Broadband multi-frequency and variable-energy absorption remain critical technical bottlenecks for electromagnetic wave absorption materials. To address this challenge, precise regulation of the frequency dispersion of impedance matching and consistent optimization in the target frequency band are essential. A strategy is proposed to construct gradient electron concentration via dual Schottky heterointerface engineering for accurate skin depth modulation and improved impedance matching, while interface relaxation is coupled with micro-nano array superstructures to enhance dispersion stability. Guided by simulated optimization of electromagnetic parameters and first-principles screened transition metal selenides, a customized broadband microwave absorption system integrating impedance optimization and polarization attenuation is successfully fabricated. Experiments show the material achieves a minimum reflection loss of -63.6 dB and an effective absorption bandwidth (EAB) of 8.36 GHz (covering X and Ku bands), outperforming mainstream absorbers. Furthermore, the EAB is extended to 13.1 GHz by constructing a gradient multi-layer periodic array. This multifunctional strategy offers new insights for developing ultra-broadband, flame-retardant, and corrosion-resistant absorbers, laying a solid foundation for practical applications. (c) 2026 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.

The severe volume expansion of bismuth (Bi) during alloying/dealloying could cause rapid capacity degradation, thereby limiting its application in sodium-ion batteries (SIBs). Herein, a "stepwise coating-thermolysis shrinkage" strategy is employed to construct Bi@C yolk-shell composites, which takes advantage of the different shrinkage behaviors between the reduced Bi core and the doublelayer phenolic-resin-derived carbon shell during carbonization. The yolk-shell architecture not only provides abundant active sites and ion-transport channels for sodium ion to enhance the sodium storage capacity, but also mitigates the substantial volume expansion of Bi during charging and discharging, thereby enhancing cycle stability. In-situ XRD demonstrates the characteristic alloying/dealloying mechanism. At room temperature, Bi@C-Void composites exhibit outstanding sodium-storage performance, including a high rate capability of 359.4 mAh g-1 at 20 A g-1 and superior cycling durability with 98.9% retention and 381.3 mAh g-1 retained after 1000 cycles at 1 A g-1. Even at low (0 degrees C) and high (60 degrees C) temperatures, Bi@C-Void composites achieve retentions of 95.9% and 91.5% after 400 cycles at 1 A g-1, respectively. Additionally, a full cell Na3V2(PO4)3 (NVP) // Bi@C-Void deliver a capacity of 101.1 mAh g-1 after 350 cycles at 0.5 A g-1. The "stepwise coating-thermolysis shrinkage" strategy could provide insights into the preparation of alloy-type anode materials for SIBs. (c) 2026 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

Aqueous zinc-sulfur batteries (ZSBs) exhibit high capacity and sustainability, but often require ZnI2 as an electrolyte additive, which introduces corrosive polyiodides (I-3(-) and I-5(-)) and leads to severe self-discharge and anode corrosion. Herein, an in situ formed organic-metal interphase (PA-Zn) is constructed on the zinc anode. The PA-Zn layer not only effectively suppresses the shuttle of iodine species but also guides uniform zinc ion deposition by reducing nucleation overpotential, enabling 3D Zn-ion diffusion, stabilizing current density, and promoting uniform zinc deposition. As a result, the symmetric cell with a PA-Zn@Zn anode achieves an ultralong cycling stability of 1000 h at 1 mA cm(-2) and 1 mAh cm(-2), together with remarkable high-current endurance of 150 h even at 5 mA cm(-2). When applied in ZSBs, Coulombic efficiency of the cell with bare Zn drops sharply after more than 50 cycles, while that of the cell with PA-Zn-modified anode remains stable. This work offers a feasible interphase engineering strategy to suppress interfacial corrosion in ZSBs, especially in electrolytes containing iodine-based additives.

The direct regeneration technology for the targeted repair of spent lithium-ion battery cathode materials represents a next-generation green recycling strategy, with Li replenishment being a key process. However, the rock salt phase on the surface of severely degraded LiNi0.5Co0.2Mn0.3O2 cathode material (S-NCM) significantly hinders the transport path of external Li+ from the surface to the bulk phase during the molten salt Li replenishment process. In this study, we employed the fast ion conductor Li2MoO4 to bridge the external lithium source and the bulk phase of S-NCM, expanding the intermediate tetrahedral channels for external Li+ entry into the bulk phase of the S-NCM. This strategy effectively reduces the energy barrier for Li replenishment and promotes the molten salt regeneration process. Subsequently, depth profiling XPS and XAFS tests demonstrated the effective repair of the structural degradation issues. Moreover, after regeneration, in-situ derived Li2MoO4 surface coating and Mo trace doping significantly enhances the structural stability and Li+ diffusion kinetics of the regenerated cathode (R-NCM). The results show that the R-NCM cathode exhibits an initial discharge capacity of 165.8 mAh g-1 at 0.1C, comparable to commercial cathodes, and demonstrates superior cycling stability (79.6 % after 200 cycles at 1C) compared to both traditional molten salt regenerated and commercial cathodes. This fast ion conductor mediated regeneration technology offers a new pathway for high-value molten salt regeneration.

Transition metal chalcogenides (TMCs) are premier candidates for pseudocapacitive energy storage but face a fundamental conflict between electrochemical activity and structural stability, governed by the intrinsic scaling relations of metal-anion bonding. Herein, using Ni0.85Se as a model system, we demonstrate an electronic-lattice dual-regulation strategy to reconcile this persistent conflict via anion vacancy engineering. The integration of synchrotron radiation characterization and density functional theory (DFT) calculations reveals that engineered selenium vacancies induce a concurrent modulation of the electronic density of states and local lattice strain. Electronically, an optimized upward shift of the Ni d-band center (from –1.31 eV to –1.24 eV) enhances the Lewis acidity of active sites, facilitating OH⁻ adsorption and enabling a kinetic transition from diffusion-controlled processes to surface-dominated pseudocapacitive behavior. Structurally, Crystal Orbital Hamilton Population (COHP) analysis reveals an intrinsic bond reinforcement mechanism, where vacancy-induced lattice contraction, characterized by Ni–Se bond shortening from 2.48 to 2.42 Å, effectively suppresses the population of destabilizing antibonding states. The significantly strengthened metal-anion bond (ICOHP increases from –0.63 to –0.69 eV/bond) creates a high energy barrier against metal dissolution. Consequently, the engineered electrode achieves an exceptional specific capacitance of 683.1 F g−1 (a 67.7% enhancement) while maintaining 80% retention over 8,000 cycles. This work establishes a rational orbital-engineering strategy to circumvent the intrinsic scaling relations, realizing concurrently active and durable TMC electrodes.

The direct utilization of magnesium (Mg) metal as the anode of Mg batteries is significantly susceptible to passivation in conventional electrolytes, which critically hinders Mg plating and stripping. To address this issue, a synergistic effect of the three-dimensional (3D) scaffolds' dispersive current strategy and the gradient conductivity artificial layer effectively promotes internal reversible Mg plating and stripping. In this study, we have synthesized 3D magnesiophilic gradient conductivity scaffolds (Sn@Ni), featuring an electronic insulation layer, uniform Mg2+transport channels, and a high specific surface area, through in situ ion-exchange reactions. It is observed that the plate-like metal chloride insulation provides the necessary potential gradient to prevent electrolyte decomposition and Mg deposition on the surface. Furthermore, the magnesiophilic metal tin (Sn) effectively lowers the nucleation barrier of Mg, enhancing the uniform diffusion of Mg. Additionally, the high specific surface area of the nickel foam skeleton effectively mitigates current density and regulates Mg deposition behavior. As a result, the Sn@Ni 3D gradient conductivity scaffolds exhibit an exceptionally low Mg nucleation overpotential (52 mV) under 500 & micro;A/cm2. Moreover, the Sn@Ni-Mg gradient conductivity anode, produced by plating Mg onto Sn@Ni, demonstrates a symmetric cell capable of sustaining an ultra-long stable reversible cycle exceeding 2800 h (5300 cycles). Full cells with Mo6S8 cathode also show an impressive capacity retention of 95.6 % after 500 cycles at 1 C. This breakthrough provides a novel approach to anode design, presenting potential advancements for next-generation Mg batteries. (c) 2026 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.

High-entropy oxides (HEOs) exhibit promising advantages for lithium-ion battery anodes due to multi-electron conversion and entropy stabilization, but are hindered by poor electronic conductivity, and insufficient rate capability. Herein, a (FeNiCuCrMn)3O4/nitrogen‐doped carbon fiber composite (NCF) is rationally designed via a synergistic strategy integrating dual-confinement and lattice carbon doping, fabricated through ultrasonic spray pyrolysis followed by electrospinning. Hollow porous (FeNiCuCrMn)3O4 microspheres, assembled from ultrafine nanoparticles, are completely encapsulated within the carbon fiber matrix, which provides both physical confinement and a 3D conductive network. Moreover, carbon atoms are incorporated into the (FeNiCuCrMn)3O4 lattice, reinforcing structural integrity, promoting charge transfer, and stabilizing Li+ adsorption. Ex situ XPS reveals reversible valence changes of Fe, Mn, Ni, and Cu upon cycling, while Cr remains inert via strong M–O–C, achieving superior cycling stability. The (FeNiCuCrMn)3O4/NCF delivers a high reversible capacity of 635.4 mAh·g-1 after 200 cycles at 200 mA·g-1 with 97.1% retention, and exhibits excellent rate capability (212 mAh·g-1 at 5 A·g-1). Density functional theory (DFT) calculations further demonstrate that carbon doping significantly enhances Li+ adsorption energy and reduces the band gap, corroborating the improved electrochemical kinetics. This work provides effective guidance for achieving high electrochemical performance HEO anodes.

The transformation from one amorphous phase to another is known as the glass-to-glass transition, which induces significant changes in the structure and properties of metallic glasses. However, the influence of this transition on the β relaxation behavior remains to be clarified. Here, based on classical molecular dynamics simulations of the Zr65Al7Fe7Co7Ni7Ag7 pseudo-high entropy alloy, we find that the as-cast sample (gA) undergoes a glass-to-glass transition upon heating at around 849 K. After isothermal annealing at 900 K, gA transforms into a new metallic glass (gB), and gB does not undergo a glass-to-glass transition upon heating. Compared to gA, gB exhibits a higher probability of Al-Al and Al-Ag bonding and a lower probability of bonding between Al and other atoms. Furthermore, gB also exhibits a more pronounced β relaxation peak and a higher characteristic temperature of β relaxation (Tβ) on the E″/E″max - T/Tα curve. By comparing the atomic mobility in gA and gB at their respective Tβ, we further demonstrate that gB contains a larger number of fast-moving atoms. This higher mobility makes a significant contribution to the more pronounced β relaxation peak observed in gB. Our findings provide a fresh perspective for utilizing the glass-to-glass transition to tune the β relaxation in metallic glasses.

Aqueous zinc-sulfur (Zn-S) batteries are regarded as highly promising energy storage systems owing to their intrinsic safety and high theoretical energy density. However, their failure mechanisms remain poorly understood and not systematically established. Herein, we reveal that battery degradation originates from the unstable inorganic solid electrolyte interphase (SEI) composed of ZnS, ZnSO3, and sulfates, which fails to withstand corrosion by iodine catalysts and hydrogen protons. A gradient organic-inorganic SEI was in situ constructed via an iodoacetamide (IAM) additive. The outer nitrogen-rich organic phase effectively suppresses interfacial corrosion, while the inner inorganic phase provides high-speed channels for electron and ion transport, ultimately enabling uniform and continuous zinc deposition. Meanwhile, the adsorbed IAM molecules synergistically homogenize the Zn2+ flux and facilitate rapid interfacial ion diffusion. Furthermore, IAM reconstructs the outer solvation sheath of Zn2+, lowering the desolvation energy barrier and further improving the reaction kinetics. As a result, the Zn-S battery achieves 75.95% capacity retention over 550 cycles (compared to only 27.26% without IAM). And even delivers an impressive specific capacity of 832 mAh/g at an ultrahigh current density of 15 A/g. This work provides a new perspective for the rational design for durable Zn-S batteries.

The energy density of layered oxides in sodium-ion batteries (SIBs) is restricted by the finite electron supply of conventional transition metal (TM) redox chemistry. Activating oxygen redox is a crucial strategy for surpassing the inherent limitation of energy density. In this work, we regulate the ionic potential via introducing cationic vacancies at TM sites to improve the oxygen redox activity in Na0.76Ni0.33Mn0.34Ti0.33O2. Cationic vacancies decrease the TM-O covalency by lowering the cationic potential, which encourages electrons to accumulate around oxygen atoms and facilitates O-O dimerization. Furthermore, the low cationic potential promotes the formation of P2/O3 biphasic configuration, which mitigates the structural degradation induced by oxygen redox, as evidenced by low volume variations of 1.12% for P2 and 0.95% for O3. Consequently, the optimized cathode Na0.76Ni0.33Mn0.34Ti0.28 square 0.05O2 achieves a remarkable capacity of 150.1 mAh g-1 and maintains a capacity retention of 92.1% over 350 cycles at 5C. Benefiting from the improved charge transfer kinetics and reduced apparent activation energy, the material also shows superior electrochemical performance across a wide temperature range (107.2 mAh g-1 at-20 degrees C; 153.4 mAh g-1 at 50 degrees C). This work offers a novel insight for achieving reversible oxygen redox and offers a feasible approach for high-energy SIBs.

Air self-charging aqueous zinc-ion batteries (AZIBs) have garnered significant attention for their integrated energy-harvesting and storage capabilities. However, their performance is often hindered by sluggish electrode reaction kinetics and restricted cation transport channels. Herein, an organic-inorganic composite cathode, 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA)@VO2, is constructed via a synergistic design strategy, in which NTCDA molecules uniformly coat and partially intercalate into the VO2 layers, thereby optimizing electron transport and ion diffusion pathways. Compared with reported organic-inorganic composite cathodes that mainly rely on inorganic additives to improve conductivity or structural stability, NTCDA@VO2 constructs an active organic-inorganic interface, in which VO2 acts as an electron donor to regulate the electronic structure of NTCDA, while its layered framework enables the ordered distribution of NTCDA molecules. Benefiting from this structural synergy, the Zn//NTCDA@VO2 battery exhibits an open-circuit voltage recovery to 1.21 V after 1 h of air exposure and delivers a high discharge capacity of 170.1 mAh g-1 at 0.2 A g-1. Experimental and theoretical analyses reveal that the carbonyl (C=O) groups serve as the main redox-active sites, participating in the cooperative insertion/extraction of Zn2+ and H+. Meanwhile, VO2 acts as an electron donor when combined with NTCDA, promoting oxygen activation and reducing the oxygen reduction reaction (ORR) energy barrier from 0.91 to 0.39 eV, thereby accelerating charge transfer and ion migration. This work elucidates the electron-ion coupling mechanism at the organic-inorganic interface regulated by the inorganic framework, providing new insights for designing efficient air self-charging energy storage systems.

Electrolytic seawater splitting is a crucial technical direction for hydrogen energy development. However, electrode corrosion induced by high-concentration chloride (Cl- ) remains a key bottleneck restricting its largescale application. Though cobalt-iron layered double hydroxide (CoFe-LDH) has good intrinsic catalytic activity, it is susceptible to Cl- corrosion, leading to degraded catalytic performance. Herein, this study proposes a research strategy for synthesizing tetraborate ion (B4O72- ) intercalation and regulated CoFe-LDH (CoFe-BLDH) via a one-step hydrothermal method. Via DFT calculation, In-situ Raman spectroscopy, and other characterization techniques, it was verified that the intercalation of cyclic B4O72- not only endows the catalyst with excellent hydrophilicity, promotes the generation of high-valent active species and regulates electron transfer, but also effectively inhibits the competitive adsorption of Cl-through a unique charge repulsion effect. In an alkaline high-chloride environment (1.0 M KOH + 2.0 M NaCl), this material exhibits remarkable catalytic activity with dual functional properties: oxygen evolution reaction (OER): 284 mV@100 mA cm- 2; hydrogen evolution reaction (HER): 179 mV@10 mA cm- 2, representing activity improvements of approximately 21.6% and 11.8%. The overall water splitting constructed with CoFe-BLDH delivers a current flux of 100 mA cm- 2 at a working voltage of only 1.820 V in a harsh high-chloride system and can exhibit stable performance for more than 100 h. This study provides practical theoretical guidance for improving the performance of layered double hydroxides in high-chloride media.

O3-type layered oxides are prone to severe structural distortion and irreversible phase transitions during deep Na+ deintercalation/intercalation, leading to rapid capacity decay and thus limiting their practical application. Herein, a lattice-doping strategy is employed to synthesize an O3-type cathode, Na0.93Ni0.37Mn0.49Cu0.13Sb0.01O2, with pronounced low-strain behavior. At 1C, the material exhibits excellent cycling stability, retaining 92.6% of its capacity after 200 cycles. In addition, it delivers a discharge capacity of 96.2 mAh g-1 at 5C, corresponding to 84.9% of its 1C capacity, and maintains 91.0% capacity retention after 200 cycles at this rate. In situ XRD combined with Rietveld refinement reveals that the unit-cell volume variation of NNMCS during cycling is only 0.34%, indicating highly reversible phase evolution with minimal lattice strain. The superior electrochemical performance is attributed to local structural/electronic reconstruction within the transition-metal layer induced by Cu/Sb codoping. XPS and XAFS analyses demonstrate that Cu/Sb codoping increases the average Mn oxidation state and induces local coordination rearrangement around Mn, leading to the formation of a low-coordination configuration. This structural feature effectively mitigates lattice distortion, suppresses irreversible structural evolution during cycling, and promotes the synergistic optimization of Na+ transport kinetics and structural stability. This work provides useful insight into the design of high-performance and long-lifetime layered cathodes for sodium-ion batteries.

Layered VOPO4.2H2O (VOP) cathodes exhibit promising advantages for aqueous zinc-ion capacitors (ZICs) but hindered by inferior structural stability and poor bulk conductivity. Herein, a PEDOT-VOPO4.2H2O (PEDOTVOP) cathode has been developed, achieving an enlarged interlayer spacing of 9.7 & Aring; (compared to 7.4 & Aring; for single VOP) through effective polymer intercalation. The it-conjugated chain of PEDOT forms a delocalized hybrid state with the orbitals of vanadium, introducing asymmetrical spin polarization and thereby enhancing the intrinsic electronic conductivity of VOP. Furthermore, the PEDOT insertion modifies the local crystal field symmetry of VOP, resulting in the reorganization of orbital splitting energy levels. This significantly modifies the bond strength between V and O by altering the original [VO6] octahedral structure into a distorted VO5 pyramidal structure, which in turn enhances structural stability. Consequently, the PEDOT-VOP cathode demonstrates a specific capacity of 512.7 mAh g- 1 at a wide potential window of 1.5 V in aqueous electrolyte under a current density of 1 A g- 1. In-situ Raman and XRD analysis confirm the excellent reversibility and long-term stability of the cathode, with 88 % of its initial capacity retained over 10,000 cycles. This study provides profound insights into the development of high-voltage, stable, and high-capacity cathode materials for ZICs by modulating the electronic structure through enhanced spin polarization of d-orbitals.

Layered oxides are considered the most promising cathode materials for sodium-ion batteries. However, their structural degradation triggered by irreversible oxygen redox remains a major obstacle. In this work, the localized electronic structure of the Na0.76Ni0.33Mn0.67O2 cathode was regulated through Ca/Ti incorporation to suppress irreversible oxygen redox. The optimized P2/O3-Na0.76Ca0.05Ni0.33Mn0.34Ti0.33O2 cathode achieves an excellent cycling stability (capacity retention of 83.4% after 500 cycles at 5C; capacity retention of 80.3% after 200 cycles at 1C). The Ca/Ti co-substitution strengthens the bond energies of metal-oxygen and metal-metal, while inducing the formation of P2/O3 biphasic configuration. Furthermore, in-situ XRD confirms the “near-zero-strain” characteristic of the optimized material with a low volume change rate of 1.00% for the P2 phase and 2.79% for O3 phase. In-situ Raman and ex-situ XPS demonstrate that the formation of reactive peroxo-like (O2)n- species is inhibited during cycling. This localized electronic structure modulation effectively reduces the formation of unhybridized O 2p states and enhances orbital hybridization, thereby mitigating undesired oxygen redox. The P2/O3 biphasic structure can alleviate bulk strain and avoid structural cracking caused during cycling. This work provides a design strategy for high-voltage layered oxide cathodes through biphasic engineering and localized electronic structure modulation.

High-valent-element doping has emerged as a key upcycling strategy for achieving a stable Ni-rich regenerated cathode. However, on the surface of the spent Ni-rich cathode LiNi0.8Co0.1Mn0.1O2 (SNCM), the scarcity of transition-metal (TM) vacancies and the strong electrostatic repulsion within the central tetrahedral channels with more than two face-sharing TM ions in the rock-salt phase hinder the diffusion of Li+ and high-valent dopants into the bulk lattice. This results in a slow Li replenishment rate and is ineffective in stabilizing the bulk lattice. Here, this work selectively etches the rock-salt phase on the SNCM surface via a preferential coordination reaction between Ni2+ and ammonia. This creates defect-rich microenvironments with a layered structure featuring significantly reduced electrostatic repulsion and abundant TM/oxygen vacancies, which provide low-energy pathways for ion migration and additional sites for dopant incorporation. Compared to conventional strategies, this method shortens the sintering time by 40%. The regenerated Mo-doped cathode exhibits high bulk doping concentration and excellent capacity retention (88.7% after 200 cycles at 1 C). The assembled full cell maintains 75.4% capacity after 800 cycles. This work provides a simple, scalable strategy for upcycling spent Ni-rich cathodes.

Aqueous zinc-ion batteries (AZIBs) have emerged as promising candidates for next-generation energy storage systems due to their inherent safety, environmental friendliness, and low cost. However, the cycling durability remains significantly constrained by the uncontrolled growth of zinc dendrites and the parasitic hydrogen evolution reaction (HER). Herein, dicyandiamide (Dcd) is introduced to regulate interfacial chemistry of zinc anodes by molecular anchoring. The highly polar amino groups anchor Dcd at the interface, facilitating the rapid transport of Zn2+ and inducing the uniform deposition. Simultaneously, the terminal cyano groups modify the solvation structure of Zn2+ and inhibit the activity of water, effectively suppressing interfacial side reactions. Driven by the synergistic interaction of the two functional groups, the zinc anode demonstrates an extended cycling lifespan exceeding 1200 h at 1.0 mA cm-2 and maintains stable performance for 100 h under an ultrahigh current density of 20 mA cm- 2, while Zn-Cu half cells exhibit over 500 cycles with high coulombic efficiency of 99.6 %. Even in the Zn||MnO2 full cell, an impressive cycling stability is achieved, with a high capacity retention of 78.21 % after 5000 cycles at 2 A g- 1. This work provides new insights into enhancing the interfacial stability of zinc anodes through low-cost multifunctional additives.

Pt-based catalysts have attracted considerable attention because of their outstanding electrocatalytic activity. However, their practical application under realistic operating conditions is still limited by the high reliance on noble-metal Pt and insufficient structural stability. Pt–TM (TM = Fe, Co, Ni, Cu, etc.) alloys are widely regarded as an effective approach to reducing Pt usage and improving ORR performance. Nevertheless, the non-noble metal components in these alloys are susceptible to dissolution and structural reconstruction in acidic media, which in turn compromises catalyst durability. In this work, PtNi alloys supported on phosphorus-doped carbon were constructed through a two-step strategy. Results show that P doping introduces abundant P-C defect sites into the carbon support, strengthens the interfacial coupling between the PtNi alloy and the support, and provides a more robust anchoring environment for the alloy nanoparticles. Meanwhile, P regulation induces a moderate compressive strain in the PtNi alloy and reconfigures its surface atomic arrangement and local electronic distribution, thereby tuning the d-band center of Pt and suppressing structural evolution during the reaction process while optimizing the adsorption behavior of oxygen intermediates. In addition, the hierarchically porous carbon framework facilitates mass transport and exerts a certain spatial confinement effect on the PtNi nanoparticles, further favoring the maintenance of a stable interfacial environment. Among the as-prepared catalysts, PtNi/PC-2 exhibits excellent ORR activity and durability, delivering a mass activity of 0.42 A mgPt-1 at 0.8 V, which is 6.3 times that of Pt/C. After 10,000 accelerated durability test cycles, the half-wave potential of PtNi/PC-2 decreases by only 12 mV, markedly outperforming Pt/C.

The crystallographic orientation of magnesium deposition is closely related to interfacial interactions between the substrate and deposited metal, which critically influences the morphology evolution and reversibility of magnesium metal anodes. Herein, vertically aligned nickel phosphide nanoarrays grown on nickel foam (Ni2P@NF) are constructed to regulate the nucleation and growth behavior of magnesium at the electrode-electrolyte interface. Density functional theory calculations reveal that the Mg (002)/Ni2P interface possesses the lowest interfacial formation energy and favorable adsorption characteristics, enabling preferential Mg nucleation along the thermodynamically favorable Mg (002) plane. The low lattice mismatch between Mg and Ni2P further promotes the epitaxial growth of Mg (002), achieving a smooth and dense magnesium deposition layer. Experimental observations confirm that magnesium deposition on Ni2P@NF exhibits highly uniform morphology and significantly improved reversibility compared with pristine NF. The Ni2P@NF electrode delivers a reduced nucleation overpotential and stable magnesium plating/stripping behavior for over 1260 h at 1 mA cm-2. Furthermore, full cells paired with a Mo6S8 cathode exhibit enhanced rate capability and long-term cycling stability. This work provides new insights into crystallographic regulation of metal deposition at heterogeneous interfaces and offers an effective strategy for stabilizing magnesium metal anodes.