Large-scale Energy Storage Research Articles

Minimizing Zn Loss Through Dual Regulation for Reversible Zinc Anode Beyond 90% Utilization Ratio.

Large-scale energy storage devices experience explosive development in response to the increasing energy crisis. Zinc ion batteries featuring low cost, high safe, and environment friendly are considered promising candidates for next-generation energy storage devices. However, their practical application suffers from the limited anode lifespan under a high zinc utilization ratio, which can be attributed to aggravated Zn loss caused by zinc conversion reactions and "dead" Zn. Herein, n-propyl alcohol is reported to stabilize the Zn anode under the high depth of discharge through dual regulation of water activity inhibition and zinc-ion plating regulation. The modified electrolyte exhibits a 76.43% cut in corrosion current benefited from low water activity and benefits SEI surface. The "dead" Zn content is also reduced by 26 times as a result of dendrite-free zinc ion plating. Thus, the highly reversible zinc plating/stripping with 99.62% CE is achieved for ≈3600 cycles. Moreover, the lifespan of Zn/Zn cells is greatly increased even under a high depth of discharge (310 h, 90%DOD and 120 h, 95.18% DOD). In Zn/NH4V4O10 full cells, the improved anode reversibility enables a remarkable capacity retention of 92.16% after 400 cycles with a low N/P ratio of 2.5.

New Non‐Invasive Method to Monitor and Reverse Faradaic Imbalance in Redox Flow Batteries

Aqueous Organic Redox Flow Batteries (AORFBs) have received much attention due to the accessibility of their active materials. However, among the key performance indicators that require improvement for AORFBs to become competitive against mature technologies, lifespan is especially critical for stationary energy storage. Faradaic imbalance driven by the occurrence of irreversible electrochemical processes decreases lifespan, so monitoring and correction of this parameter is required to prolong lifespan. This work presents a novel, simple and non‐invasive automatized method to monitor the Faradaic imbalance. This method is based on detecting the variation of the minimum derivative of the cell voltage upon cycling, and it is used as the activation criterion for a rebalancing device. The system is tested using an alkaline flow battery consisting of ferrocyanide and 2,6‐dihydroxyanthraquinone (2,6‐DHAQ), extending the cycle life of the battery to 400 cycles (235 h) without any capacity decay and without Ar‐filled glovebox. This demonstrates the feasibility of the proposed system to monitor the state‐of‐health (SOH) due to Faradaic imbalance and recover the capacity loss.

Elucidating the Origins of High Capacity in Iron-Based Conversion Materials: Benefit of Complementary Advanced Characterization toward Mechanistic Understanding.

ConspectusLithium-ion batteries are recognized as an important electrochemical energy storage technology due to their superior volumetric and gravimetric energy densities. Graphite is widely used as the negative electrode, and its adoption enabled much of the modern portable electronics technology landscape. However, developing markets, such as electric vehicles and grid-scale storage, have increased demands, including higher energy content and a diverse materials supply chain. Alternatives that provide the opportunity to increase capacity and address supply chain concerns are of interest.Understanding the fundamental mechanisms that govern battery function is crucial to driving further improvements in the field. Advanced characterization techniques, such as those enabled by synchrotron light sources and high-resolution electron microscopes, that can uncover these mechanisms have become a necessity for elucidating structural evolution upon electrochemical conversion at the nano- to mesoscales. Performing these experiments with relevant electrochemistry using in situ and operando experiments imparts the ability to identify critical reaction pathways and capture intermediate (dis)charge products not discernible by traditional experiments.This Account describes a series of recent studies focused on the advanced characterization of spinel-type iron oxide-based anode materials. These studies begin with magnetite (Fe3O4), a low cost iron oxide which, when synthesized with appropriate coprecipitation based crystallite size control, provides opportunity to realize eight electrons per formula unit via electrochemical reduction. We then transition to bi- and trimetallic ferrites (such as ZnFe2O4 and CoMnFeO4) and conclude with high-entropy spinel ferrite oxides (HEOs) that contain at least 5 transition metals. For each material type, a variety of characterization techniques are utilized to describe the fundamental reaction mechanisms and rationalize electrochemical behavior. X-ray absorption spectroscopy (XAS) is featured prominently, as it allows for element specific analysis of electronic structure and local atomic environments, including nanocrystalline products of electrochemical conversion. Combining XAS-based techniques with diffraction and microscopy, the transition of iron oxide-type electrodes from spinel to rock-salt to metal nanoparticles upon full lithiation can be deciphered. For magnetite and its bi- and trimetallic ferrite analogues, delithiation results in return to a highly disordered network of FeO-like domains. Notably, while magnetite and the bi- and trimetallic ferrites appear to be limited to reoxidation of Fe to the 2+ state, through introduction of entropy-induced structural stability, higher Fe oxidation states (up to 2.6+) can be accessed upon electrochemical oxidation. These materials may hold promise as alternatives to traditional graphite electrodes where their combination of high capacity and compositional flexibility provides an avenue toward low-cost, sustainable energy storage.

Review of Layered Transition Metal Oxide Materials for Cathodes in Sodium-Ion Batteries

The growing interest in sodium-ion batteries (SIBs) is driven by scarcity and the rising costs of lithium, coupled with the urgent need for scalable and sustainable energy storage solutions. Among various cathode materials, layered transition metal oxides have emerged as promising candidates due to their structural similarity to lithium-ion battery (LIB) counterparts and their potential to deliver high energy density at reduced costs. However, significant challenges remain, including limited capacity at high charge/discharge rates and structural instability during extended cycling. Addressing these issues is critical for advancing SIB technology toward industrial applications, particularly for large-scale energy storage systems. This review provides a comprehensive analysis of layered sodium transition metal oxides, focusing on their structural properties, electrochemical performance, and degradation mechanisms. Special attention is given to the intrinsic and extrinsic factors contributing to their instability, such as structural phase transitions, and cationic/anionic redox behavior. Additionally, recent advancements in material design strategies, including doping, surface modifications, and composite formation, are discussed to highlight the progress toward enhancing the stability and performance of these materials. This work aims to bridge the knowledge gaps and inspire further innovations in the development of high-performance cathodes for sodium-ion batteries.

High Capacity and Ultralong Lifespan Aqueous Lithium-Bromine Batteries Realized by Low-Cost Concentrated Electrolyte Coupled with Dependable Lithium Titanium Phosphate.

Aqueous halogen batteries are gaining recognition for large-scale energy storage due to their high energy density, safety, environmental sustainability, and cost-effectiveness. However, the limited electrochemical stability window of aqueous electrolytes and the absence of desirable carbonaceous hosts that facilitate halogen redox reactions have hindered the advancement of halogen batteries. Here, a low-cost, high-concentration 26 m Li-B5-C15-O6 aqueous solution incorporating lithium bromide (LiBr), lithium chloride (LiCl), and lithium acetate (LiOAc) was developed for aqueous batteries, which demonstrated an expanded electrochemical stability window of ca. 2.5 V. In addition, the electrochemical performance of the electrolyte in various carbonaceous hosts (graphene, activated carbon, and nitrogen-doped activated carbon (NAc)) was systematically investigated. In-depth analysis using X-ray photoelectron spectroscopy and Raman spectroscopy revealed that the NAc host promoted the redox kinetics of active bromine species and improved the delivery capacity of the battery. Results revealed that the electrolyte in the NAc host achieved a discharge specific capacity exceeding 376 mA h g-1 while maintaining a capacity retention rate of up to 97% after 7800 cycles. When paired with hierarchically porous LTP@C/CNTs anode material, a LTP@C/CNTs-NAc full cell was constructed, which delivered a discharge specific capacity of 238.4 mA h g-1 and an average output voltage of 1.24 V. Moreover, it demonstrated a reversible specific capacity of 158.2 mA h g-1 with near-complete Coulombic efficiency over more than 10,000 cycles.

Regulation of Zinc Hydroxide Sulfate Growth Environment for Stable Zinc Anode/Electrolyte Interfaces.

Metallic Zn is a promising anode for high-safety, low-cost, and large-scale energy storage systems. However, it is strongly hindered by unstable electrode/electrolyte interface issues, including zinc dendrite, corrosion, passivation, and hydrogen evolution reactions. In this work, an in situ interface protection strategy is established by turning the corrosion/passivation byproducts (zinc hydroxide sulfates, ZHSs) into a stable hybrid protection layer. The hydrolysis of the diglycolamine buffer layer on the zinc anode provides a homogeneous basic electrolyte environment for the generation of small-sized ZHS, thereby leading to the formation of a ZHS-based hybrid layer. Benefiting from this hybrid layer, uniform zinc ion flux and high anticorrosion ability can be achieved. As a result, the decorated symmetric cell presents a long cycling lifespan of over 1500 h at a current density of 1 mA cm-2 and an area capacity of 1 mAh cm-2. It also contributes to the appealing cycling and rate performance of Zn|NH4V4O10 full cells. This work provides insight into regulating and reusing interfacial byproducts for high-performance zinc metal batteries.

Uncovering ZnS growth behavior and morphology control for high-performance aqueous Zn-S batteries.

Aqueous Zn-S batteries provide competitive energy density for large-scale energy storage systems. However, the cathode active material exhibits poor electrical conductivity especially at the discharged state of ZnS. Its morphology generated in cells thus directly determines the cathode electrochemical activity. Here, we reveal the ZnS growth behavior and control its morphology by the anion donor number (DN) of zinc salts in electrolytes. The anion DN affects the salt dissociation degree and furthermore sulfide solubility in electrolytes, which finally determines ZnS growth preference on existing nuclei or carbon substrates. As a result, 3D ZnS is realized from the high DN ZnBr2 electrolyte, whereas a 2D passivation film is formed from low DN Zn(TFSI)2. Thanks to the facile electron paths and abundant reaction sites with 3D morphology, the sulfur cathode reaches a high capacity of 1662 mA h g-1 at 0.1 A g-1 and retains 872 mA h g-1 capacity after 400 cycles at 3 A g-1.

Toward Green and Sustainable Zinc-Ion Batteries: The Potential of Natural Solvent-Based Electrolytes.

Zinc-ion batteries (ZIBs) are emerged as a promising alternative for sustainable energy storage, offering advantages such as safety, low cost, and environmental friendliness. However, conventional aqueous electrolytes in ZIBs face significant challenges, including hydrogen evolution reaction (HER) and zinc dendrite formation, compromising their cycling stability and safety. These limitations necessitate innovative electrolyte solutions to enhance ZIB performance while maintaining sustainability. This review explores the potential of natural solvent-based electrolytes derived from renewable and biodegradable resources. Natural deep eutectic solvents (DES), bio-ionic liquids, and biomass-derived organic compounds present unique advantages, including a wider electrochemical stability window, reduced HER activity, and controlled zinc deposition. Examples include DESs based on choline chloride (ChCl), glycerol-based systems, and biomass-derived solvents such as γ-valerolactone (GVL) and aloe vera, demonstrating improved cycling stability and dendrite suppression. Despite their promise, challenges such as high viscosity, cost, and scalability remain critical barriers to commercialization. This review underscores the need for further research to optimize natural solvent formulations, enhance Zn anode compatibility, and integrate these systems into practical applications. By addressing these challenges, natural solvent-based electrolytes can pave the way for safer, high-performance, and environmentally sustainable ZIBs, particularly large-scale energy storage systems.

High-Energy Aqueous Sodium-Ion Batteries Using Water-in-Salt Electrolytes and 3D Structured Electrodes.

Aqueous sodium-ion batteries (SIBs) are gradually being recognized as viable solutions for large-scale energy storage because of their inherent safety as well as low cost. However, despite recent advancements in water-in-salt electrolyte technologies, the challenge of identifying anode materials with sufficient specific capacity persists, complicating the wider adoption of these batteries. This study introduces an innovative and straightforward approach for synthesizing vanadium oxide laser-scribed graphene (VOx-LSG) composites, which function as effective anode materials in aqueous sodium-ion batteries. By combining a rapid laser-scribing technique with precise thermal control, the method not only allows for changing the morphology of the vanadium oxide, but also tuning its oxidation state. This is achieved while embedding these electrochemically active particles within a highly conductive graphene scaffold. When paired with a Prussian blue-based cathode (Na1.88Mn[Fe(CN)6]0.97) in a concentrated NaClO4-based aqueous electrolyte, the battery's charge storage mechanism is found to be largely surface-controlled, leading to exceptional rate performance. The full cell demonstrates specific capacities of 128 mA h/g@0.05 A/g and 65.6 mA h/g@1 A/g, with an energy density of 47.7 W h/kg, outperforming many existing aqueous sodium-ion batteries. This strategy offers a promising path forward for integrating efficient, eco-friendly, and low-cost anode materials into large energy storage devices and systems.

A safe and robust in-situ polymerized cementitious electrolyte coupled with NiCo2S4@CuCo2S4 electrode for superior load-bearing integrated electrochemical capacitor.

Load bearing/energy storage integrated devices (LEIDs) featuring cementitious electrolytes have become ideal for large-scale energy storage. Nevertheless, the progression of LEIDs is still in its nascent phase and considerable endeavors concerning cementitious electrolytes and electrode materials are necessary to further boost the charge storage ability. Here, we propose a facile synchronous reaction method for preparing sodium acrylate (SA)-based in-situ polymerized cementitious electrolyte. The soft polymer network and hard cement matrix are interwoven together. The resulting cementitious electrolyte not only exhibits improved mechanical properties (flexural strength of 14.7MPa and compressive strength of 44.7MPa), but also possesses enhanced ionic conductivity (26.7mScm-1). Moreover, a core-shell NiCo2S4@CuCo2S4/NF heterostructure is synthesized on nickel foam (NF) substrate by hydrothermal assisted electrodeposition techniques, which showcases a remarkable capacitance of 5626.6mFcm-2 at 1mAcm-2. As a proof, with integrated merits of the optimal cementitious electrolyte and NiCo2S4@CuCo2S4/NF electrode, the as-built LEID demonstrates a high energy density of 138.5μWhcm-2 at 0.75mWcm-2 and a cycling durability of 90.7% after 8000 cycles, showing good practicability in lighting light-emitting diodes (LEDs) or driving a thermal hygrometer. Notably, the LEID can endure external forces without distinctly sacrificing electrochemical properties. This work provides insight into developing novel cementitious electrolytes and electrode materials toward superior LEIDs.

Epitaxial Electrodeposition of Zinc on Different Single Crystal Copper Substrates for High Performance Aqueous Batteries.

The aqueous zinc metal battery holds great potential for large-scale energy storage due to its safety, low cost, and high theoretical capacity. However, challenges such as corrosion and dendritic growth necessitate controlled zinc deposition. This study employs epitaxy to achieve large-area, dense, and ultraflat zinc plating on textured copper foil. High-quality copper foils with Cu(100), Cu(110), and Cu(111) facets were prepared and systematically compared. The results show that Cu(111) is the most favorable for zinc deposition, offering the lowest nucleation overpotential, diffusion energy, and interfacial energy with a Coulombic efficiency (CE) of 99.93%. The study sets a record for flat-zinc areal loading at 20 mAh/cm2. These findings provide some clarity on the best-performing copper and zinc crystalline facets, with Cu(111)/Zn(0002) ranking the highest. Using a MnO2-Zn full cell model, the research achieved an exceptional cycle life of over 800 cycles in a cathode-anode-free battery configuration.

Building a Better All-Solid-State Lithium-Ion Battery with Halide Solid-State Electrolyte.

Since the electrochemical potential of lithium metal was systematically elaborated and measured in the early 19th century, lithium-ion batteries with liquid organic electrolyte have been a key energy storage device and successfully commercialized at the end of the 20th century. Although lithium-ion battery technology has progressed enormously in recent years, it still suffers from two core issues, intrinsic safety hazard and low energy density. Within approaches to address the core challenges, the development of all-solid-state lithium-ion batteries (ASSLBs) based on halide solid-state electrolytes (SSEs) has displayed potential for application in stationary energy storage devices and may eventually become an essential component of a future smart grid. In this Review, we categorize and summarize the current research status of halide SSEs based on different halogen anions from the perspective of halogen chemistry, upon which we summarize the different synthetic routes of halide SSEs possessing high room-temperature ionic conductivity, and compare in detail the performance of halide SSEs based on different halogen anions in terms of ionic conductivity, activation energy, electronic conductivity, interfacial contact stability, and electrochemical window and summarize the corresponding optimization strategies for each of the above-mentioned electrochemical indicators. Finally, we provide an outlook on the unresolved challenges and future opportunities of ASSLBs.

Unveiling Aqueous Potassium-Ion Batteries with Prussian Blue Analogue Cathodes.

Aqueous rechargeable potassium-ion batteries have considerable advantages and potentials in the application of large-scale energy storage systems, owing to its high safety, abundant potassium resources, and environmental friendliness. However, the practical applications are fraught with numerous challenges. Identification of suitable cathode materials and potassium storage mechanisms are of great significance. Herein, an aqueous potassium-ion battery comprising Prussian blue analogs cathode (K1.15Fe[Fe(CN)6]·1.36H2O) and perylene-3,4,9,10-tetracarboxylic anode is designed, which delivers a high energy density of 52.0 Wh kg-1 and excellent cycling stability with high capacity retention of 84.5% after 4000 cycles. Importantly, a synergistic study of the relationships among crystal structure, spin state, kinetics, and electrochemical performances is thoroughly conducted. By employing in situ and ex situ characterizations, the potassium storage mechanism is comprehensively elucidated from multiple perspectives.

Anode-Free Zinc-Bromine Batteries Enabled by a Simple Prenucleation Strategy.

The design of anode-free zinc (Zn) batteries with high reversibility at high areal capacity has received significant attention recently, which is quietly challenging yet. Here, a Zn alloyed interface through electroplating is introduced, providing homogeneous Zn prenucleation sites to stabilize subsequent Zn nucleation and plating. By employing Zn-Cu alloy as a module, the complementary simulations and characterizations confirm that the prenucleation alloyed interfaces achieve a homogeneous electric field distribution and greatly enhance the stability of the Zn anode. Accordingly, the Zn//Zn-Cu@Cu half-cells show a long cycle life of over 900h and an average Coulombic efficiency (CE) of 99.8% at an areal capacity of10 mAh cm-2. The assembled anode-free zinc-bromine (Zn-Br2) battery exhibits an attractive stable cycling of 11 000 cycles at 1 mAh cm-2, while over 1000 cycles at the higher areal capacity of 10 mAh cm-2. Excitingly, the Zn-Br2 pouch cell with a capacity of 1000 mAh operates stably over 50 cycles, and achieves successful integration with photovoltaic systems. This anode-free Zn-Br2 batteries constructed through a prenucleation strategy offer new insights into the potential for large-scale energy storage applications.

Recent Advances in Fast-Charging Sodium-Ion Batteries.

Sodium-ion batteries (SIB), stemming from the abundance of sodium resources and their cost-effectiveness, have positioning them favorably a potential candidate for stationary energy storage and public electric vehicles. As an intermediary of the grid system and output terminals of the charging station, fast-charging performance has actually become a crucial metric, which greatly relates to the charging station utilization and cost- and time-efficient. Besides, the fast-charging capacity is also relevant to the long-term stable operation public transportation. Given the remarkable advancements in fast-charging SIBs reported recently, a review about this topic and scope is timely and important at present. In this study, the bottlenecks of fast-charging SIBs are first assessed, after that, a comprehensive overview of the employed strategies for improving the fast-charging capacities of SIBs from three aspects: structures design, reaction mechanism regulation, and optimization of solvation structure and interfacial property is given. Finally, challenges and prospects for further research toward fast-charging SIBs are proposed. The authors hope this review will provide a deep understanding of the design principles of fast-charging SIBs and inspire more endeavors to conquer the practicability issue of SIBs in energy storage fields.

A comparative study on the structural, chemical, morphological and electrochemical properties of α-MnO2, β-MnO2 and δ-MnO2 as cathode materials in aqueous zinc-ion batteries

Aqueous zinc-ion batteries (AZIBs) are considered to be highly promising electrochemical energy storage device due to their affordability, inherent safety, large zinc resources, and optimal specific capacity. Among various cathode materials, manganese dioxide (MnO2) stands out for its high voltage, environmental benignity, and theoretical specific capacity. This study systematically investigates the phase formation and structural parameters of α-MnO2, β-MnO2, and δ-MnO2 synthesized via hydrothermal method, employing Rietveld refinement. FTIR and Raman spectroscopy confirms Mn-O and O-H bond formation. BET analysis reveals surface areas, and pore size distribution is calculated with BJH method. High-resolution XPS spectra exhibit a spin energy split of ~ 11.9 eV for Mn 2p confirming the presence of MnO2. Electrochemical studies shows an initial discharge capacities of 230.5, 188.74 and 263.30 mAh g− 1 at 0.1 A g− 1 for α-MnO2, β-MnO2 and δ-MnO2. The EIS spectra revealed the capacitive behaviour and electrode reaction kinetics where a RcT value of 484.14, 327.6, 162.5 Ω for α-MnO2, β-MnO2 and δ-MnO2. These study give insights into relation of various properties of MnO2 with electrochemical performance and its viability in grid storage applications.Graphical

Manganese Intercalation Enabling High-Performance Aqueous Fe-VO2 Batteries.

The aqueous iron ion batteries (AIIBs) are an attractive option for large-scale energy storage applications. However, the inadequate plating and stripping of Fe2+ ions underscore the need to explore more suitable cathode materials. Herein, we optimize the structure of tunnel-like VO2 nanosheets by introducing Mn2+ ion intercalation as a cathode material to enhance their performance in AIIBs. Mn2+ serves as a stabilizing pillar for VO2, which brings some oxygen vacancies to provide extra electrochemically active sites, and accelerates the reversible (de)insertion of Fe2+ ions. In addition, the density functional theory (DFT) calculations show that the introduction of Mn2+ reduces the band gap of VO2 and also decreases the electrostatic interaction between Fe2+ and VO2. Consequently, the VO2 with interlayer Mn2+ pillars (5% MVO) electrodes exhibit a remarkable capacity of 284.32 mAh g-1 at a current density of 0.1 A g-1 and demonstrate excellent cycle life, maintaining 81.7% of their capacity at 1.0 A g-1 after 600 cycles. Therefore, these results offer a promising choice for the cathode material to achieve outstanding electrochemical performance in AIIBs.

The Defect Structure Evolution in MgH2-EEWNi Composites in Hydrogen Sorption–Desorption Processes

This paper presents the results of the study of the composite based on magnesium hydride with the addition of nanosized nickel powder, obtained by the method of an electric explosion of wires. The obtained MgH2-EEWNi (20 wt.%) composite with the core-shell configuration demonstrated the development of a defect structure, which makes it possible to significantly reduce the hydrogen desorption temperature from 418 °C for pure magnesium hydride to 229 °C for hydride with the addition of nickel powder. In situ studies of the evolution of the defect structure using positron annihilation methods and diffraction methods made it possible to draw conclusions about the influence of the Mg2NiH0.3 and Mg2NiH4 phases on the sorption and desorption properties of the composite. The results obtained in this work can be used in the field of hydrogen energy in mobile or stationary hydrogen storage systems.

Mechanism of solid electrolyte interphase film formation using ethylene carbonate-based local high concentration electrolyte in sodium-ion batteries.

Sodium-ion batteries (SIBs) have the advantages of abundant resources and low cost, making them potential candidates for the next-generation large-scale energy storage technology. However, the capacity fade during cycling used in sodium-ion batteries is a major challenge. The rational design of the electrolyte is one of the ways to solve these problems. In this work, 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (HFE) is introduced into a sodium hexafluorophosphate (NaPF6)/ethylene carbonate (EC) electrolyte to design a locally high concentration electrolyte (LHCE), which helps stabilize the solid electrolyte interphase (SEI) in sodium-ion batteries (SIBs). By modulating the solvation structure of the electrolyte, a NaF-rich SEI is formed on the surfaces of electrodes. With sodium iron phosphate (NFPO) as the cathode, the cell maintained a capacity retention rate of 91.5 % after 300 cycles at 0.5C. In addition, a sodium nickel iron manganese oxide (NFMO)||Hard carbon (HC) pouch cell achieves a capacity retention of 84.2 % after 500 cycles at 1C. This study provides a new perspective for the understanding and design of locally high concentration electrolytes for sodium-ion batteries.

Interfacial Water Orientation in Neutral Oxygen Catalysis for Reversible Ampere-Scale Zinc-Air Batteries.

The neutral oxygen catalysis is an electrochemical reaction of the utmost importance in energy generation, storage application, and chemical synthesis. However, the restricted availability of protons poses a challenge to achieving kinetically favorable oxygen catalytic reactions. Here, we alter the interfacial water orientation by adjusting the Brønsted acidity at the catalyst surface, to break the proton transfer limitation of neutral oxygen electrocatalysis. An unexpected role of water molecules in improving the activity of neutral oxygen catalysis is revealed, namely, increasing the H-down configuration water in electric double layers rather than merely affecting the energy barriers for reaction limiting steps. The proposed porous nanofibers with atomically dispersed MnN3 exhibit record-breaking activity (EORR@1/2/EOER@10 mA = 0.85/1.65 V vs. RHE) and reversibility (2500 h), outperforming all previously reported neutral catalysts and rivaling conventional alkaline systems. In particular, practical ampere-scale zinc-air batteries (ZABs) stack are constructed with a capacity of 5.93 Ah and can stably operate under 1.0 A and 1.0 Ah conditions, demonstrating broad application prospects. This work provides a novel and feasible perspective for designing neutral oxygen electrocatalysts and reveals the future commercial potential in mobile power supply and large-scale energy storage.