Achieving Ultra-Long Cycle Life of Zn Anode Using ZnSn(OH)6 Coating Layer via Desolvation Effect and Uniform Zn2+ Flux.

Aqueous zinc-ion batteries (AZIBs) are considered as a promising energy storage system because of good safety, low cost, abundant resources, and environmental friendliness. However, the bottlenecks including dendrite growth, hydrogen evolution, and corrosion seriously limit their practical application. Herein, a novel ZnSn(OH)6 coating layer with rich hydroxyl groups is employed to achieve highly stable Zn anode. The hydroxyl groups can feasibly interact with H2O molecules, contributing to the desolvation of hydrated Zn2+ and the inhibition of side reactions on Zn anode surface. Furthermore, according to the DFT calculation, the adsorption energy of Zn2+ among various sites on the surface of ZnSn(OH)6 coating layer is relatively large, which helps the uniform distribution of Zn2+ flux and the prevention of dendrite growth. Consequently, the ZnSn(OH)6@Zn anode delivers ultra-long cycle life (6770 h), low polarization voltage (27 mV), and high Coulombic efficiency (99.2% over 800 cycles) at 1 mA cm-2, 1 mAh cm-2. Besides, the assembled NaV3O8·xH2O//ZnSn(OH)6@Zn full cell can operate stably for 1500 cycles at 2 A g-1 with a high specific capacity of 144.9 mAh g-1, demonstrating an excellent application potential. This simple and effective coating layer with high electrochemical performance provides an appealing strategy for the development of rechargeable AZIBs.

Thin Zinc Electrodes Stabilized with Organobromine-Partnered H2O-Zn-MeOH Cluster Ions for Practical Zinc-Metal Pouch Cells.

The utilization of thin zinc (Zn) anodes with a high depth of discharge is an effective strategy to increase the energy density of aqueous Zn metal batteries (ZMBs), but challenged by the poor reversibility of Zn electrode due to the serious Zn-consuming side reactions at the Zn||electrolyte interface. Here, we introduce 2-bromomethyl-1,3-dioxolane (BDOL) and methanol (MeOH) as electrolyte additive into aqueous ZnSO4 electrolyte. In the as-formulated electrolyte, BDOL with a strong electron-withdrawing group (-CH2Br) tends to pair with the H2O-Zn-MeOH complex, leading to the formation of organobromine-partnered H2O-Zn-MeOH cluster ions. During the Zn electrodeposition process, the formed ZnO-dominated by-products induce the polymerization of BDOL monomers, which are previously adsorbed on the electrode. As a result, a uniform dual-layer SEI with ZnO-dominated outer layer and polyether-dominated inner layer is built on the surface of Zn electrode. With such an in-situ formed dual-layer SEI, the Zn||Mg0.9Mn3O7·2.7H2O pouch cell using a 10-um Zn anode (corresponding to a low negative to positive areal capacity ratio of 3.56) successfully operated for 300 cycles with a high capacity retention of 86%, promising a high practical energy density of > 120 Wh/kg (based on the total mass of Zn and Mg0.9Mn3O7·2.7H2O).

Ultrathin surface coating of conductive and zincophilic titanium oxynitride enables stable zinc anodes for aqueous zinc-ion batteries.

The lifespan of aqueous zinc ion batteries (AZIB) has been hindered by the instability of zinc anodes, encountering challenges such as irregular dendritic growth, corrosion and hydrogen evolution reactions. In this study, we address these challenges by employing atomic-layer deposition (ALD) to create an ultrathin, conductive titanium oxynitride (TiNxOy) coating with abundant zincophilic sites. This atomic-scale coating serves as a bi-functional barrier that isolates the zinc metal from the electrolyte, thereby reducing spontaneous corrosion and mitigating hydrogen evolution. Additionally, the TiNxOy layer improves the distribution of the interfacial electric field and promotes uniform zinc plating and stripping. As a result, the TiNxOy-coated zinc anode demonstrates a significantly reduced over-potential and enhanced cycling stability, maintaining performance over 1300 h at 1 mA cm-2 in a symmetric cell. When coupled with a MnO2 cathode, the full cell achieves a capacity of 85.3 mAh g-1 after 4500 cycles at a high current density of 10C.

Anion Receptor-manipulated solvation chemistry and electric double layer enables high Zn-Utilization rate and lean Zn metal batteries.

The practical application of aqueous Zn metal batteries (AZMBs) is impeded by inferior reversibility and stability of Zn metal anode (ZMA) originated from side reactions and dendrite growth. Herein, anion receptor l-Proline (LP) is selected to simultaneously manipulate solvation chemistry and electric double layer (EDL) for constructing dendrite-free and stable AZMBs with an ultra-high depth of discharge (DOD of 100 %) and low negative/positive capacity ratio (N/P of 1.1). Experimental and computational results demonstrate that the strong interaction between -SO32- group from OTf- anion and LP promotes the coordination effect of cation and solvent, which improves the stability of electrolyte and induces fine and uniform Zn nucleus formation. Meanwhile, the preferential reduction of OTf- and adsorption of LP establish an anion-derived ZnF2-rich solid electrolyte interface by altering EDL structure, which enhances the mechanical stability and Zn2+ diffusion kinetics of the interface and prevents the contact of H2O molecules. Consequently, ZMA in LP/Zn(OTf)2 electrolyte delivers a satisfactory cycling lifespan under DOD of 100 % and an outstanding Coulombic efficiency of 99.93 % for 10,000 cycles at 10 mA cm-2. Moreover, Zn||Od-NH4V4O10 full cells with LP/Zn(OTf)2 electrolyte demonstrate excellent cycle stability at high cathode loading (20.412 mg), low N/P (1.1), and high temperature (50 °C).

Tailoring Zn2+ Flux by an Ion Acceleration Layer Modified Separator for High-Rate Long-Lasting Zn Metal Anodes.

A large concentration gradient originating from sluggish ion transport on the surface of Zn metal anodes will result in uneven Zn2+ flux, giving rise to severe dendrite growth, especially at high current density. Herein, an ion acceleration layer is introduced by a facile separator engineering strategy to realize modulated Zn2+ flux and dendrite-free deposition. Zinc hexacyanoferrate as the modifying agent featuring strong zincophilicity and rapid diffusion tunnel can enable fast trap for Zn2+ near the electrode surface and immediate transport onto deposition sites, respectively. The ion acceleration effect is substantiated by improved ion conductivity, decreased activated energy, and promoted Zn2+ transference number, which can moderate concentration gradient to guide homogenous Zn2+ flux distribution. As a result, the separator engineering guarantees Zn||Zn symmetrical cells with long-term stability of 2700 h at 2 mA cm-2, and 1770 h at a large current density of 10 mA cm-2. Moreover, cycling stability and rate capability for full cells with different cathodes can be substantially promoted by the modified separator, validating its superior practical feasibility. This study supplies a new scalable approach to tailoring ion flux near the electrode surface to enable robust Zn metal anodes at a high current density.

Anion Chemistry towards On-Site Construction of Solid-Electrolyte Interface for Highly Stable Metallic Zn Anode.

Reversibility of metallic Zn anode serves as the corner stone for the development of aqueous Zn metal battery, which motivates scrutinizing the electrolyte-Zn interface. As the representative organic zinc salt, zinc trifluorosulfonate (Zn(OTf)2) facilitates a broad class of aqueous electrolytes, however, the stability issue of Zn anode remains crucial. The great challenge lies in the lack of Zn anode protection by the pristinely formed surface structure in aqueous Zn(OTf)2 electrolytes. Accordingly, an electrochemical route was developed to grow a uniform zinc trifluorosulfonate hydroxide (ZTH) layer on Zn anode as an artificial SEI, via regulation on metal dissolution and strong coordination ability of zinc ions. Co-precipitation was proposed to be the formation mechanism for the artificial SEI, where the reduction stability of OTf‾ anion and the low-symmetry layer structure of ZTH was unmasked. This artificial SEI favors interfacial kinetics, depresses side reactions, and well maintains its integrity during cycling, leading to a prolonged lifespan of Zn stripping/plating with a high DOD of ~85%, and an improved cycling stability of ~92% retention rate for V2O5/Zn cell at 1 A g-1. The unveiled role of anion on Zn anode drives the contemplation on the surface chemistry for the blooming aqueous rechargeable battery.

Grain Boundary Filling Empowers (002)-Textured Zn Metal Anodes with Superior Stability.

Aqueous Zn battery is promising for grid-level energy storage due to its high safety and low cost, but dendrite growth and side reactions at the Zn metal anode hinder its development. Designing Zn with (002) orientation improves the stability of the Zn anode, yet grain boundaries remain susceptible to corrosion and dendrite growth. Addressing these intergranular issues is crucial for enhancing the electrochemical performance of (002)-textured Zn. Here, a strategy based on grain boundary wetting to fill intergranular regions and mitigate these issues is reported. By systematically investigating boundary fillers and filling conditions, In metal is chosen as the filler, and one-step annealing is used to synergistically convert commercial Zn foils into single (002)-textured Zn while filling In into the boundaries. The inter-crystalline-modified (002)-textured Zn (IM(002) Zn) effectively inhibits corrosion and dendrite growth, resulting in excellent stability in batteries. This work offers new insights into Zn anode protection and the development of high-energy Zn batteries.

High-Performance Aqueous Calcium Ion Batteries Enabled by Zn Metal Anodes with Stable Ion-Conducting Interphases.

Aqueous calcium ion batteries, promising for energy storage, are still challenged by very limited anode choices. Although a Zn metal anode is popular in aqueous batteries, interface instability due to incessant corrosion and severe Zn dendrites hinders its development. Here, an interphase layer with densely packed nanocrystals of Ca3(CO3)2(OH)2·1.5H2O and ZnF2, and amorphous organic species, is demonstrated for a Zn metal anode with 1 M calcium trifluoromethyl sulfonate aqueous electrolyte. The hybrid interface fully avoids direct Zn-H2O contact, maintains fast ion conductivity, and effectively prevents corrosion and dendrite growth. Therefore, the symmetric cell stably lasts for 1600 h at 0.5 mA cm-2 and 2.5 mAh cm-2, far superior to 150 h for the control cell. Furthermore, the device maintains 80% capacity retention after 700 cycles at 1 A g-1, outperforming 13% retention after 200 cycles for the control device. This work indicates that interface and interphase engineering is also crucial for aqueous batteries.

Dual-Functional Interfacial Layer Enabled by Gating-Shielding Effects for Ultra-Stable Zn Anode.

Large-scale application of low-cost, high-safety and environment-compatible aqueous Zn metal batteries (ZMBs) is hindered by Zn dendrite failure and side reactions. Herein, highly reversible ZMBs are obtained by addition of trace D-pantothenate calcium additives to engineer a dual-functional interfacial layer, which is enabled by a bioinspired gating effect for excluding competitive free water near Zn surface due to the trapping and immobilization of water by hydroxyl groups, and guiding target Zn2+ transport across interface through carboxyl groups of pantothenate anions, as well as a dynamic electrostatic shielding effect around Zn protuberances from Ca2+ cations to ensure uniform Zn2+ deposition. In consequence, interfacial side reactions are perfectly inhibited owing to reduced water molecules reaching Zn surface, and the uniform and compact deposition of Zn2+ is achieved due to promoted Zn2+ transport and deposition kinetics. The ultra-stable symmetric cells with beyond 9000 h at 0.5 mA cm-2 with 0.5 mAh cm-2 and over 5000 h at 5 mA cm-2 with 1 mAh cm-2, and an average Coulombic efficiency of 99.8% at 1 mA cm-2 with 1 mAh cm-2, are amazingly realized. The regulated-electrolyte demonstrates high compatibility with verified cathodes for stable full cells. This work opens a brand-new pathway to regulate Zn/electrolyte interface to promise reversible ZMBs.

Nonflammable Fluorinated Electrolyte Realizing High Voltage Anode-Free Zn Dual-Ion Batteries.

Due to the low decomposition potential of H2O and its corrosive effect to Zn foil, the Zn metal battery with aqueous electrolytes operates within a narrow electrochemical window and exhibits low anode utilization ratio. Fluorinated carbonate ester, exhibiting low highest occupied molecular orbital (HOMO) energy level, is suitable for constructing high-voltage batteries, yet its application in Zn metal battery has been scarcely explored. Herein, we propose an electrolyte based on fluorinated solvents and ethoxy (pentafluoro) cyclotriphosphazene (PFPN) additive, which exhibits a high decomposition voltage of 2.75 V in Zn batteries. The fluorinated carbonate esters possess non-flammability and exhibit reduced solvation capacity which in turn promotes the incorporation of anions into Zn2+ solvation shell. Consequently, an anion-derived interface layer is formed on Zn anode, aiding the compact and planar growth of deposited Zn. Therefore, the Zn//Zn cell exhibits an impressive Zn utilization of 91 % for 140 h, a level seldom reported previously. Benefitting from the oxidation resistant solvents and cathode-electrolyte interface layer formed by PFPN additive, the Zn//graphite dual-ions battery shows an extended cycling life of 1000 cycles. Furthermore, an anode-free cell was constructed and stably operated for 100 cycles, with a notably high average discharge midpoint voltage of 1.84 V.

Selection of Negative Charged Acidic Polar Additives to Regulate Electric Double Layer for Stable Zinc Ion Battery.

Zinc-ion batteries are promising for large-scale electrochemical energy storage systems, which still suffer from interfacial issues, e.g., hydrogen evolution side reaction (HER), self-corrosion, and uncontrollable dendritic Zn electrodeposition. Although the regulation of electric double layer (EDL) has been verified for interfacial issues, the principle to select the additive as the regulator is still misted. Here, several typical amino acids with different characteristics were examined to reveal the interfacial behaviors in regulated EDL on the Zn anode. Negative charged acidic polarity (NCAP) has been unveiled as the guideline for selecting additive to reconstruct EDL with an inner zincophilic H2O-poor layer and to replace H2O molecules of hydrated Zn2+ with NCAP glutamate. Taking the synergistic effects of EDL regulation, the uncontrollable interface is significantly stabilized from the suppressed HER and anti-self-corrosion with uniform electrodeposition. Consequently, by adding NCAP glutamate, a high average Coulombic efficiency of 99.83% of Zn metal is achieved in Zn|Cu asymmetrical cell for over 2000 cycles, and NH4V4O10|Zn full cell exhibits a high-capacity retention of 82.1% after 3000 cycles at 2 A g-1. Recapitulating, the NCAP principle posted here can quicken the design of trailblazing electrolyte additives for aqueous Zn-based electrochemical energy storage systems.

Sieving-type Electric Double Layer with Hydrogen Bond Interlocking to Stable Zinc Metal Anode.

The stability of aqueous zinc metal batteries is significantly affected by side reactions and dendrite growth on the anode interface, which primarily originate from water and anions. Herein, we introduce a multi H-bond site additive, 2, 2'-Sulfonyldiethanol (SDE), into an aqueous electrolyte to construct a sieving-type electric double layer (EDL) by hydrogen bond interlock in order to address these issues. On the one hand, SDE replaces H2O and SO4 2- anions that are adsorbed on the zinc anode surface, expelling H2O/SO4 2- from the EDL and thereby reducing the content of H2O/SO4 2- at the interface. On the other hand, when Zn2+ are de-solvated at the interface during the plating, the strong hydrogen bond interaction between SDE and H2O/SO4 2- can trap H2O/SO4 2- from the EDL, further decreasing their content at the interface. This effectively sieves them out of the zinc anode interface and inhibits the side reactions. Moreover, the unique characteristics of trapped SO4 2- anions can restrict their diffusion, thereby enhancing the transference number of Zn2+ and promoting dendrite-free deposition and growth of Zn. Consequently, utilizing an SDE/ZnSO4 electrolyte enables excellent cycling stability in Zn//Zn symmetrical cells and Zn//MnO2 full cells with lifespans exceeding 3500 h and 2500 cycles respectively.

Molecular Filter Net Synergy with Regulation in Ion Percolation for High-Performance Zn Metal Batteries.

The uncontrollable dendrite growth and complex parasitic reactions of Zn metal anodes cause short cycle lives and low Coulombic efficiency, which seriously affect their applications. To address these issues, this research proposes an efficient ion percolating interface constituted by a hydrogen-bonded organic framework (HND) for a highly stable and reversible Zn anode. The hydrogen-bonded skeleton acts as a molecular filter net, capturing water molecules by forming targeted hydrogen-bonding systems with them, sufficiently inhibiting parasitic reactions. Additionally, the interaction of the rich-N and -O electrochemically active sites with Zn2+ effectively regulates its percolation, which greatly enhances the diffusion kinetics of Zn2+, thus facilitating rapid and uniform migration of Zn2+ at the anode surface. Through the above synergistic effect, dendrite-free anodes with highly reversible Zn plating/stripping behaviors can be achieved. Hence, the modified Zn anode (HND@Zn) performs a steady cycling time of more than 1700 h at 1 mA cm-2. Moreover, the HND@Cu||Zn asymmetric cell exhibits a stable charge/discharge process of over 1600 cycles with an average Coulombic efficiency of up to 99.6% at 5 mA cm-2. This work provides some conceptions for the evolution and application of high-performance Zn metal batteries.

High-Entropy-Inspired Multicomponent Electrical Double Layer Structure Design for Stable Zinc Metal Anodes.

Regulating the electrical double layer (EDL) structure can enhance the cycling stability of Zn metal anodes, however, the effectiveness of this strategy is significantly limited by individual additives. Inspired by the high-entropy (HE) concept, we developed a multicomponent (MC) EDL structure composed of La3+, Cl-, and BBI anions by adding dibenzenesulfonimide (BBI) and LaCl3 additives into ZnSO4 electrolytes (BBI/LaCl3/ZnSO4). Specifically, La3+ ions accumulate within EDL to shield the net charges on the Zn surface, allowing more BBI anions and Cl- ions to enter this region. Consequently, this unique MC EDL enables Zn anodes to simultaneously achieve uniform electric field, robust SEI layer, and balanced reaction kinetics. Moreover, the synergistic parameter - a novel descriptor for quantifying collaborative improvement - was first proposed to demonstrates the synergistic effect between BBI and LaCl3 additives. Benefitting from these advantages, Zn metal anodes achieved a high reversibility of 99.5 % at a depth of discharge (DoD) of 51.3 %, and Zn|MnO2 pouch cells exhibited a stable cycle life of 100 cycles at a low N/P ratio of 2.9.

Lithiation Induced Hetero-Superlattice Zn/ZnLi as Stable Anode for Aqueous Zinc-Ion Batteries.

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.

3D Porous Fibers with Spatial Traps and Excellent Zn2+ Transport Kinetics Enable Stable Zn-Based Aqueous Battery.

Adverse side reactions and uncontrolled Zn dendrites growth are the dominant factors that have restricted the application of Zn ion batteries. Herein, a 3D self-supporting porous carbon fibers (denoted as PCFs) host is developed with "trap" effect to adjust the Zn deposition. The unique open structural design of N-doped carbon can act as the zincophilic sites to induce uniform deposition and inhibit adverse side reactions. More importantly, the porous hollow PCFs host with "trap" effect can induce Zn deposition in the fiber by adjusting the local electric field and current density, thereby increasing the specific energy density of the battery and inhibiting dendrite growth. In addition, the 3D open frameworks can regulate Zn2+ flux to enable outstanding cycling performance at ultra-high current densities. As expected, the PCFs framework guarantees the uniform Zn plating and stripping with an outstanding stability over 6000 cycles at the current density of 40 mA cm-2. And the Zn@PCFs||MnO2 full battery shows an excellent lifespan over 1300 cycles at 2000 mA g-1.

Hybrid Molecular Sieve-Based Interfacial Layer with Physical Confinement and Desolvation Effect for Dendrite-free Zinc Metal Anodes.

The side reactions and dendrite growth at the interface of Zn anodes greatly limit their practical applications in Zn metal batteries. Herein, we propose a hybrid molecular sieve-based interfacial layer (denoted as Z7M3) with a hierarchical porous structure for Zn metal anodes, which contains 70 vol % microporous ZSM-5 molecular sieves and 30 vol % mesoporous MCM-41 molecular sieves. Through comprehensive molecular dynamics simulations, we demonstrate that the mesopores (∼2.5 nm) of MCM-41 can limit the disordered diffusion of free water molecules and increase the wettability of the interfacial layer toward aqueous electrolytes. In addition, the micropores (∼0.56 nm) of ZSM-5 can optimize the Zn2+ solvation structures by reducing the bonded water molecules, which simultaneously decrease the constraint force of solvated water molecules to Zn2+ ions, thus promoting the penetrability and diffusion kinetics of Zn2+ ions in Z7M3. The synergetic effects from the hybrid molecular sieves maintain a constant Zn2+ concentration on the surface of the Zn electrode during Zn deposition, contributing to dendrite-free Zn anodes. Consequently, Z7M3-coated Zn electrodes achieved excellent cycling stability in both half and full cells.

A Protective Layer of UIO-66/Reduced Graphene Oxide to Stabilize Zinc-Metal Anodes toward High-Performance Aqueous Zinc-Ion Batteries.

Rechargeable aqueous Zn-ion batteries with a Zn anode hold great promise as promising candidates for advanced energy storage systems. The construction of protective layer coatings on Zn anode is an effective way to suppress the growth of Zn dendrites and water-induced side reactions. Herein, we reported a series of UIO-66 materials with different concentrations of reduced graphene oxide (rG) coated onto the surface of Zn foil (Zn@UIO-66/rGx; x = 0.05, 0.1, and 0.2). Benefiting from the synergistic effect of UIO-66 and rG, symmetric cells with Zn@UIO-66/rGx (x = 0.1) electrodes exhibit excellent reversibility (e.g., long cycling life over 1100 h at 1 mA cm-2/1 mAh cm-2) and superior rate capability (e.g., over 1100 and 400 h at 5 mA cm-2/2.5 mAh cm-2 and 10 mA cm-2/5 mAh cm-2, respectively). When the Zn@UIO-66/rG0.1 anode was paired with the NaV3O8·1.5H2O (NVO) cathode, the Zn@UIO-66/rG0.1||NVO cell also delivered a high reversible capacity of 189.9 mAh g-1 with an initial capacity retention of 61.3% after 500 cycles at 1 A g-1, compared to the bare Zn||NVO cell with only 92 cycles.

Organic Cations Texture Zinc Metal Anodes for Deep Cycling Aqueous Zinc Batteries.

Manipulating the crystallographic orientation of zinc (Zn) metal to expose more (002) planes is promising to stabilize Zn anodes in aqueous electrolytes. However, there remain challenges involving the non-epitaxial electrodeposition of highly (002) textured Zn metal and the maintenance of (002) texture under deep cycling conditions. Herein, a novel organic imidazolium cations-assisted non-epitaxial electrodeposition strategy to texture electrodeposited Zn metals is developed. Taking the 1-butyl-3-methylimidazolium cation (Bmim+) as a paradigm additive, the as-prepared Zn film ((002)-Zn) manifests a compact structure and a highly (002) texture without containing (100) signal. Mechanistic studies reveal that Bmim+ featuring oriented adsorption on the Zn-(002) plane can reduce the growth rate of (002) plane to render the final exposure of (002) texture, and homogenize Zn nucleation and suppress H2 evolution to enable the compact electrodeposition. In addition, the formulated Bmim+-containing ZnSO4 electrolyte effectively sustains the (002) texture even under deep cycling conditions. Consequently, the combination of (002) texture and Bmim+-containing electrolyte endows the (002)-Zn electrode with superior cycling stability over 350 h under 20 mAh cm-2 with 72.6% depth-of-discharge, and assures the stable operation of full Zn batteries with both coin-type and pouch-type configurations, significantly outperforming the (002)-Zn and commercial Zn-based batteries in Bmim+-free electrolytes.

Bi-Functional Electrolyte Additive Leading to a Highly Reversible and Stable Zinc Anode.

A stable stripping/plating process of the zinc anode is extremely critical for the practical application of aqueous zinc metal batteries. However, obstacles, including parasitic reactions and dendrite growth, notoriously deteriorate the stability and reversibility of zinc anode. Herein, Methyl l-α-aspartyl-l-phenylalaninate (Aspartame) is proposed as an effective additive in the ZnSO4 system to realize high stability and reversibility. Aspartame molecule with rich polar functional groups successfully participates in the solvation sheath of Zn2+ to suppress water-induced side reactions. The self-driven adsorption of Aspartame on zinc anode improves uniform deposition with a dose of 10 mm. These synergetic functions endow the zinc anode with a significantly long cycling lifespan of 4500 h. The cell coupled with a vanadium-based cathode also exhibited a high-capacity retention of 71.8% after 1000 cycles, outperforming the additive-free counterparts.