Metallic tin, distinguished by its intrinsically high theoretical specific capacity, superior electrical conductivity, and inherent eco-compatibility, has been strategically validated as a next-generation anode candidate for lithium-ion batteries. Nonetheless, the significant volume change and large reversible capacity loss during the electrochemical reaction limit its application. In this paper, MnO2 is successfully introduced into Sn material by magnetron sputtering method to create additional particle interfaces to buffer the volume expansion of the SnMnO2 composite films. Simultaneously, the synergistic interaction between MnO2 and Sn particles facilitates the enhancement of lithium-ion diffusion and transmission rates within the composite film, thereby improving its specific discharge capacity and cyclic stability. Consequently, compared with a pure Sn anode, the Sn-MnO2 composite film demonstrates exceptional comprehensive electrochemical performance. At current densities of 99 mA g-1 and 994 mA g-1 , the specific capacities of the Sn-MnO2 composite film can reach up to 1550 and 1058 mAh g- 1 respectively, which is much higher than the pure Sn electrode. This study demonstrates that the uncomplicated design concept, manufacturing methodology, and remarkable performance collectively, show that the novel Sn-based composite film holds promise as a promising anode material for Li-ion batteries.

Lithium-rich manganese layered oxides (LRMOs) are regarded as promising cathode materials for next-generation Li-ion batteries due to their high capacity. However, LRMOs are prone to irreversible oxygen desorption and localized stress concentrations during cycling, leading to structural collapse and capacity decay, limiting their practical application. Herein, this study innovatively proposes a dual-phase composite reinforcement engineering that achieves a homogeneous distribution of Li+ from the bulk to the surface, significantly enhancing the structural stability and electrochemical performance of the LRMO cathode. By in situ constructing dual-phase composite nanostructures on the surface of LRMO, specifically comprising an Fe-enhanced spinel outer surface and an Fe-gradient-doped layered structure in the subsurface. This strategy significantly reduces the Li+ diffusion barrier while effectively improving the uniformity of Li+ concentration distribution and the stability of the surface structure. Furthermore, Fe in the lattice forms highly stable Fe & horbar;O bonds, which increase the formation energy of oxygen vacancies and reduce the excessive oxidation of lattice oxygen. The modified LRMO exhibits an impressive capacity of 249.76 mAh & centerdot;g- 1 at 1C and maintains an outstanding capacity retention rate of 91.5% after 200 cycles. This innovative engineering tackles surface degradation for LRMOs, paving the way toward high-capacity and stable cathode materials.

LiMn0.6Fe0.4PO4 (LMFP) cathodes possess high operating voltages, yet their application is severely hindered by sluggish electron/lithium-ion transport kinetics and interfacial instability during cycling. To address these challenges, this work proposes a surface engineering strategy utilizing a boron-doped carbon coating to modulate the interfacial kinetics of LMFP. The introduction of boron modifies the local electronic structure, inducing defects and holes that facilitate Li-ion migration, while simultaneously maintaining the layer's physical continuity and protective function against manganese dissolution. Within the investigated doping range, the 2% B-doped sample exhibits the best equilibrium between rate performance and cyclability, retaining 95.66% capacity after 100 cycles at 1 C and 93.20% after 300 cycles at 5 C, significantly outperforming the pristine sample (82% and 74%, respectively). In situ electrochemical impedance spectroscopy (EIS) combined with distribution of relaxation times (DRT) analysis reveals that the coating synergistically reduces interfacial charge-transfer resistance throughout the charge-discharge process. Consequently, this study defines an optimal boron-doping window to successfully navigate the trade-off between achieving rapid Li-ion kinetics and ensuring robust interfacial stability in olivine cathodes.

P2-type layered oxide NaxMnO2 holds promise as a cathode material owing to its high theoretical energy density (approximate to 260 Wh kg-1), low cost, and environmental friendliness. However, structural degradation triggered by the Mn3+-collaborative Jahn-Teller distortion and lattice oxygen loss during cycling severely impedes its practical deployment. In this work, a "Zn2+ pinning" strategy is employed to construct a rigid layered structure, which significantly enhances structural stability and rate performance. The pinned Zn2+ in the lattice prevent structural collapse induced by the accumulation of Jahn-Teller distortion, thereby enhancing structural stability. Furthermore, the incorporation of Zn2+ increases the interlayer spacing, facilitating the migration rate of Na+. Particularly, Na0.62Zn0.03Mn0.97O2 delivers a reversible capacity of 155 mAh g-1 at 1 C (150 mA g-1) with a capacity retention of 83% after 200 cycles, far exceeding the 34% retention of Na0.62MnO2. Even at 10 C, it maintains a reversible capacity of 120 mAh g-1, and retains 84 mAh g-1 after 500 cycles. This "Zn2+ Pinning" strategy enables the scalable production of high-rate, long-life layered oxide cathodes for sodium-ion batteries.

Nickel-rich layered oxide cathodes are considered one of the most promising lithium-ion battery cathodes due to their high specific capacity and low cost. However, interfacial side reactions and microcrack propagation during long cycle processes limit the industrial application of nickel-rich cathodes. This paper synthesized nickel-rich cathode materials with different primary particle sizes through careful microstructural design, and systematically studied the effect of primary particle size on the lithium ions diffusion kinetics and cycling stability of nickel-rich layered cathode materials. By comparing the lithium ions diffusion kinetics of different particle sizes and the cycling performance at different rates, the relationship between primary particle size and the cycling stability of nickel-rich cathodes was determined. Small-sized primary particle samples exhibit higher lithium-ion diffusion rates, but their dense grain boundaries exacerbate interfacial side reactions. In contrast, large-sized primary particle samples reduce grain boundary density, thereby improving interfacial stability. Unfortunately, large-sized primary particle samples lengthen lithium-ion diffusion paths, leading to sluggish lithium-ion diffusion kinetics. Medium-sized primary particle samples balance the effects of surface side reactions and diffusion kinetics, suppressing H2-H3 phase transition degradation while improving lithium-ion diffusion kinetics during cycling, significantly enhancing the stability of nickel-rich cathodes. Medium-sized primary particle samples maintain a capacity retention of up to 83.7 % after 150 cycles at 1C, significantly outperforming smallsized and large-sized primary particle samples. This study provides valuable insights into the relationship between primary particle size and electrochemical stability, which can guide the rational design and synthesis of high-performance nickel-rich layered oxide cathodes.

P2-NaxMnO2 layered oxides are highly regarded cathode materials for sodium-ion batteries due to their high theoretical specific capacity, low cost, and environmental friendliness. However, their large-scale application is hindered by the slow diffusion kinetics of sodium ions and structural degradation due to manganese ion dissolution. Herein, we employ a strategy of combined bulk and surface modification to improve the sodium ion mobility and structural stability, strengthening the structural stability and electrochemical performance of Na0.62MnO2 (NMO). The implanted Mg2+ increases the sodium ion migration rate by enlarging the Na layer spacing of NMO and suppressing the oxygen redox and Mn-O anisotropy changes in the bulk, thereby maintaining the stability of the bulk laminar structure by mitigating the O loss and the dissolution of transition metal ions. The in-situ Na2B4O7 coating with 3D Na+ transport channels on the NMO surface not only improves the interfacial diffusion rate during charging/discharging processes but also avoids the direct contact between the electrode and the electrolyte, which alleviates the side reactions on the electrode surface, thus increasing the cycling life of the electrode. The modified material exhibits high reversible capacities of 171.18 mAh g-1 and 145.88 mAh g-1 at rates of 150 mA g-1 and 750 mA g-1, and the capacity retention rate is 80 % after 500 cycles at 750 mA g-1. In addition, the Na2B4O7 coating improves the air stability of NMO by preventing the generation of hydrated phases on the surface of the material. This simple superposition modification strategy provides important guidance for the scale-up preparation of layered oxide cathode materials with high-rate performance and structural stability, which is expected to advance the industrial application of sodium manganate layered cathode materials.

Halide superionic conductors have garnered considerable attention due to their high ionic conductivity, mechanical deformability, and excellent oxidative stability. However, their incompatibility with lithium metal results in a thermodynamically unstable interface that increases interfacial impedance, thereby limiting the performance of halide-based all-solid-state lithium-metal batteries (ASSLBs). In this study, we report the synthesis of a series of iodide-chloride solid electrolytes, Li2ZrCl6-xIx (x = 0-3), designed to enhance the reduction stability of the electrolyte through the high polarizability of I-. The substitution of I- promotes covalent bonding with the central cation, thereby reducing its reduction tendency. The Li/Li2ZrCl4I2/Li symmetric cell exhibits stable cycling for over 6000 h at 0.2 mA cm-2 and withstands high critical current densities up to 6 mA cm-2. Full cells incorporating Li2ZrCl4I2 as the solid electrolyte exhibit enhanced cycling stability and capacity retention. Furthermore, the characterization by XPS and ToF-SIMS revealed the formation of an interfacial passivation layer composed of LiI and LiCl, which effectively stabilized the lithium-metal electrode and inhibited further electrolyte decomposition. These findings highlight the potential of iodide-substituted halide electrolytes in addressing interfacial challenges associated with lithium metal anodes, providing a promising pathway for the practical implementation of high-energy-density ASSLBs.

Co-free Li-rich Mn-based cathode materials (LMNO) have gradually become powerful competitors with ultra-high specific discharge capacity and energy density. However, high-rate performance and severe voltage decay restrict the commercial application of LMNO. Herein, LiAl5O8 acts as a templating agent to construct 3D neural-like networks in LMNO, enabling fast ion diffusion and improving rate performance. Proton exchange is predominantly facilitated by the process of LiAl5O8 constructed to generate vacancies for oxygen preservation, while strong Al-O bonds stabilize interfacial lattice oxygen, effectively suppressing voltage decay due to structural evolution. As a result, the designed cathode exhibits a discharge specific capacity of 154.65 mAh g-1 at 5 C and 91.68% capacity retention after 400 cycles (vs . 66.67% of LMNO), effectively suppressing voltage decay with 90.90% voltage retention (vs . 81.08% of LMNO). The constructed neural-like network structure engineering provides an innovative direction for improving the high-rate performance and structural stability of LMNO.

Nickel-rich cathode materials hold immense potential for electric vehicle batteries due to their high energy density and cost-effectiveness. However, structural degradation and capacity fading during high-rate operation hinder their widespread adoption. This groundbreaking study presents a novel "three birds with one stone" strategy to simultaneously optimize microstructure, lattice oxygen stability, and surface modification in LiNi0.97Co0.02Mn0.01O2 (NCM97) cathode materials. By introducing Mo ions through a facile one-step method, a porous structure is achieved for stress dissipation, Li2MoO4 spinel coating for improved interfacial stability, and rigid Mo & horbar;O bonds for lattice oxygen stabilization. This holistic approach significantly enhances the structural stability and electrochemical performance of NCM97, resulting in higher capacity retention and superior rate performance. The modified NCM97 boasts an impressive initial capacity of 232.6 mAh g-1 at 0.1C and 182.3 mAh g-1 at 5C, along with an exceptional capacity retention rate of 80.6% after 300 cycles at 5C. Most notably, when integrated into a pouch full cell with a graphite anode, the NCM97-Mo cathode achieves a remarkable 88.4% capacity retention after 800 cycles at 2C. This innovative strategy paves the way for the industrial development of high energy density nickel-rich cathode materials, revolutionizing the electric vehicle battery landscape.

Single‐crystal Li‐rich Mn‐based cathode materials (SLRMs) are promising for high‐energy lithium‐ion batteries due to their structural robustness. However, interfacial instability under high voltage triggers structural collapse and rapid capacity fading, hindering practical applications. Herein, an innovative strategy is proposed to deeply enhance the surface stability of SLRMs by constructing an Al 3+ ‐reinforced spinel shallow surface structure and an Al 3+ gradient‐doped layered subsurface structure in single‐crystal Li 1.2 Mn 0.54 Ni 0.13 Co 0.13 O 2 . This composite structure effectively protects reactive oxygen species from electrolyte attack, mitigating capacity fading caused by interfacial side reactions. Theoretical calculations reveal that the oxygen vacancy formation energy of the Al 3+ ‐reinforced spinel shallow surface structure increases from 4.21 to 5.40 eV, while that of the Al 3+ ‐doped layered subsurface structure rises from 3.88 to 4.05 eV. Such enhancedoxygen vacancy formation energy effectively suppressed irreversible oxygen release and phase transitions, thereby strengthening the interfacial stability of SLRMs. The modified SLRMs deliver a discharge capacity of 232 mAh g −1 at 1 C, with only 5% capacity loss after 200 cycles. This study resolves interfacial degradation in SLRMs via atomic‐level tailored deep surface engineering, establishing a blueprint for designing cathode materials with structural robustness.

Ultrahigh‐nickel cathodes have become a promising option for high‐performance lithium‐ion batteries (LIBs). However, traditional ultrahigh‐nickel secondary particles often crack at the interfaces between primary grains, causing significant surface side reactions. On the other hand, single‐crystalline particles face issues like long lithium‐ion diffusion paths and surface reconstructions. To address these challenges, this study introduces a sub‐single‐crystal structural strategy designed to shorten lithium‐ion diffusion paths within the particles and uses a grain‐boundary bonding technique to reduce the risk of secondary microsphere fracturing due to uneven mechanical stress. Specifically, 1 µm LiNi 0.93 Mn 0.07 O 2 single‐crystal particles are bonded with Li 3 BO 3 to create secondary particles. These smaller single‐crystal particles not only reduce the diffusion distance but also improve Li+ transport channels at grain boundaries. The bonding layer effectively limits electrolyte–electrode contact, prevents harmful grain phase changes, and boosts the cycle stability of the electrode material. In full battery tests with graphite anodes at a 1 C‐rate, the capacity retention rate is nearly 90% after 800 cycles at room temperature and about 82% after 800 cycles at 60°C. These results show that the structural design strategy greatly enhances structural stability. This research provides a solution for ultra‐high nickel cathodes, offering strong potential for advancing their practical applications.

The application of lithium-rich manganese-based layered oxides (LRMLOs) is constrained by the deterioration of their electrical properties, which is attributable to inadequate lattice oxygen stability. Herein, a dual-strategy synergistic Li 1.2 Mn 0.54 Ni 0.13 Co 0.13 O 2 was synthesized by simultaneously creating oxygen vacancies and Mo-O bonds via the pyrolysis of (NH4)2MoO4 & sdot;4 H2O. The generation of oxygen vacancies on the surface of LRMLOs helps prevent the formation of O-O dimers and reduce the loss of lattice oxygen. Additionally, incorporating Mo6 + into the bulk phase of LRMLOs enhances the stability of lattice oxygen by modifying its coordination environment. The combined effects of these two factors effectively suppress irreversible lattice oxygen release in LRMLOs, resulting in a significant enhancement of cyclic stability. The initial Coulombic efficiency of the modified LRMLOs improves from 77.70 % to 83.74 %, while the specific discharge capacity increases from 271.53 mAh g-1 to 287.12 mAh g-1 at 0.1 C. Meanwhile, the modified LRMLOs exhibit a capacity retention of 90.23 % over 200 cycles at 1 C. This study presents a straightforward and viable method for addressing lattice oxygen loss in LRMLOs, which has the potential to advance high-energy-density lithium-ion batteries.

Emerging halide superionic conductors with remarkable oxidative stability and deformability, making them a potential game-changer for high-performance all-solid-state Li batteries (ASSLBs). The recently reported Li2ZrCl6 (LZC) with low cost possess great potential. However, its ionic conductivity at 25 degrees C is below 1 mS cm(-1). Herein, we developed a Li-richened strategy to LZC by doping O2- at Cl- site via a mechanochemical method to form oxychloride electrolytes Li2+xZrCl6-xOx (0 <= x <= 1.8), resulting in high ionic conductivity up to 1.46 mS cm(-1) at room temperature (RT). The experimental results and theoretical calculations (ab initio molecular dynamics simulations) demonstrate that the Li2O doping leading to a Li-richened LZC lattice effectively enhances the Li+ conductivity in solid-state electrolytes (SSEs). Significantly, an increasing O2- substitution in the Li2+xZrCl6-xOx microcrystalline framework induces a progressive structural evolution from triangular to monoclinic phases, accompanied by a redistribution of Li+. Furthermore, the ASSLBs formed by Li3.4ZrCl4.6O1.4 (LZCO) with Li-In anode and bare LiCoO2 cathode shows excellent long-term cycling stability (94 % capacity retention for 600 cycles at 1 C) and high-rate performance (105.7 mAh g(-1) at 2 C). This exploratory study provides a promising strategy to facilitate the application of low-cost LZC-based SSEs for high-performance ASSLBs.

Li-rich Mn-based materials provide higher capacity than commercial NCM layered materials due to the synergistic redox effect of cations and anions. However, lattice straining and structural collapse caused by the irreversible oxygen release at high voltage range during cycling, which results in severe capacity and voltage decay. Herein, a synergistic strategy of surface-induced spinel structure and F doping is provided to improve the structural stability. The surface spinel structure helps to reduce the structural collapse caused by electrolyte corrosion on the cathode and effectively inhibits voltage decay resulted from structural evolution. The stronger Mn -F bonds are formed by F doping to inhibit migration of transition metal (TM) and induce the uniform deposition of LiF to form the thinner and more stable CEI on the cathode. Accordingly, the designed cathode (LMNO-NF) shows remarkable cycling performance with the capacity retention of 86.68 % and voltage retention of 96.6 % for 200 cycles at 1C, higher than pristine material (68.76 % and 85.75 %). Therefore, this simple dual -modi fication strategy of one-step synthesis is promising for solving the structural evolution and voltage decay of Li-rich Mn-based cathode materials effectively, achieving further commercialization.

Silicon is considered as the most felicitous anode material candidate for lithium-ion batteries on account of abundant availability, suitable operating potential, and high specific capacity. Nevertheless, drastic volume expansion during the cycle impedes its practical utilization. Herein, Si and MnO2 (Si-MO) constructed the binder-free intertwined electrode that is reported to effectively improve upon the cycling stability of Si-based materials. The Si-based electrode without a binder has good electrical conductivity, strong adhesion to the substrate, and ample space for mitigating volume expansion. The incorporation of MnO2 establishes a multiphase interface, which mitigates the electrode volume expansion, and supports the electrode structure. Furthermore, MnO2 (∼1230 mAh g-1 theoretical capacity) synergistically enhances the overall capacity of the composite electrodes. Consequently, the Si-MO composite electrode exhibits a reversible specific capacity of 1300 mAh g-1 at 420 mA g-1 and remarkable cycling performance with a specific capacity of 830 mAh g-1 after 500 cycles. In particular, a reversible specific capacity of 837 mAh g-1 at 4200 mA g-1 is achieved and remains stable during 200 cycles. This work provides a potentially feasible way to achieve the Si-based anode commercialization for LIBs.

The ultra-high nickel-layered cathodes(Ni ≥ 90％)has garnered significant attention due to its high specific capacity.However,the widespread application of ultra-high nickel-layered cathodes still suffers limitation by structural instability and poor rate performance.Herein,a crystal-face-induced strategy is proposed to enhance rate and cycling performances of the electrode by constructing rapid Li+diffusion channel and reducing internal grain boundaries of secondary particles.The crystal-face-induced strategy facilitates the growth of {010} lattice plane.Highly exposed {010} planes provide wide-open and unobstructed channels for Li+deintercalation/intercalation,enhances the electrode diffusion kinetics,and thus improves the electrode rate performance.In addition,this strategy promotes the primary particle growth,reduces the grain boundaries of secondary particles and mitigates the electrode/electrolyte interface side reactions,enhancing the structural stability and cycling life of the electrode.Accordingly,the modified sample achieved a reversible specific capacity of 198.3 mAh g-1 at 1 C(1 C=180 mA g-1)and maintained a capacity retention rate of 88.5％after 100 cycles,higher than that of the original sample(73.6％,146 mAh g-1).At the high rate of 5 C,it can maintain a high specific capacity of 178 mAh g-1(capacity retention rate of 99％)after 150 cycles.This work is a leap in ultra-high nickel-layered cathodes development and provides insights into the design of electrode materials for other batteries.

Silicon is a promising anode material for lithium-ion batteries（LIBs） due to its high theoretical capacity, low discharge potential, environmental friendliness and cost-effectiveness. However, its low conductivity, high volume variation and poor cycling performance hamper its practical application. Herein, we prepare Si-Al（Al N）composite film anodes containing a nitrided aluminum metal conductive skeleton. The Al（Al N） creates a multiphase interface, buffers the volume expansion of the electrode, and also plays a role in conducting electricity and supporting the electrode structure. As a result, the Si-Al（Al N） electrode exhibits excellent performance with a high initial coulombic efficiency of 86 %, an outstanding cycling stability of roughly 1955 m Ah g -1 after 200 cycles at420 m A g -1 and retains 916 m Ah g -1 after 300 cycles even at 4200 m A g -1 （the capacity retention rate of 83 %）.This work provides an effective method for adjusting anode performance with greater freedom.