Ultralong Cycle Research Articles

I3--Mediated Oxygen Evolution Activities to Boost Rechargeable Zinc-Air Battery Performance with Low Charging Voltage and Long Cycling Life.

An effective strategy to facilitate oxygen redox chemistry in metal-air batteries is to introduce a redox mediator into the liquid electrolyte. The rational utilization of redox mediators to accelerate the charging kinetics while ensuring the long lifetime of alkaline Zn-air batteries is challenging. Here, we apply commercial acetylene black catalysts to achieve an I3--mediated Zn-air battery by using ZnI2 additives that provide I3- to accelerate the cathodic redox chemistry and regulate the uniform deposition of Zn2+ on the anode. The Zn-air battery performs an ultra-long cycle life of over 600 h at 5 mA cm-2 with a final charge voltage of 1.87 V. We demonstrate that I- mainly generates I3- on the surface of carbon catalysts during the electrochemically charging process, which can further chemically react with OH- to generate oxygen and further revert to I-, thus obtaining a stable electrochemical system. This work offers a strategy to simultaneously improve the cycling life and reduce the charging voltage of Zn-air batteries through redox mediator methods.

Regulating the space charge at interface by negative polar biomolecule enabling ultrastable Zn anode chemistry

The irreversibility of Zn metal anode arising from uncontrollable dendrite growth and hydrogen evolution reaction, especially at high current densities, has challenged the commercialization application of aqueous Zn-ion batteries. Here we report biomolecule additive, named xanthan gum, to solve these issues through making use of dissociated electronegative groups to reduce space charge near the anode-electrolyte interface, tuning solvation structure and form H2O-poor electrical double layer to regulate the Zn deposition behaviors. Meanwhile, the dissolved xanthan gum with multiple polar groups can break the association between H2O and Zn2+ to reconstruct solvated structures of Zn ions to suppress hydrogen evolution reaction (HER). Therefore, the Zn//Zn symmetric cells in ZnSO4 electrolyte with xanthan gum deliver an ultra-long cycle life (>4700 h), and also present excellent cycling performances in other electrolytes (Zn(OAc)2 and Zn(OTf)2). More importantly, a high coulombic efficiency of 99.7 % is achieved using Zn//Cu half cells tested and excellent cycling life for KVO//Zn full cells. This work provides a guidance to design the electrolyte additive for highly reversible Zn metal batteries.

A Flexible Asymmetric Supercapacitor with High-Performance and Long-Lifetime: Fabrication of Nanoworm-Like-Structured Electrodes Based on Polypyrrole-Thiosemicarbazone Complex.

A thiosemicarbazone-based iron(III) complex is prepared and used in the preparation of a supercapacitor electrode material. This electrode is produced by a solvothermal reaction of polypyrrole and the complex on carbon felt. The characterization of the complex and material is carried out using UV-vis, elemental analysis, FT-IR, XRD, BET, and TGA methods, and the surface morphology is examined using SEM technique. Because the interaction of electrode and electrolyte is of great importance in energy storage systems, as the surface area and pore volume increase, electrode ions at the electrode/electrolyte interface leak to the inner surfaces and interact with the larger surface area, which increases the charge storage performance. The electrode material, nano-worm structure, reached the highest specific capacitance value of 764.6 F g-1 at 5 mV s-1. Compared to the capacitance value of polypyrrole in its pure form, it is observed to exhibit an 187.2% increase. The highest specific capacitance value of the asymmetric supercapacitor (ASC) formed with a graphite electrode is 318.1 F g-1 at the current density of 1 Ag-1. Moreover, ASC reached a wide working potential of 1.8 V in an aqueous electrolyte and exhibited ultra-long cycle life (112%), maintaining its stability after 10000 cycles.

Dual zinco-phobic/-philic ferroelectric nanorods coated mesh for stable Zn anode

Aqueous Zn-ion batteries are emerging as a promising option for energy storage systems due to their safety and environmental benefits. However, their stability and reversibility are often hindered by dendrite growth and interfacial side reactions. In this study, we introduce an innovative strategy to address these issues by engineering an artificial interfacial layer (AIL) on Zn anode surface. This AIL is composed of a dual zinco-phobic/-philic ferroelectric nanorods (FE NRs) mesh, which contrasts with the traditional BaTiO3 nanoparticles. The BTO NRs, particularly those with exposed P4/mmm (100) and (211) facets enriched with oxygen vacancy, facilitate a partial phase transition from the FE tetragonal P4mm phase to the paraelectric tetragonal P4/mmm phase, thereby creating dual zinco-phobic/-philic sites. Additionally, the integration of microchannels within the FE BTO NRs mesh can efficiently modulate the electric field distribution and Zn2+ concentration, leading to a more uniform Zn deposition, as conformed by electrochemical simulations. The Zn anode coated with the FE BTO NRs mesh exhibits impressive performance, achieving an ultralong cycle life of 3050 h at 1 mA cm−2 and 1mAh cm−2. It sustains a Coulombic efficiency exceeding 99.8 % over 2000 cycles, highlighting its exceptional reversibility. These findings underscore the potential of the dual zinco-phobic/-philic FE NRs mesh in overcoming the challenges faced in aqueous metal-ion batteries, showcasing its versatility and the significant performance enhancements it can offer.

Decrypting Synergy of Alloy & Metal Nanoparticles Within Nitrogen-Doped Carbon Nanosheets for Zn-Air Batteries with Ultralong Cycling Stability.

The exploration of efficient, robust, and low-cost bifunctional electrocatalysts to drive the commercial application of Zn-air batteries (ZABs) is of great significance but still remains a challenge. Herein, a 1D coordination polymer (1D-CP) derived FeNi alloy & Co nanoparticles (NPs) co-implanted N-doped carbon nanosheets (FNC/NCS) is judiciously crafted and employed as a high-performance electrocatalyst for ultralong lifetime ZABs. The key to this strategy is the leveraging of metal-coordinated melamine to direct the pyrolysis of 1D-CP, enabling the in situ formation of well-dispersed FeNi alloy and Co NPs within the carbon matrix. The resulting FNC/NCS exhibits prominent oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity with a small overall oxygen potential difference (ΔE = 0.68V). Density functional theory (DFT) simulation demonstrates that the synergistic effect between FeNi alloy and Co NPs can reduce energy barriers, promote electron transfer, and optimize the formation of crucial intermediates, thereby largely boost ORR/OER activity of FNC/NCS. The FNC/NCS-assembled ZABs possess high specific capacity, large power density, and ultralong cycling life in both aqueous (> 3300h) and solid-state (150h) electrolytes. This work provides a viable strategy for 1D-CP-derived bifunctional electrocatalysts and dissects the synergistic effect between different metal species, affording significant guidance for the development of renewable energy materials.

A Fast and Highly Stable Aqueous Calcium-Ion Battery for Sustainable Energy Storage.

Aqueous alkali-ion batteries are gaining traction as a low-cost, sustainable alternative to conventional organic lithium-ion batteries. However, the rapid degradation of commonly used electrode materials, such as Prussian Blue Analogs and carbonyl-based organic compounds, continues to challenge the economic viability of these devices. While stability issues can be addressed by employing highly concentrated water-in-salt electrolytes, this approach often requires expensive and, in many cases, fluorinated salts. Here, we show that replacing monovalent K+ ions with divalent Ca2+ ions in the electrolyte significantly enhances the stability of both a copper hexacyanoferrate cathode and a polyimide anode. These findings have direct implications for developing an optimized aqueous Ca-ion battery that demonstrates exceptional fast-charging capabilities and ultra-long cycle life and points toward applying Ca-based batteries for large-scale energy storage.

Partial‐Oxidation Enabling Homologous Ru/RuO2 Heterostructures With Proper d‐Dand Center as Efficient and Durable Cathode Catalysts for Ultralong Cycle Life in Li–O2 Batteries

AbstractThe sluggish cycle kinetics is one of the major obstacles to the commercial application of Li–O2 batteries (LOBs), despite their large theoretical energy density. Efficient and long‐term durable cathode catalysts are urgently desired to strengthen their cycle stability and rate performance. Density functional theory calculations reveal that Ru/RuO2 Mott–Schottky heterostructures can manipulate the adsorption capacities of intermediates by modulating the d‐band center and redistribute interfacial charges, enabling efficient redox kinetics, reducing overpotentials, and optimizing the growth pathway of discharge products. Herein, a wet impregnation approach followed by partial oxidization of Ru nanodots to construct homologous Ru/RuO2 heterostructures as advanced cathode catalysts for boosting the electrochemical activities of LOBs is employed. They exhibit superior electrochemical performance, including high discharge specific capacity (17 120 mAh g−1 at 200 mA g−1), small overpotential (0.96 V), and ultralong cycle lifetime of 1209 cycles (>2400 h) at 500 mA g−1. Over 1260‐h stable cycle in air atmosphere at 500 mA g−1 demonstrates the potential application prospects of the Ru/RuO2 heterostructures in Li‐air batteries. Multiple ex/in situ measurements and theoretical calculation are conducted to investigate the optimizing mechanism of electrochemical performances.

P-Block-metal bismuth embedded in N/P co-doped carbon nanorods for kinetics-enhanced rechargeable lithium-oxygen batteries

Rechargeable lithium-oxygen batteries (LOBs) are considered one of the most promising electrochemical energy storage devices due to their extremely high theoretical energy density. However, the slow redox kinetics of the oxygen cathode leads to low coulombic efficiency and poor cycling performance, which limits the development of high-performance LOBs. Herein, Bi@NPC heterostructure nanorods are designed with the assistance of p-block metal Bi and successfully synthesized as bifunctional cathode catalysts for LOBs. Experimental and theoretical calculations show that Bi@NPC electrode can significantly reduce overpotential during discharge/charge processes due to the easily tunable localized p-orbitals and resulting versatile electronic structures. Benefiting from p-orbital electrons regulation of Bi atoms, the Bi@NPC electrode exhibited superior specific capacity over 11852.6 mAh g−1, outstanding rate capabilities, and ultralong cycle stability over 83 cycles at 200 mA g−1 with the fixed capacity of 500 mAh g−1. This work reveals an efficient pathway to synthesize p-block metal-based catalysts for high-performance LOBs.

Dual Fe/I Single-Atom Electrocatalyst for High-Performance Oxygen Reduction and Wide-Temperature Quasi-Solid-State Zn-Air Batteries.

Oxygen reduction reaction (ORR) electrocatalysts are essential for widespread application of quasi-solid-state Zn-air batteries (ZABs), but the well-known Fe-N-C single-atom catalysts (SACs) suffer from low activity and stability because of unfavorable strong adsorption of oxygenated intermediates. Herein, the study synthesizes dual Fe/I single atoms anchored on N-doped carbon nanorods (Fe/I-N-CR) via a metal-organic framework (MOF)-mediated two-step tandem-pyrolysis method. Atomic-level I doping modulates the electronic structure of Fe-Nx centers via the long-range electron delocalization effect. Benefitting from the synergistic effect of dual Fe/I single-atom sites and the structural merits of 1D nanorods, the Fe/I-N-CR catalyst shows excellent ORR activity and stability, superior to Pt/C and Fe or I SACs. When the Fe/I-N-CR is employed as cathode for quasi-solid-state ZABs, a high power density of 197.9mW cm-2 and an ultralong cycling lifespan of 280h at 20mA cm-2 are both achieved, greatly exceeding those of commercial Pt/C+IrO2 (119.1mW cm-2 and 47h). In addition, wide-temperature adaptability and superior stability from -40 to 60 °C are realized for the Fe/I-N-CR-based quasi-solid-state ZABs. This work provides a MOF-mediated two-step tandem-pyrolysis strategy to engineer high-performance dual SACs with metal/nonmetal centers for ORR and sustainable ZABs.

Inhomogeneous Coordination in High-entropy O3-type Cathodes Enables Suppressed Slab Gliding and Durable Sodium Storage.

O3-type layered oxides are highly promising cathodes for sodium-ion batteries (SIBs), however they undergo complex phase transitions and exhibit high sensibility to air, leading to subpar cycling performance and commercial viability. In this work, we report a layered cathode material (NaNi0.29Cu0.1Mg0.05Li0.05Mn0.2Ti0.2Sn0.11O2) with a sate-of-the-art high-entropy compositional design. We unveil that such a configuration featuring inhomogeneous coordination environment of transition metal (TM) elements, can enable enhanced gliding energy (-0.38 vs -0.58 eV) of TMO2 slabs upon desodiation both theoretically and experimentally, which underlies the fundamental origin of the outstanding structural stability of HEO materials. As a consequence, the complex phase transitions (O3-O'3-P3-P'3-P3'-O3') of conventional O3-type cathode have been eliminated, and the as-obtained material demonstrates exceptional structural robustness and integrity with an ultra-long cycle life in a quasi-solid-state cell (maintaining 73.2% capacity after 1000 cycles at 2 C). Moreover, the material presents satisfactory air stability, with minimal structural and electrochemical degradation when directly exposed to the air. An Ah-scale pouch cell based on the cathode material is constructed, demonstrating a capacity retention of 83.6% after 500 cycles, signaling substantial promise for commercial applications.

Demonstration of MAX phases as triple functional artificial solid electrolyte interphase for ultralong life lithium metal anodes

Solid electrolyte interphase (SEI) has significant role in controlling lithium (Li) dendrites. However, lack of chemical stability, mechanical strength and self-perfection for conventional SEI cannot persistently suppress Li dendrites, leading to inferior cycling life. Herein, MAX phases (Ti2SnC and Ti2SC) as triple functional artificial SEI (ASEI) with high modulus, chemical stability and self-smoothing ability are introduced on Li foils (Ti2SnC@Li and Ti2SC@Li) for ultralong life Li metal anodes (LMAs). The high mechanical strength with lithiophilicity of the MAX can induce uniform Li deposition and suppress dendrite growth, while the excellent chemical stability and self-smoothing ability of the MAX guarantee the consistency of the ASEI, achieving ultralong life of the LMAs. As a result, the Ti2SnC@Li||Li@Ti2SnC half-cells demonstrate ultralong cycling performance of 5000 h at 5 mAh cm−2 and 5 mA cm−2. The Ti2SnC@Li||LiFePO4(LFP) full-cells demonstrate ultralong stability up to 3000 cycles at 5C. At harsh conditions including 24.3 mg cm−2 of LFP, 6.0 g (Ah)−1 of electrolyte and 2.6 of negative/positive ratio, the Ti2SnC@Li||LFP full-cells maintain 2.9 mAh cm−2 after 130 cycles at 0.3C. This work demonstrates the MAX phases with high modulus, chemical stability and self-smoothing ability as triple functional ASEI for metal anode protection.

Laser-Induced Solid-Phase Strategy to Synthesize Single-Atomic Lithiophilic Sites Enabled Dendrite-Free Lithium Deposition on Graphene Matrix.

The introduction of metal Single-atom (SA) to construct lithium-philic active sites shows the ability to guide uniform lithium deposition and improve the stability of lithium hosts. Nevertheless, the development of facile and expedient methods for synthesizing SA remains a considerable challenge. Herein, The SA metal loaded on graphene (Bi@LrGO) is designed by laser-induced solid-phase strategy. The bismuth salts simultaneously decompose under the high local temperature and in the reductive atmosphere induced by laser to form SA metal. Simultaneously, graphene oxide (GO) nanosheets absorb photon energy to be reduced/graphitized into graphene, which serves as anchoring sites for Bismuth Sing-atom (Bi SA) immobilization. The SA metals, supported on the graphene not only provide sufficient lithiophilic sites but also significantly increase the adsorption energy (-2.11eV) with lithium atoms, promote the uniform nucleation and deposition of lithium, and inhibit the growth of lithium dendrites. Additionally, the layered structure of the graphene film adapts to the volume change during the repeated lithium plating/stripping process. Therefore, the symmetrical battery-based Li deposited on Bi@LrGO (Bi@LrGO@Li) achieves an ultra-long stable cycle life of ≈2400h at 1mAcm-2. In particular, a full cell with LiFePO4 cathode provides a good capacity retention of 81.2% at 4C after 600 cycles.

Disodium Malate Electrolyte Additive Facilitates Dendrite-Free Zinc Anode: Deposition Kinetics and Interface Regulation.

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 2m 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 10mA cm-2 and 5 mAh cm-2. The Zn||VO2 full cells with DM additive exhibits an ultralong cycling lifespan without capacity loss.

Deposition and etching of (101)Zn facet exposed zinc electrode induced by trace COS achieving ultra-long cycle stability in zinc batteries

Rechargeable aqueous zinc-based batteries (RZBs) often suffer from poor cycling stability due to the instability of zinc deposition and etching processes. This work achieves dendrite-free zinc deposition with a smaller nucleation radius and rapid completion of the nucleation stage by a “triple regulation strategy” with trace chitosan oligosaccharide (COS) in ZnSO4 electrolyte (2 g L−1 COS). Theoretical and experimental results indicate that COS, with hydroxyl and amino functional groups, exhibits a high affinity for the (002)Zn and (100)Zn facets. Under the influence of a small amount of COS, the selective exposure of the (101)Zn facet is facilitated. The extensively exposed (101)Zn facet is protected by COS, which inhibits the occurrence of side reactions. Moreover, the presence of trace COS-02 changes the etching mode from three-dimensional (3D) to two-dimensional (2D), ensuring a uniform distribution of Zn2+ in the electric field during the deposition process. The unique 3D deposition and 2D etching mechanism induced by the COS additive result in exceptional cycling stability, exceeding 3800 h (1 mA cm−2) and 430 h (5 mA cm−2) in zinc symmetrical cells. Additionally, COS acts as a “molecular pillar” to stabilize VS2, enabling the Zn||VS2 full cell to achieve 1000 stable cycles with 89.6% capacity retention and an average coulombic efficiency of 99.95%. This work reveals a novel multiple regulation mechanism by using trace COS in RZBs, and provides a new approach for the development of long-term stable RZBs with preferential exposure facets.

A novel naphthalenediimide-based metal-organic framework for inkless erasable printing with ultra-long cycling performance

A novel naphthalenediimide-based metal-organic framework for inkless erasable printing with ultra-long cycling performance

Hollow carbon nanofibers with self-induced internal electric field for high-performance full-carbon sodium ion capacitors

Self-induced internal electric field (SIEF) is crucial to achieve high capacity, high rate and long cycle life of carbon anodes in Na+ storage, but it is also a huge challenge currently. Herein, a template-assisted electrospinning process and subsequent low-temperature pyrolysis method is employed to synthesize S, N co-doped hollow carbon nanofibers (SNHCF) with rich micropores and chemisorption sites. The rich micropores and interconnected macroporous in SNHCF provide large internal availability that effectively exposing the active sites, inhibiting the volume expansion and shortening the Na+ diffusion distance. Besides, S, N co-doping in the carbon skeleton can act as an electron acceptor and electron donor respectively to form a SIEF to boost adsorption of Na+. Theoretical calculation and ex-situ characterizations confirmed that S, N co-doping can regulate the electronic configuration and reduce the diffusion barrier of Na+. As a result, SNHCF anode has ultra-high specific capacity (588.2mAh g−1 at 0.05 A/g) and impressive rate performance (264.3mAh g−1 at 20 A/g). The full-carbon sodium ion capacitors assembled with SNHCF anode and activated carbon cathode exhibits high energy density (119 Wh kg−1) and ultra-long cycle stability (80.06 % capacity retention after 12,000 cycles).

N/O-functionalized ultrathin carbon nanosheets for zinc-ion hybrid capacitors

2D carbon materials have outstanding electrical properties and rich anchoring sites, and can be used as zinc ion storage electrodes. However, it remains a formidable challenge to fabricate these materials with tunable composition by a simple synthesis strategy. Herein, folic acid-derived N/O-functionalized ultrathin carbon nanosheets are synthesized via the activation effect of nano-ZnO template. The as-fabricated FACN-800 exhibits extremely thin thickness (∼1.6 nm), hierarchically porous structure and rich N/O heteroatoms (14.9 at.% of N and 8.4 at.% of O), which is conducive to accelerate ion transport and provide additional active sites for Zn-ion storage. Thus, the optimized FACN-800 based aqueous zinc-ion hybrid capacitor delivers excellent zinc-ion storage capabilities with high specific capacity (163.6 mAh g−1 at 0.1 A g−1), admirable energy density (130.8 Wh kg−1) and ultralong cycle stability (90.3 % capacity retention over 40,000 cycles) and FACN-800 has a specific surface area of 554.3 m2 g−1. Moreover, a series of ex-situ measurements and DFT theoretical calculations further elucidate the electrochemical mechanism between zinc ion storage and N/O dopants.

Structural modulation of Na4Fe3(PO4)2P2O7 via cation engineering towards high-rate and long-cycling sodium-ion batteries

Mixed iron-based phosphate Na4Fe3(PO4)2P2O7/C (NFPP) has gradually emerged as a promising cathode material for sodium-ion batteries (SIBs) owing to its affordability and convenient preparation. However, poor electrical conductivity and inadequate sodium-ion diffusion limit the exertion of its electrochemical properties. Herein, a structural modulation strategy based on Cd doping is applied to NFPP to address the above limitations. In situ X-ray diffraction analysis reveals that Cd-doped NFPP (NFCPP) undergoes an incomplete solid-solution reaction driven by Fe2+/Fe3+ redox. Cd doping effectively stabilises the crystal structure, resulting in a minimal 1 % change in unit cell volume during cycling. Density of state calculations indicate that Cd doping reduces the band gap, increases the local electron density and significantly improves electron conductivity. Benefitting from the enhanced electrochemical kinetics and intercalation pseudocapacitance, the optimised Na4Fe2.91Cd0.09(PO4)2P2O7/C (NFCPP@3%) exhibits exceptional rate performance (capacity of 62 mAh/g at 20 C) and ultra-long cycling life (82.7 % after 6000 cycles at 20 C). A full SIB prepared using NFCPP@3% and hard carbon, display a 91 % capacity retention rate at a current density of 130 mA g−1 over 200 cycles. This work demonstrates that doping can effectively enhance electrochemical performance and offers insights into future development of SIBs.

Synergistic Regulation of Anode and Cathode Interphases via an Alum Electrolyte Additive for High-Performance Aqueous Zinc-Vanadium Batteries.

A zinc (Zn) metal anode paired with a vanadium oxide (VOx) cathode is a promising system for aqueous Zn-ion batteries (AZIBs); however, side reactions proliferating on the Zn anode surface and the infinite dissolution of the VOx cathode destabilise the battery system. Here, we introduce a multi-functional additive into the ZnSO4 (ZS) electrolyte, KAl(SO4)2 (KASO), to synchronise the in situ construction of the protective layer on the surface of the Zn anode and the VOx cathode. Theoretical calculations and synchrotron radiation have verified that the high-valence Al3+ plays dual roles of competing with Zn2+ for solvation and forming a Zn-Al alloy layer with a homogeneous electric field on the anode surface to mitigate the side reactions and dendrite generation. The Al-containing cathode-electrolyte interface (CEI) considerably alleviates the irreversible dissolution of the VOx cathode and the accumulation of byproducts. Consequently, the Zn||Zn cell with KASO exhibits an ultra-long cycle of 6000 h at 2 mA cm-2. Importantly, the VOx cathodes (VO2, V2O5 and NH4V4O10) in the ZS-KASO electrolyte showed excellent cycling stability, including Zn powder||VO2 cells and Zn||VO2 pouch cells. Even better, the full cell exhibits excellent cycling stability at low negative/positive (N/P) ratio of 2.83 and high mass loading (~16 mg cm-2). This study offers a straightforward and practical reference for concurrently addressing challenges at the anode and cathode of AZIBs.

Electrolyte Additive l-Lysine Stabilizes the Zinc Electrode in Aqueous Zinc Batteries for Long Cycling Performance.

Rechargeable aqueous Zn-ion batteries (AZIBs) have been recognized as competitive devices for large-scale energy storage due to their characteristics of low cost, safe operation, and environmental friendliness. Nevertheless, their practical applications are greatly limited by zinc dendrite growth and side reactions occurring at the anode/electrolyte interface. Herein, we propose an effective and simple electrolyte engineering strategy, which is the introduction of l-lysine additive containing two amino groups and one carboxyl group into a ZnSO4 electrolyte to achieve stable and reversible Zn depositions. Theoretical calculations and experimental results reveal that the l-lysine can adsorb on the Zn anode surface due to the strong coordination effects between amino groups and Zn metal (Zn-N binding) and induce the reduction of ZnSO4 into inorganic ZnS, which can not only prevent interfacial side reactions but also regulate interfacial electric field on the zinc electrode surface to guide uniform Zn2+ electrodeposition to inhibit zinc dendrites. Consequently, the l-lysine additive in the electrolyte enables Zn||Zn symmetric cells to achieve an ultralong stable cycling up to 2400 h at 1 mA cm-2 with a low polarization of only about 16 mV and Zn||Cu asymmetric cells to obtain a high average Coulombic efficiency of 99.80% after stably cycling for more than 2000 h at 2 mA cm-2 (1 mAh cm-2). In addition, the Zn||MnO2@CNT full cell in an l-lysine-containing electrolyte also exhibits good cycling performance. This study offers a new perspective on multifunctional electrolyte additive for achieving highly reversible Zn metal anodes in AZIBs.