Silicon has emerged as an anode material of great promise for lithium-ion batteries (LIBs) due to its ultra-high theoretical capacity. Nevertheless, severe volume expansion during lithiation/delithiation processes and intrinsically low electronic conductivity impede its practical application. Although silicon-carbon composites have been recognized as an effective solution to address these challenges, the mechanical ball milling method, a commonly used preparation technique, often results in structural damage to the carbon material. In this study, a simple, cost-effective, and scalable fabrication method for high-performance micron-sized silicon-carbon composites (pSi@C) is successfully developed. The findings confirm that the porous silicon obtained through nonacidic etching exhibits moderate mechanical strength, and the graphite within the outer carbon layer maintains a substantial amount of layered crystalline structure after ball milling. This structural feature effec-tively enhances the mechanical strength, enabling it to better accommodate the volume expansion of silicon, while also improving its electrical conductivity. Consequently, the designed pSi@C anode significantly enhances the cycling stability and rate performance. The pSi@C anode achieves impressive capacity retention of 99.6 % after 200 cycles at 0.5 A g-1, and still delivers a specific capacity of 691.3 mAh g-1 at 1 A g-1. Moreover, full cells assembled with pSi@C anodes and LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes deliver a high specific capacity of 160.0 mAh g-1 with capacity retention of 95.5 % after 400 cycles at 1C. The atomic force microscopy (AFM) characterization results further confirm the significantly enhanced mechanical strength and uniform modulus distribution of pSi@C. This work provides a highly promising and practical approach for the low-cost fabrication of high-performance silicon-carbon anode materials for LIBs.
The growing demand for high-energy-density lithium-ion batteries (LIBs) has renewed interest in silicon-based anodes owing to their ultrahigh theoretical capacity. Nevertheless, the practical deployment of silicon anodes is hindered by...
Rechargeable magnesium batteries (RMBs) have emerged as highly promising next-generation energy storage systems, owing to the high theoretical capacity of magnesium, the natural abundance of magnesium resources, and high safety. However, the commercialization of RMBs is significantly hindered with the magnesium metal anode, including interfacial passivation, volume expansion, and non-uniform Mg stripping/plating. While progress has been made in exploring novel anode materials and interfacial chemistry regulation strategies, the development of stable anodes that simultaneously deliver high energy/power density and long cycle life remains a formidable challenge. This review comprehensively examines recent advances in magnesium anode interface research. We systematically analyze the fundamental mechanisms of interfacial passivation and establish constitutive relationships between material composition, microstructure, and surface properties. The discussion encompasses advanced strategies for interface engineering, including electrolyte design based on coordination chemistry and novel magnesium salts, interfacial modification through solvation structure modulation, and the construction of artificial protective layers. Furthermore, we highlight how advanced characterization techniques and theoretical simulations have revealed underlying operating mechanisms. Finally, we identify current cognitive limitations and technological bottlenecks, providing critical perspectives towards developing stable magnesium anodes with high energy/power density and long cycle life. By clarifying the current cognitive limitations and technical bottlenecks, we aim to provide scientific guidance for the construction of high stability and high kinetic activity of the magnesium anode interface, and accelerate the realization of high-performance practical magnesium batteries.
With the growing demand for high-energy-density and long-lifespan lithium-ion batteries (LIBs), silicon/graphite composites have emerged as promising anode materials, as they synergize the ultrahigh capacity of silicon (Si) and the structural stability of carbon. To address the intrinsic volume variation issue of silicon, this work demonstrates a scalable and environmentally benign synthesis of micron-sized porous silicon/graphite composites (NGT-pSi/C) via the integration of FeCl3-etched spherical porous silicon (pSi) and waste-derived natural graphite tailings (NGT). The as-prepared NGT-pSi/C features a watermelon-like multi-core-shell architecture. The pores in pSi effectively accommodate the large volume expansion during cycling. Meanwhile, the upcycled NGT form a conductive layer to disperse mechanical stress, and the glucose-derived carbon layer constructs a conductive network. This waste-to-wealth approach enables the conversion of industrial byproducts into highperformance LIB anode materials. Comprehensive physicochemical and electrochemical characterizations reveal that abundant pores and continuous conductive networks in NGT-pSi/C synergistically mitigate Si pulverization, suppress interfacial degradation and enhance charge transfer kinetics. The NGT-pSi/C anode delivers exceptional cycling stability (591.2 mAh g-1 after 400 cycles at 0.5 A g-1) and superior rate capability. Furthermore, full cells paired with NCA90 (LiNi0.9Co0.05Al0.05O2) cathodes maintain 72.6% of their initial capacity after 800 cycles. The corresponding pouch cell exhibits a high discharge capacity of 0.7 Ah and retains 74.43% capacity after 500 cycles. This practical strategy achieves a cost-performance synergy. Overall, by using near-zero-cost graphite waste and adopting a non-acidic etching process, this work establishes a sustainable and economically viable pathway for the scalable production of high-performance Si-based anodes.
Alluaudite-type iron-based sulfates are one of the most promising candidates for high-performance sodium-ion batteries (SIBs), yet suffer from sluggish kinetics, severe side reactions and chemical degradation in ambient conditions. Herein, by evaluating the dual element substitution chemistry (F-, Li+, K+, Mg2+, Cr2+, Mn2+, Ni2+, Cu2+, Zn2+, Sn2+, Al3+), a targeted substitution strategy has been successfully proposed. We report a dual-site modified Na2.45Sn0.02Fe1.75(SO3.98)(3)F-0.06@CNT (NFS-Sn-F) cathode with high capacity, exceptional rate capability (50 C), and ultra-stable cycling stability (10000 cycles). By evaluating the dual element substitution chemistry, a targeted substitution strategy employing both Sn and F elements has been successfully proposed. Systematic experimental studies and theoretical calculations reveal that the electronic conductivity of the NFS-Sn-F cathode spherical material has been largely improved, while the Na+ diffusion energy barrier is largely suppressed. Even under a wide-temperature operating condition (-15 degrees C to 60 degrees C), the NFS-Sn-F cathode exhibits a high specific capacity (100.7 mAh g(-1)), good rate capability (similar to 56 mAh g(-1) at a current density of 5300 mA g(-1) at 60 degrees C), and ultra-stable cycling performance (similar to 80.0% capacity retention even after 10000 cycles, with almost no cycling capacity decay at -15 degrees C). Meanwhile, the combined regulation of Sn2+/F- and the carbon coating layer suppresses the attack of H2O on the cathode, enabling the material to maintain a stable structure and cycling performance even after exposure to air for 30 days. The hard carbon||NFS-Sn-F full cell verifies their superior electrochemical performance, which exhibits a long-term cycling life exceeding 6000 cycles. This work provides a universal strategy and a deep understanding in designing high-performance, low-strain and air-stable alluaudite-type iron-based sulfate cathodes for sodium-ion batteries.
Seawater-based zinc-ion batteries (ZIBs), in terms of integration with high safety, environmental friendliness, and low cost, have been regarded as one of the most promising next-generation large-scale electrochemical storage systems. However, the complex ionic environment of seawater-based electrolytes, which leads to chloride pitting corrosion, zinc (Zn) dendrite growth, and hydrogen evolution reactions (HER), impedes their practical applications. Herein, we design a multi-functional binary additive electrolyte incorporating carboxymethyl cellulose (CMC) and magnesium sulphate (MS) into seawater-based electrolytes to tackle these challenges. The addition of CMC with strong Zn/Zn2+ affinity can significantly modify the solvation structures within the seawater-based electrolyte and facilitate the reversible deposition behaviour of Zn2+ ions. Moreover, the cation-binding properties of CMC2- enable it to effectively induce Mg2+ ions and seawater cations toward the Zn anode. Simultaneously, Mg2+ ions, possessing the highest charge density among seawater ions, show strong electrostatic forces toward free-water. Thus, it can induce the multiple seawater cations to form a water-poor layer on the Zn anode surface, thereby inhibiting the HER and the corrosion reactions. Notably, the intercalation reactions of multiple cations effectively suppress the structural collapse of cathode materials. Equally important, we innovatively introduced a unidirectional gas valve to resolve gas generation issues of the pouch cell, effectively resolving the key issue of gas accumulation in practical applications. Benefiting from the superior modification effect of the binary additive, the Zn//Zn symmetric cells in seawater-based electrolyte exhibit a long-term stability of over 5197 h at 5 mA cm-2. Furthermore, the Zn//Cu asymmetric cells possess an average CE of 99.74% over stable cycling for 4000 cycles at 5.0 mA cm-2. The Zn//NVO full cells retain 150 mAh g-1 after 1000 cycles at 2 A g-1. This novel strategy of combining organic/inorganic additives with seawater-based electrolytes offers an inspired and straightforward approach to solving the fundamental challenges in ZIBs, driving progress in seawater energy storage applications.
Rechargeable magnesium batteries (RMBs) have emerged as a promising alternative to lithium-ion batteries owing to abundant magnesium (Mg) resources and their high volumetric capacity. Nevertheless, the practical application of RMBs is constrained by the inadequate compatibility between Mg metal anodes and electrolytes, which manifests as issues such as passivation layer formation and dendrite growth. Herein, to address these challenges, a controllable vacuum thermal evaporation technology was first employed to construct an ultra-thin and flat bismuth (Bi) nanoparticle artificial interface on the Mg metal surface (Bi@Mg), yielding a high-performance Mg anode for a practical Mg battery pouch cell. During the charge-discharge cycling, the nano-sized Bi-metal particles undergo an in situ alloying reaction to form the Mg3Bi2 alloy layer, generating abundant magnesiophilic sites that accelerate Mg2+ ion transport and induce uniform Mg deposition. Benefiting from this unique Mg2+ ion deposition mechanism, the symmetric Bi@Mg cell exhibits remarkable cycling stability, with a lifespan exceeding 4000 h (at the current density of 0.2 mA cm-2) and low polarization in the all-phenyl complex (APC) electrolyte. Furthermore, the Bi@Mg & Vert;Mo6S8 full cell demonstrates a high specific capacity of 73.78 mAh g-1 and 94.86% capacity retention even after 2000 cycles at 1C. Notably, the Bi@Mg anode enables stable operation of a pouch cell (100 cycles at 1C), further confirming its potential for practical applications. This study provides a novel strategy for constructing stable Mg metal anodes and offers valuable insights for the development of high-performance practical RMBs.
O3-type layered transition metal (TM) oxides have emerged as the most promising cathodes for high-energy sodium-ion batteries (SIBs) due to their high theoretical capacity. However, for prototypical O3-type NaNi1/3Fe1/3Mn1/3O2 (NNFM), the cycle life remains a significant challenge, particularly under harsh operating conditions, such as high voltage and low/high temperatures, due to the severe structural/interfacial degradation. Because of the complex electrochemical phase transition, the layered structure undergoes anisotropic lattice variation and dramatic volume change, which is accompanied by unfavorable structural distortion and microcrack formation, inevitably resulting in rapid capacity fading. Herein, a customized dual-site engineering is proposed to enhance the cycling stability of layered oxides. Through a screening mechanism based on ionic radius (Li+, K+, Ca2+, Sr2+, and Ba2+), electronegativity, and bond dissociation energy, calcium (Ⅱ) is identified as optimal Na-site dopant paired with TM-site dopant of titanium (Ⅳ) to construct an oxygen-stabilized framework for NNFM, and its impacts on structural evolution, interfacial stability, and electrochemical behavior are systematically investigated. Systematic experimental studies and theoretical calculations reveal that the dual-site synergistic effect effectively mitigates adverse phase transitions, reduces oxygen evolution, and improves reaction kinetics. The designed NNFM-CaTi electrode demonstrates ultra-stable cycling over 500 cycles at 1 C and retains stability for more than 200 cycles even under a high cut-off voltage of 4.2 V. The Ah-level pouch cell with a high energy density of 145 Wh kg⁻1 achieves 77.79% capacity retention even after 500 cycles at 1 C. This dual-site engineering provides a deep insight into the development of O3-type layered cathodes for durable, high-energy SIBs.
Ni-rich layered oxide cathodes are promising candidates for next-generation high-energy-density lithium-ion batteries owing to their high capacity and cost-effectiveness. However, their widespread application is hindered by structural instability, interfacial side reactions, lattice distortion, and microcrack formation during cycling. Herein, a previously unreported synergistic dual rare-earth (Yb/Y) co-doping strategy is proposed for a LiNi0.9Co0.05Al0.05O2 (NCA) cathode to simultaneously stabilize the bulk crystal structure and the electrode-electrolyte interface. Combined experimental results and density functional theory (DFT) analyses demonstrate that Yb/Y incorporation into transition-metal sites effectively enlarges Li+ diffusion pathways, suppresses Li+/Ni2+ cation disorder, and stabilizes lattice oxygen through strong Yb/Y-O bonds, thereby mitigating bulk structural degradation. In addition, a uniform, dense, and mechanically robust cathode-electrolyte interphase (CEI) is formed in situ, effectively mitigating electrolyte corrosion, lowering the interfacial resistance, and suppressing particle cracking for NCAYbY. Consequently, the modified NCAYbY cathode exhibits outstanding electrochemical performance, delivering a high reversible capacity of 222.8 mA h g-1 at 0.2C with 95.79% capacity retention after 100 cycles. Remarkably, the corresponding full cell retains 78.35% capacity after 700 cycles at 1C, while a pouch cell exhibits an initial discharge capacity of similar to 900 mA h with 78.60% retention after 300 cycles. This work establishes dual rare-earth co-doping as an effective and practical design principle for realizing structurally and interfacially robust Ni-rich cathodes for high-performance, long-life lithium-ion batteries.
Silicon (Si) is considered a promising candidate anode for next-generation high-performance lithium-ion batteries (LIBs) due to its ultrahigh theoretical capacity. However, silicon anodes suffer from huge volume expansion and inherently low electron conductivity for LIBs. Nanostructured silicon could address the limitations of bulk Si anodes, but the high cost would limit its commercial application. Herein, an eco-efficient, nonacidic etched, and cost-effective method is successfully proposed to prepare high-performance micron-sized porous silicon/carbon composites. The physicochemical/electrochemical characterizations demonstrated that the abundant pores and continuous conductive network structure in the pSi@C composites can effectively alleviate the volume expansion of silicon and largely enhance the electrical conductivity in long-term cycling. The designed pSi@C anode can largely enhance the long-term cycling performance and rate capability, with a high capacity of 629.6 mA h g-1 after 400 cycles at 0.5 A g-1 and a superior rate performance of 501.3 mA h g-1 even at 1 A g-1. Furthermore, the full cells with the pSi@C anodes and LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes deliver a high specific capacity of 143.5 mA h g-1 and 83.9% capacity retention after 300 cycles. This eco-efficient and cost-effective method provides a promising and practical way for commercializing high-performance silicon-carbon anode materials for LIBs.
The promising development potential of sodium-ion batteries (SIBs) as complementary candidates to lithium-ion batteries (LIBs) for large-scale energy storage systems calls for a more fundamental investigation and performance optimization of layered transition metal (TM) oxide cathode materials. However, insufficient rate capability and rapid capacity decay have hindered the potential application of low-cost O3-type Ni/Fe/Mn-based layered oxides. Herein, a universal strategy using the multifunctional rare earth elements (REs = Lu, Yb, Er, etc.) as cationic dopants for NaNi1/3Fe1/3Mn1/3O2 cathodes to manipulate the intrinsic local chemical environment has been successfully reported, which effectively stabilizes the structural framework and improves the Na+ ion transport kinetics, owing to the reinforced TM-O bonds, the weakened Na-O bonds, and the more favorable chemical states of Ni and Mn. As expected, such a RE-doping strategy based on tailoring local chemistry allows for an electrochemical performance improvement. The designed Lu-modified NaNi1/3Fe1/3Mn1/3O2 cathode exhibits a high capacity of 151.36 mA h g-1 at 0.1 C, excellent rate capability (119.06 mA h g-1 with a 78.66% retention at 10 C), and a long-term cycling performance with a capacity retention of 82.39% after 500 cycles even at 5 C. The full cell with a hard carbon anode demonstrates a high energy density of 281.3 W h kg-1 and a long-term cycling performance over 500 cycles at 5 C. This work will demonstrate the role of REs in strategically tailoring the local chemistry of layered oxide cathode materials, boosting the rapid and qualitative development of high-performance SIBs.
High-Ni layered oxide cathode materials are promising cathode materials for high-energy-density lithium-ion batteries (LIBs). However, high-Ni layered oxide cathodes still face issues, such as rapid structural collapse and surface parasitic reactions. Herein, a universal strategy using rare earth (La, Pr, Sm, Eu, Tb, Ho, etc.) lattice-optimized spray-drying preparation combined with the integration of a solid-state synthesis process for preparing spherically high-Ni cathodes is probed. This practical method synergizes rare earth lattice optimization and an artificial coating strategy for high-performance high-Ni LiNi0.84Co0.12Al0.03Ho0.01O2 cathodes. The doping of Ho mitigates the mixing of Li+ and Ni2+ ions, and the suitable ionic radius ofHo element enlarges the plane spacing and promotes the rapid diffusion of Li+ within the particles without causing significant lattice distortion. The cathodes show a high capacity of 223.7 mAh g-1 at 0.2 C and keep an ultra-stable cycling stability even after 1200 cycles at the full-cell level. This work provides a facile and highly efficient strategy for designing spherical, high-capacity, and long-cycle-life high-Ni layered oxide cathodes for practically sustainable LIBs.
Magnesium-air (Mg-air) batteries have emerged as a promising sustainable energy storage technology, offering exceptional theoretical energy density, low cost, and environmental compatibility. Despite these advantages, their development remains largely confined to experimental phase. A critical barrier to commercialization is the poor corrosion resistance of the anode resulting in low anodic efficiency. This article presents a comprehensive review of strategies aimed at improving the utilization efficiency of Mg anodes, with a particular focus on addressing corrosion issues from a microstructural standpoint. Firstly, the principle of Mg-air batteries has been outlined and the corrosion behavior has been discussed. The review then delves into a variety of representative anode materials. Special attention is given to innovative material designs that mitigate the challenges typically encountered by Mg-air batteries. Finally, the paper provides an outlook on future research directions, identifying critical technological barriers and highlighting areas that warrant further investigation. By offering a detailed analysis of material structures, this article aims to contribute valuable insights for advancing the development of high-performance Mg-air batteries.
Co-free high-Ni layered cathode materials LiNixMeyO2 (Me = Mn, Mg, Al, etc.) are a key part of the next-generation high-energy lithium-ion batteries (LIBs) due to their high specific capacity and low cost. However, the hindered Li+ kinetics and the high reactivity of Ni4+ result in poor rate performance and unsatisfied cycling stability. This work designs a promising strategy for designing a high-performance high-entropy doping Co-free high-Ni layered cathode LiNi0.9Mn0.03Mg0.02Ta0.02Mo0.02Na0.01O2 (HE-Ni90-1.557) by elemental screening and compositional fine-tuning. Compositional fine-tuning optimizes the synergistic relationship between the high-entropy dopant elements, thereby significantly suppresses the kinetic hysteresis induced by Li+/Ni2+ mixing. The pillar effect significantly enhances the diffusion kinetics of Li+ at the high state of charge (SOC). Meanwhile, the high-entropy fine-tuning significantly postpones the H2-H3 phase transition and reduces the dissolution of transition metals and the loss of lattice oxygen in the cathodes. Consequently, the diffusion kinetics of Li+ at the atomic and electrode particle scales are significantly enhanced. The HE-Ni90-1.557 cathode exhibits an initial capacity of 225.1 mAh g-1 at 0.2 C and a full cell with a high capacity retention of 83.1% after 1500 cycles at 3C. This work provides a promising avenue for commercializing Co-free high-Ni cathodes for next-generation LIBs.
Developing “beyond lithium-ion ” batteries with reduced cost per unit of stored energy, high safety, and good electrochemistry performance is regarded to be an urgent task for rechargeable battery systems ascribing to the coming technical bottleneck of the state-of-the-art commercial Li-ion batteries. Rechargeable multivalent ion batteries (RMIBs), such as Zn 2+ , Mg 2+ , Ca 2+ , and Al 3+ ion batteries, have attracted intensive attention due to their low cost, high safety, high energy density, and operating availability. However, the development of high-performance RMIBs, is severely hindered due to the lack of appropriate cathode materials, electrolytes with wide electrochemical windows, and highly reversible and stable anodes.Therefore, some research progress on RMIBs is reviewed and summarized However, most of the reported reviews mainly focus on the cathode and electrolyte of RMIBs. A comprehensive review of anode chemistry is not reported yet. In particular, the fundamental electrodeposition chemistry of RMIBs is not fully understood. This review summarizes the recent advances and the basic mechanism in researching anode electrodeposition chemistry for RMIBs. The understanding of the anode electrodeposition chemistry can accelerate the development of the application of practical RMIBs is hoped.
Aqueous zinc‐ion batteries (AZIBs) have emerged as a promising energy storage solution owing to their intrinsic safety, low cost, environmental friendliness, and high theoretical specific capacity. However, their practical application is hindered by uncontrollable dendrite growth and side reactions at the zinc metal anode. To address these challenges, a simple and cost‐effective electrodeposition strategy is proposed to construct a quaternary Zn‐Cu‐Sn‐Bi alloy artificial interface layer on zinc foil (ZCSB@Zn) as the anode of AZIBs. Density functional theory (DFT) calculations and in situ optical dendrite observation confirm that this dense alloy interface layer reduces the migration barrier and weakens hydrogen adsorption, facilitating uniform zinc deposition while effectively suppressing side reactions and dendrite formation. The symmetric ZCSB@Zn cell exhibits extraordinary cycle stability exceeding 8000 h. Furthermore, the assembled ZCSB@Zn//CSB‐MnO 2 full cell demonstrates a high specific capacity of 199 mAh g −1 at 1 A g −1 , maintaining stability even under high loading of 10 mg cm −2 and high temperature conditions (50 °C). This study presents a scalable and cost‐effective strategy for constructing quaternary artificial interface layers in zinc metal anodes, highlighting their potential for practical AZIB applications.
Manganese-based layered compounds offer promising cathode materials for aqueous zinc-ion batteries (AZIBs) due to their high safety, low cost, and environmental friendliness. However, their sluggish reaction kinetics, poor conductivity, and irreversible manganese dissolution result in severe capacity fading. Herein, a simple two-step method is successfully proposed to intercalate Ba2+ ions into layered manganese oxide (Ba-MnO2), which were utilized as cathode materials for AZIBs. Ba2+ ions have been innovatively introduced into the MnO2 cathode, generating abundant oxygen vacancies. Notably, the incorporated Ba2+ spontaneously forms an in situ BaSO4 layer during charging, which functions as a protective cathode electrolyte interface. These improvements promote the conductivity and ion diffusion of MnO2, enabling a reversible MnO2/Mn2+ deposition/dissolution reaction. The Zn//Ba-MnO2 full battery delivers a high capacity of 355 mA h g-1 at 0.3 C and maintains an ultrastable cycling stability of over 1200 cycles even at 3 C. This work provides an innovative strategy and a profound understanding of designing high-performance cathodes for AZIBs.
Magnesium-ion batteries (MIBs) have become the focus of next-generation energy storage technology due to their unique advantages: Mg is abundant in the Earth's crust, with an abundance of 2.3 %, and the theoretical volumetric energy density can reach 3833 mAh cm-3. Additionally, the magnesium deposition/stripping process poses no risk of dendrite formation. However, the high charge density of divalent Mg2+ induces strong polarization effects, resulting in ion diffusion kinetics delay in the cathode material. At the same time, side reactions caused by electrode/electrolyte interface mismatches severely restrict the cycling performance of the battery. Among these, intercalation-type cathode materials have become the core research direction to overcome the performance bottlenecks of MIBs, owing to their rigid crystal framework and minimal voltage hysteresis effect. This paper systematically reviews the Chevrel phase, layered transition metal oxides, layered transition metal sulfides, transition metal carbides/nitrides, polyanion compounds, and Prussian blue analogs, thoroughly exploring their magnesium storage mechanisms, research progress, and performance limitations. It focuses on interface engineering, defect engineering, and pre-intercalation modification strategies to enhance material performance. By analyzing the current research efforts, this work provides theoretical support and technical pathways for the industrialization of safe and long-life MIBs.
Na2+2xFe2-x(SO4)3 (NFSO) is a promising cathode material for sodium-ion batteries (SIBs) due to its low cost and high operating potential (≈3.8 V). However, poor intrinsic electronic conductivity and sluggish kinetics are major drawbacks to its practical application. Herein, magnesium doped Na2+2xFe2-x(SO4)3 microspheres (Na2.54(Fe0.97Mg0.03)1.73(SO4)3) are synthesized via a designed spray-drying process. The optimized cathode material (NFSO@C-Mg0.02) possesses excellent rate performance up to 50C (50.8 mAh g-1 at 50C) and long-cycle stability (capacity retention of 78.3% even after 9000 cycles at 10C). Despite an increase in the mass loading to 10 mg cm-2, the electrode continues to represent a reversible capacity of 72.1 mAh g-1 at 3C. Furthermore, NFSO@C-Mg0.02║HC full cell demonstrates superior cycling stability (80% capacity retention over 8000 cycles at 5C) and high energy density (≈310 Wh kg-1, based on the cathode). In situ X-ray diffraction (XRD) results reveal that the Mg doping strategy successfully mitigates the variation in lattice volume. The density functional theory (DFT) calculations verify that the prominent rate performance is attributed to the enhanced Na+ diffusion kinetics and low ionic-migration energy barrier. This work provides an effective strategy and a fundamental understanding to enhance the electrochemical performance of cathode materials for SIBs.
Zn powder anodes hold great promise for aqueous zinc-ion batteries (AZIBs) owing to their structural tunability, facile processability, and cost-effectiveness. However, their practical application is hindered by severe side reactions and uncontrolled dendrite formation, leading to rapid capacity degradation. Herein, we develop a Zn powder-based anode (ZnSn@ZP) with a Zn-Sn metal interface layer, fabricated via a simple electrodeposition strategy, to achieve uniform Zn deposition/stripping. The dense Zn-Sn interphase layer effectively mitigates anode corrosion, regulates nucleation, and suppresses dendritic growth, leading to remarkable electrochemical performance. The symmetric ZnSn@ZP cell exhibits exceptional cycling stability exceeding 1500 h at 1 mA cm-2 with an initial voltage hysteresis of 16.4 mV. The ZnSn@ZP//Cu asymmetric cell demonstrates superior average coulombic efficiency of 99.6% over 2500 cycles, indicating improved Zn deposition/stripping performance. Furthermore, the full cell assembled with the MnO2 cathode exhibits excellent cycling performance, maintaining stable cycling for 1800 cycles even at 1 A g-1 with negligible capacity decay. This work presents an effective, cost-effective and scalable interface engineering strategy, offering new insights for developing high-stability Zn powder-based anodes.