separator, a wetted PTFE separator exhibited high mechanical strength (stress of 34.3 MPa at 41.4% strain) and favorable hydrophilicity, which both efficiently suppress dendrite growth. The uniform and robust pore structures are proven to facilitate a homogeneous Zn2+ ion flux and a high transfer number of Zn2+ (0.81), which has guaranteed reversible Zn plating/stripping. As a proof of concept, the PTFE separator extended the cycle life considerably to over 3000 h and promoted a Zn plating/stripping efficiency of 99.5% in the unmodified 2 m ZnSO4 aqueous electrolyte. This advancement underscores the significant potential of the PTFE separator for enhancement of the cycling durability of aqueous zinc‐ion batteries (AZIBs). [ABSTRACT FROM AUTHOR]

Aqueous Zn‐ion batteries are an attractive electrochemical energy storage solution for their budget and safe properties. However, dendrites and uncontrolled side reactions in anodes detract the cycle life and energy density of the batteries. Grain boundaries in metals are generally considered as the source of the above problems but we present a diverse result. This study introduces an ultra‐high proportion of grain boundaries on zinc electrodes through femtosecond laser bombardment to enhance stability of zinc metal/electrolyte interface. The ultra‐high proportion of grain boundaries promotes the homogenization of zinc growth potential, to achieve uniform nucleation and growth, thereby suppressing dendrite formation. Additionally, the abundant active sites mitigate the side reactions during the electrochemical process. Consequently, the 15 μm Fs−Zn||MnO2 pouch cell achieves an energy density of 249.4 Wh kg−1 and operates for over 60 cycles at a depth‐of‐discharge of 23 %. The recognition of the favorable influence exerted by UP‐GBs paves a new way for other metal batteries. [ABSTRACT FROM AUTHOR]

The electric double layer (EDL) at the electrode/electrolyte interface plays a crucial role to the electrochemical reactions of zinc ion batteries. For Zn anode, the EDL consists of H2O dipoles, which can cause Zn corrosion and passivation. Herein, the localized electronic‐rich (LER) structure performing as soild electrolyte interphase (SEI) changes the electron distribution, leading to the rapid capture of Zn2+, thus promoting the desolvation of the cH2O shell. Moreover, the LER generates an electrostatic repulsion effect to SO42−. Consequently, a unique H2O‐poor EDL is reconstructed with the distribution of Zn2+‐H2O‐SO42−, which inhibits side reactions and improves the deposition kinetics of Zn2+. In situ Raman intuitively confirms that the zinc‐ion‐flux is uniform during the whole electroplating process. LER as regulator for EDL structure, leads to smooth and fast Zn2+ deposition. The performance enhancement is demonstrated by LER@Zn//LER@Zn cells, which exhibit exceptional lifespan for 4800 h. Furthermore, the LER@Zn///MnO2 cell shows improved cycling stability over 1500 cycles, with a high capacity of 124 mAh g−1 at 5 C. [ABSTRACT FROM AUTHOR]

Practical aqueous zinc‐ion batteries require low‐cost thin zinc anodes with long‐term reversible stripping/depositing. However, thin zinc anodes encounter more severe issues than thick zinc, such as dendrites and uneven stripping, resulting in subpar performance and limited lifetimes. Here, this work proposes a three‐in‐one zinc anode obtained by a large‐scale two‐step method to address the above issues. In a three‐in‐one zinc anode, the copper foil as an inactive current collector solves the gradual reduction of the active area when only the pure zinc as an active current collector. This work develops an automatic electroplating device that can continuously deposit a zinc layer on a conducting foil to meet the demand for zinc‐coated copper foils. The sodium carboxymethylcellulose (CMC)‐zinc fluoride (ZnF2) protective layer prevents direct contact between zinc and separator, and provides a uniform and sufficient supply of zinc ions. The CMC‐ZnF2‐coated copper foil performs up to 3000 reversible zinc deposition/stripping cycles with a cumulative capacity of 6 Ah cm−2 and an average Coulombic efficiency of 99.94%. The Zn||ZnVO cell using the three‐in‐one anode achieved a high capacity retention of over 70% after 15 000 cycles. The proposed three‐in‐one anode and the automatic electroplating device will facilitate industrialization of practical thin zinc anodes. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries are promising for next‐generation energy storage systems. However, the zinc dendrite growth, corrosion, and hydrogen evolution reaction at the electrochemical interface severely impede their further development. Herein, a Zn2+‐rich and H2O‐poor Helmholtz plane is constructed to regulate the electrochemical interface between the zinc anode and the electrolyte. Electrochemical and in situ spectroscopy characterizations reveal that the designed electric double layer with abundant Zn2+ coordination sites and less H2O content can facilitate rapid electron transfer, homogenize Zn2+ deposition, and alleviate the side reactions induced by active H2O. Benefiting from the high reversibility and stability of zinc anode, the Zn||Zn symmetric cell can be cycled over 1000 h at 1 mA cm−2 and the Zn||NH4V4O10 full cell can maintain a capacity of 85.23% for 1000 cycles at 3 A g−1. This work aims at Helmholtz plane reconfiguration and provides a realizable strategy in interface construction for other similar systems. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous zinc metal batteries (AZMBs) are considered as a potential alternative to lithium‐ion batteries due to their low cost, high safety, and environmental friendliness. However, the Zn anodes in AZMBs face severe challenges, such as dendrite growth, metal corrosion, and hydrogen evolution, all of which are closely related to the Zn/electrolyte interface. This article offers a short review on surface passivation to alleviate the issues on the Zn anodes. The composition and structure of the surface layers significantly influence their functions and then the performance of the Zn anodes. The recent progresses are introduced, according to the chemical components of the passivation layers on the Zn anodes. Moreover, the challenges and prospects of surface passivation in stabilizing Zn anodes are discussed, providing valuable guidance for the development of AZMBs. [ABSTRACT FROM AUTHOR]

With the development of social industrialization, energy issues have become a hot topic at present. Traditional lithium-ion batteries, due to their poor safety and high cost, cannot meet the current application needs in the energy storage field in the long term. Therefore, the development of suitable new energy has aroused people's deep thinking. Aqueous zinc-ion batteries (AZIBs) have attracted attention from the scientific research community in recent years due to their high safety, cleanliness, and other advantages. However, dendrites are easily grown on the zinc anode, and free water molecules can also corrode the zinc anode, causing side reactions such as hydrogen evolution and passivation, seriously affecting the long-term cycling performance and stability of the battery. This work introduces a new type of ionic liquid additive 1-cyanobutyl-3-methylimidazole chloride (MCBI) to optimize aqueous electrolytes. Before the deposition of zinc ions on the anode surface, MCBI cations will preferentially land on the anode. Due to their special structures of Electron-withdrawing group and nitrogen heterocycles, they will tightly adsorb on the zinc surface in a unique shape of the “Check mark” posture. This provides abundant sites for the deposition of zinc ions, allowing zinc atoms to arrange regularly between MCBI ions, thereby reducing the generation of dendrites. Due to the steric hindrance effect, by-products (Zinc hydroxide sulfate) will also accumulate in an orderly manner around additive ions, forming channels for uniform deposition of zinc ions; The hydrophobic alkyl groups of MCBI cations will repel most of the free water molecules outside the anode, thereby reducing hydrogen evolution reaction (HER). In this work, under the optimal concentration conditions, the Coulomb efficiency of Zn//Cu asymmetric cell with MCBI additive can reach 99. 37% after 200 cycles; Zn//Zn symmetric batteries can stably cycle for more than 1600 h at low current density (0. 5 mA/cm2), and can cycle for more than 1000 h at 10 mA/cm², 5 mA·h/cm². Finally, VO2 as the cathode maintains a high-capacity retention rate of 88. 5% after 500 cycles in the full battery. This work provides new ideas for the anode modification strategy of aqueous zinc ion batteries. [ABSTRACT FROM AUTHOR]

The stability of Zinc metal anodes (ZMAs) significantly limits the electrochemical performance and practical application of aqueous Zn‐ion batteries (ZIBs). An efficient and economical solution is the use of trace additives. However, efforts on trace additives are sparse, and essential uncertainties remain concerning their role in the stabilization of ZMAs. Herein, a low‐cost ZnSO4‐based aqueous electrolyte containing trace amounts of Acesulfame‐K (AK) (only 1.0 mg mL−1) is reported, which effectively suppresses the parasitic reactions occurring on the ZMA surface to realize a dendrite‐free Zn2+ deposition process, an ultra‐long cycle life over 1600 h and a high Coulombic efficiency of 99.86%. Accordingly, the practical Zn//NH4V4O10 full cell with AK also exhibits a high discharge capacity and capacity retention. In situ spectroscopies coupled with theoretical calculations reveal that the trace AK tends to accumulate at the ZMA/electrolyte interface to alleviate electrolyte corrosion. More importantly, the adsorbed AK can regulate the interfacial H2O structures (i.e., disrupting the interfacial H‐bonds to form more isolated H2O) to reduce the proton/hydroxides transport, thus suppressing the parasitic hydrogen evolution reaction and improving low‐temperature acclimation. This study provides design inspiration for trace additives expected to enable low‐cost and practical ZIBs with long lifespans. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐based energy storage devices have competitive advantages such as high power density, good safety, and wide source. However, because of the direct touch among zinc anode and aqueous electrolyte, dendrite growth and electrode side reactions are easy to occur in the plating and striping process, which seriously hinders the further development of aqueous zinc‐based energy storage devices. Therefore, it is urgent to solve the above problems to expand the existing energy storage devices. In this work, by adding an imidazo[1,2‐b]pyridazine (IP) electrolyte additive, the dendrites' growth and corrosion on the zinc anode surface could be effectively inhibited by the shielding‐anchoring double effects, which are verified by the comprehensive in situ and ex situ characterization techniques as well as the theoretical calculation support. Accordingly, the IP‐based electrolyte encourages extremely high stable zinc anode (cycling 2200 h at 1 mA cm−2) with high average Coulombic efficiency (98.72%). Moreover, the IP‐based Zn‐V2O5 full battery also exhibits excellent reversible capacity, reaching 160.8 mAh g−1 after 400 cycles at 2 A g−1. Through a straightforward alteration to the Zn anode surface, this study considerably enhances the use of highly stable and secure aqueous zinc‐ion batteries. [ABSTRACT FROM AUTHOR]

The trivalent Gd3+ ions are introduced as electrolyte additives to form an electrostatic shielding layer on the surface of the zinc anode, resulting in a highly stable and reversible zinc metal anode. [Display omitted] • The Gd3+ ions can form an electrostatic shielding layer on the zinc anode to promote the uniform deposition of Zn2+ ions. • The adsorbed Gd3+ ions acted as a buffer interface, reducing the direct contact between the zinc anode and H 2 O and thus inhibiting the interfacial parasitic reaction. • The Zn//Zn and Zn//MnO 2 cells exhibit extended cycle life and enhanced rate capability. Aqueous zinc-ion batteries (AZIBs) have become an ideal candidate for large-scale energy storage systems owing to their inherent safety and highly competitive capacity. However, severe dendrite growth and side reactions on the surface of zinc metal anodes lead to quick performance deterioration, seriously impeding the commercialization of AZIBs. In this work, a self-regulated zinc metal/electrolyte interface is constructed to solve these problems by incorporating the trivalent Gd3+ additive with a lower effective reduction potential into the aqueous ZnSO 4 electrolyte. It is revealed that the inert Gd3+ ions preferentially adsorb on the active sites of the zinc anode, and the induced electrostatic shielding layer is beneficial to uniform Zn deposition. Meanwhile, the adsorbed Gd3+ ions act as a buffer interface to lower the direct contact of the zinc anode with water molecules, thereby suppressing the interfacial parasitic reaction. These features endow the Zn//Zn battery using 0.2 M Gd3+ ions with 2940 h of cycling life at 5 mA cm−2 and a cumulative plating capacity (CPC) of 6.2 Ah cm−2 at 40 mA cm−2. When assembling with a MnO 2 cathode, the full cell using the modified electrolyte exhibits a high capacity of 268.9 mAh/g at 0.2 A/g, as well as improved rate capability and cycle stability. The results suggest the great potential of a rare earth ion additive in reinforcing Zn metal anodes for developing practical AZIBs. [ABSTRACT FROM AUTHOR]

The rapid advancement of wearable devices and flexible electronics has spurred an increasing need for high-performance, thin, lightweight, and flexible energy storage devices. In particular, thin and lightweight zinc-ion batteries require battery materials that possess exceptional flexibility and mechanical stability to accommodate complex deformations often encountered in flexible device applications. Moreover, the development of compact and thin battery structures is essential to minimize the overall size and weight while maintaining excellent electrochemical performance, including high energy density, long cycle life, and stable charge/discharge characteristics, to ensure their versatility across various applications. Researchers have made significant strides in enhancing the battery's performance by optimizing crucial components such as electrode materials, electrolytes, separators, and battery structure. This review provides a comprehensive analysis of the design principles essential for achieving thinness in zinc-ion batteries, along with a summary of the preparation methods and potential applications of these batteries. Moreover, it delves into the challenges associated with achieving thinness in zinc-ion batteries and proposes effective countermeasures to address these hurdles. This review concludes by offering insights into future developments in this field, underscoring the continual advancements and innovations that can be expected. [ABSTRACT FROM AUTHOR]

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 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. [ABSTRACT FROM AUTHOR]

Zinc‐ion batteries (ZIBs) have attracted wide attention due to their low redox potential, high capacity, and intrinsic safety. However, key issues such as zinc dendrite growth, corrosion, and passivation on zinc anode detrimentally affect the electrochemical performance. Herein, as proof of a concept of oligopeptide, glutathione with functional groups including –NH2 and −SH is introduced as an electrolyte additive to construct a multifunctional electrode–electrolyte interface layer on the zinc anode. A protonated amino group (NH3+) is formed, which prevents the adsorption of water molecules on the Zn anode, building a hydrophobic interface layer and thus attenuating corrosion. Moreover, the strong interaction between the −SH and the zinc allows glutathione molecules to be tightly anchored to the electrode surface, constructing a robust interface layer. Consequently, a long cycling life of nearly 3000 h at 1 mA cm−2 for the Zn||Zn symmetric battery is achieved, and a stable cycling life of 1600 h is demonstrated at 3 mA cm−2. Furthermore, Zn||activated carbon (AC) hybrid capacitor with the glutathione‐containing electrolyte runs stably for nearly 28 000 cycles at 5 A g−1, among the best results of reported Zn hybrid capacitors. [ABSTRACT FROM AUTHOR]

ErCl 3 as an electrolyte additive can significantly improve the cycle stability of Zn anode due to the synergistic effect of Er3+ and Cl−, as a result, the Zn||Zn symmetric batteries can stably cycle more than 1100 h. [Display omitted] • ErCl 3 was first introduced as an additive to stabilise the Zn anode. • The ErCl 3 additive could enhance the Zn anode stability by "electrostatic shielding" effect and reducing polarization. • Zn|| Zn-symmetric battery can be stable cycling for 1100 h at 1 mA cm−2 with a fixed capacity of 1 mAh cm−2. • Zn||MnO 2 full battery based on ErCl 3 -added electrolyte illustrates a reversible capacity of 157.1 mAh/g after 500 cycles. Rechargeable aqueous-zinc ion batteries (AZIB) have notable benefits in terms of high safety and low cost. Nevertheless, the challenges, such as dendrite growth, zinc anode corrosion, and hydrogen evolution reaction, impede its practical implementation. Hence, this study proposes the introduction of an economical ErCl 3 electrolyte additive to stabilize the Zn anode surface and address the aforementioned issues. The introduced Er3+ will cover the raised zinc dendrite surface and weaken the "tip effect" on the surface of the zinc anode via the "electrostatic shielding" effect. Simultaneously, the introduced Cl– can reduce the polarization of the zinc anode. Due to the synergistic effect of Er3+ and Cl–, the zinc anode corrosion, dendrite growth and hydrogen evolution have been efficiently inhibited. As a result, the Zn||Zn-symmetric battery using ErCl 3 additive can stably cycle for 1100 h at 1 mA cm−2, 1 mAh cm−2, and exhibit a high average coulomb efficiency (99.2 %). Meanwhile, Zn||MnO 2 full battery based on ErCl 3 -added electrolyte also demonstrates a high reversible capacity of 157.1 mAh/g after 500 cycles. Obviously, the capacity decay rate of the full battery is also improved, only 0.113 % per cycle. This study offers a straightforward and economically efficient method for stabilizing the zinc anode and realizing high-performance AZIBs. [ABSTRACT FROM AUTHOR]

Resting, a common procedure performed before cycling, is identified to have a significant impact on the cycle performance of acidic aqueous zinc‐ion batteries (AZBs). It is demonstrated that resting duration significantly affects the Zn anode's cyclability and is closely related to the evolution of zinc hydroxide sulfate (ZHS), a byproduct formed on the Zn anode in AZBs, even without electrochemical cycling. Mechanism analysis suggests that both the uniformity and quantity of ZHS are critical factors in determining the electrode's cycling stability. Consequently, controlling the interfacial ZHS effectively enhances the cycle performance of the Zn electrode by preventing Zn corrosion and promoting uniform Zn stripping/plating during cycling. It is demonstrated that an effective hydrothermal ZHS layer can protect the Zn electrode, rendering it less susceptible to resting impacts, resulting in a long cycle life of over 3800 h at 2 mA cm−2−0.5 mAh cm−2. With a 30% depth of discharge, this strategy helps to extend the cycle life to >1000 h. (4 mA cm−2–2 mAh cm−2). The findings not only highlight the importance of standardizing the resting period in evaluating the AZBs performance, but also lead to the relationship understanding among resting, ZHS evolution, and Zn electrode cyclability, further guiding strategy to improve the cycling stability of AZBs. [ABSTRACT FROM AUTHOR]

Abstract The commercial utilization of Zn metal anodes with high plating capacity is significantly hindered by the uncontrolled growth of dendrites and associated side reactions. Herein, a robust artificial ion‐sieving MXene flake (MXF)‐coating layer, with abundant polar terminated groups, is constructed to regulate the interfacial Zn2+ deposition behavior. In particular, the fragmented MXF coupled with in situ generated quantum dots not only has strong Zn affinity to homogenize electric fields but also generates numerous zincophilic sites to reduce nucleation energy, thus securing a uniform dendrite‐free surface. Additionally, the porous coating layer with polar groups allows the downward diffusion of Zn2+ to achieve bottom‐up deposition and repels the excessive free water and anions to prevent parasitic reactions. The ion‐sieving effect of MXF is firmly verified in symmetric cells with high areal capacity of 10–40 mAh cm−2 (1.0 mA cm−2) and depth of discharge of 15%–60%. Therefore, the functional MXF‐coated anode manifests long‐term cycling with 2700 h of stable plating/stripping in Zn||Zn cell. Such rational design of MXF protective layer breaks new ground in developing high plating capacity zinc anodes for practical applications.

Aqueous zinc-ion batteries (AZIBs) are promising contenders for energy storage systems owing to their low cost and high safety. However, their practical application is hindered by uncontrolled Zn dendrites and other side reactions. Here, the three-dimensional (3D) TiO2/Cu2Se/C heterostructure layer derived from MXene/Cu-MOF is constructed on the Zn anode to control the deposition/dissolution behavior, which has numerous active sites, better electrical conductivity and excellent structural stability. Based on DFT calculation, the built-in electric field (BIEF) formed of TiO2/Cu2Se/C can enhance charge transfer and ionic diffusion to inhibit the dendrites. Furthermore, hydrophobic coating has the ability to impede the corrosion and hydrogen evolution reaction (HER) of zinc anode. Thus, TiO2/Cu2Se/C@Zn enable the stable and reversible Zn plating/stripping process with the outstanding lifetime of 1100 h at 2 mA·cm–2 and even 650 h at 10 mA·cm–2. The batteries constructed with commercial MnO2 cathodes demonstrate the remarkable capacity (248.7 mAh·g−1 at 0.1 A·g−1) and impressive cycle stability (with 71.3% capacity retention after 300 cycles). As well as extending the life of AZIBs, this study is also motivating for other metal anode based secondary batteries.