Prelithiation is effective for compensating active lithium-ion (Li+) loss in silicon (Si)-based battery electrode materials. However, owing to the dynamic growth of the solid electrolyte interface (SEI), capacity fading remains the biggest challenge for the industrialization of Si electrodes. To address this problem, a novel ether-based prelithiation reagent was rationally designed by exploiting the weak solvent-solute coordination and the competitive reduction mechanism among electrolyte components. Precise regulation of the Li+ solvation structure enhanced Li+ transport during prelithiation, achieving an exceptional initial Coulombic efficiency (ICE) of similar to 100% for the Si/carbon (Si/C) anode after performing contact prelithiation for 2 min. Furthermore, the lithium fluoride (LiF)-rich interface with high mechanical toughness was pre-formed to assist in the formation of a stable SEI film by controlling the lowest unoccupied molecular orbital (LUMO) energy and binding energy of the prelithiation reagent, thereby improving the half-cell cycle performance. Consequently, the ICE of the full-cell incorporating the prelithiated Si/C anode increased by 40% compared with that containing as-received materials, and the corresponding energy density was 551.2 Wh kg-1 based on the electrode material after 3 cycles. Furthermore, theoretical calculations combined with in situ characterization techniques confirmed the strong potential of the contact prelithiation design strategy for large-scale industrial applications. (sic)(sic)(sic)(sic)(sic)(sic)(sic) (Si) (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) (Li+) (sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) (SEI) (sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)Si(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)-(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)Li+(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic) (Si/C) (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)100%(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) (ICE) .(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) (LUMO) (sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) (LiF) (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)SEI(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)Si/C(sic)(sic)(sic)(sic)(sic)(sic)(sic)ICE(sic)(sic)(sic)40%, (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)551.2 Wh kg-1 ((sic)(sic)(sic)(sic)(sic)) .(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)Si/C(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).

Iron oxyfluoride (FeOF), as a conversion-type cathode material, offers higher theoretical capacity and energy density than traditional intercalation-type cathodes owing to multi-electron transfer reactions. However, its practical application in all-solid-state lithium batteries (ASSLBs) is hindered by poor intrinsic ionic/electronic conductivity, sluggish reaction kinetics, and reaction-induced mechanical degradation, while most previous studies have mainly focused on liquid-electrolyte systems. Here, aliovalent Ni2+ doping is employed to regulate the defect chemistry and ion/electron transport properties of FeOF. Experimental and theoretical results show that Ni2+ incorporation modifies the local electronic structure and defect environment, thereby enhancing electronic conductivity and facilitating Li+ migration. The improved mixed transport and reduced reaction-induced volume changes promote spatially uniform reactions and mitigate local stress accumulation, thereby preserving solid–solid interfacial contact during cycling. Consequently, the FeOF-Ni3 cathode delivers a high-rate capacity of 319 mAh g−1 at 3 C, 75% capacity retention after 1000 cycles at 2 C, and a high energy density of 1320 Wh kg−1 at 0.2 C based on the active material. This work demonstrates that atomic-scale defect regulation can simultaneously improve transport kinetics and chemo-mechanical stability of conversion-type cathodes for high-energy-density ASSLBs.

Iron-based mixed phosphate Na4Fe3(PO4)2P2O7 (NFPP) is one of the most promising cathodes for sodium-ion batteries due to its good rate capability and long lifespan, while its practical application is hindered by sluggish ionic/electronic kinetics and interfacial instability. Herein, we report a novel solid-source ammonium fluoride (NH4F) plasma-driven synergistic "Trinity" engineering strategy to realize simultaneous reconstruction of NFPP cathodes in bulk, interface, and surface architectures. Mechanistic investigations reveal that the coupling reactions between the NH4F plasma and NFPP lattice/surface trigger simultaneous bulk F-substitution and F/N interface doping as well as surface reconstruction. Specifically, the bulk F- substitution strengthens Fe─O bonding and widens Na+ channels. Concurrently, plasma-generated radicals promote the formation of F/N co-doped carbon network and NaF at the interface, while also promoting the development of a NaF-rich cathode electrolyte interphase at the surface via modulating the NFPP/electrolyte status. This trinity engineering establishes fast transport pathways and a stable cathode electrolyte interface, effectively minimizing charge transfer impedance while suppressing deleterious side reactions. Consequently, the optimized cell exhibits high capacity and superior high-rate cycling life with 95.5% retention after 6000 cycles at 30 C. The developed plasma-driven approach offers mechanistic insights for the synergistic optimization of polyanionic cathodes for advanced sodium ion storage.

Sulfide-based solid-state electrolytes (SSEs) are attractive candidates for high-energy all-solid-state lithium-ion batteries due to their high ionic conductivity. However, the intrinsic chemical instability against Li metal leads to continuous interfacial degradation. Herein, we design a gradient hybrid electrolyte by introducing a borohydride-based interfacial buffer to achieve complete anode-electrolyte isolation without sacrificing energy density. The borohydride component, with its intrinsic reducibility and deformability, facilitates the formation of a stable solid electrolyte interphase (SEI) while maintaining ionic transport comparable to pristine sulfide SSEs. Benefiting from this interfacial stabilization, the hybrid SSE enables long-term cycling over 2000 h and delivers a high specific capacity of 516.3 mAh g(-1) at 10 C with selenium cathode featuring dual-electron reactions. This study demonstrates that borohydride-mediated interfaces effectively suppress parasitic reactions and provide a universal and scalable strategy to unlock the potential of sulfide-based solid-state batteries.

Ta-doped garnet Li7-xLa3Zr2-xTaxO12 (LLZTO) solid electrolytes are emerging as a premier oxide electrolyte, however, its practical application is hindered by surface Li2CO3 inert layers and poor electrode compatibility. Herein, we report a novel and efficient solid-source ammonium fluoride plasma method to modify the surface of LLZTO to address its interfacial challenges. The synergistic modification via NH4F plasma achieves one-step conversion of Li2CO3 into beneficial LiF/Li3N composite interphase layer on LLZTO in several minutes. The formation mechanism of dual-phase LiF/Li3N layer is due to coupling reactions between Li2CO3 and F-and Nx-radicals from NH4F plasma. This synergistic design not only eliminates the Li2CO3 inert layer, but also simultaneously optimizes interfacial wettability, minimizes impedance, and reinforces mechanical integrity, supported by theoretical calculations. The plasma modification also activates LLZTO lattices with increased room-temperature ionic conductivity from 6 & times; 10-4 to 7.6 & times; 10-4 S cm-1. Consequently, symmetric cells assembled with the modified LLZTO exhibit stable cycling life for 4000 h at 0.4 mA cm-2 and 0.4 mAh cm-2. Furthermore, full cells paired with LFP and NCM cathodes demonstrate enhanced rate performance and cycling stability. The developed plasma approach resolves the interfacial bottlenecks of LLZTO, offering mechanistic insights for oxide electrolyte optimization for advanced solid-state batteries.

All-solid-state lithium batteries (ASSLBs) have garnered significant attention as a next-generation energy storage technology, providing superior safety, enhanced stability, and high energy density. However, current research predominantly remains confined to laboratory-scale demonstrations, with limited translation into scalable technological solutions. Addressing this academia-industry disconnect is critical to unlocking the commercial viability of ASSLBs. This review focuses on bridging this gap by systematically analyzing advancements in solid-state electrolytes (SSEs)—the cornerstone of ASSLB technology. We delve into the structural characteristics, ion transport mechanisms, and performance metrics of various SSEs, alongside a comprehensive summary of modification strategies. Beyond theoretical advancements, we emphasize the practical implications of these strategies in addressing energy density limitations, interfacial instability, and safety concerns. A distinctive feature of this review lies in its multidimensional analysis of early-stage ASSLB industrialization hurdles, integrating perspectives from materials synthesis scalability, electrode processing innovations, device-level performance validation, advanced characterization methodologies, and application-specific requirements. This work not only maps current research frontiers but also establishes actionable guidelines for academia–industry collaboration, offering scientists a roadmap for targeted innovation and equipping enterprises with evidence-based insights to streamline technology development and commercialization strategies.

Achieving both adequate mechanical performance and pronounced energy storage functionality within inorganic construction material systems still remains a significant challenge. This study focuses on geopolymer structural capacitors. By introducing in situ foaming with H2O2 and regulating the pre-curing temperature, a structural energy storage system with controllable pore structure and gel network characteristics was constructed, with particular emphasis on elucidating the intrinsic relationships among pore structure evolution, gel polymerization behavior, and ion transport properties. The effects of different regulation pathways on the capacitive behavior and mechanical response of geopolymer structural capacitors were systematically analyzed from the perspectives of pore connectivity, gel network development, and variations in ion migration resistance. Results show that the pore structure primarily governs capacitive behavior by modulating ion migration pathways and transport resistance, whereas the development of gel network predominantly determines the mechanical stability. These two factors are coupled through temperature-driven reaction kinetics and foaming-induced pore formation processes, jointly dictating the structure-function response of geopolymer structural capacitors. Overall, this work reveals the coupled roles of pore structure and gel network evolution in simultaneously regulating ion transport behavior and mechanical performance, providing new physicochemical insights into structure-function coupling mechanisms in energy storage systems based on inorganic construction materials.

O3-type NaNi1/3Fe1/3Mn1/3O2 (NFM) is a promising cathode material for sodium-ion batteries, yet its practical application is hindered by interfacial instability during cycling and rapid surface degradation upon air exposure. These drawbacks stem from the high surface reactivity of the exposed lattice, which induces persistent parasitic reactions, excessive cathode-electrolyte interphase (CEI) formation, and sluggish Na+ transport. In this study, a low-temperature plasma-enhanced chemical vapor deposition strategy is employed to construct a NaF/C artificial CEI on NFM without altering the bulk structure. This approach achieves simultaneous surface chemical passivation and interfacial kinetic regulation. The NaF-rich phase stabilizes the CEI and facilitates Na+ migration, while the incorporated carbon ensures continuous electron conduction, collectively reducing polarization and accelerating Na+ diffusion. As a result, the modified NFM@NaF/C cathode delivers a capacity retention of 85.2% after 100 cycles at 1 C. Moreover, it retains 80% of its initial capacity even after 7 days of air exposure, demonstrating significantly enhanced structural and air stability.

Lithium-ion batteries (LIBs), as the most representative energy storage devices, have become deeply integrated into our daily lives. However, the formation of solid electrolyte interphase during the initial cycle consumes a substantial amount of lithium ions (Li+). Moreover, the continuous consumption of Li+ in subsequent cycles further shortens the lifespan of LIBs. To compensate for this irreversible lithium loss, prelithiation technology has attracted substantial attention in recent years and is now recognized as an effective strategy to boost battery performance. Among various prelithiation additives, lithium oxalate (Li2C2O4) stands out as a particularly attractive cathode prelithiation additive, owing to its low cost, excellent air stability, and the absence of solid residual by-products. To date, no systematic review has focused exclusively on Li2C2O4 as a prelithiation additive. In this review, we present a comprehensive overview of the research progress on Li2C2O4, focusing on three critical aspects: delithiation mechanism, modification strategies, and application methods. Furthermore, we discuss future directions and prospects for Li2C2O4, aiming to offer guidance for subsequent research in this field.

It is a great challenge for conventional approaches to prepare high-quality carbon coating on oxide cathodes to overcome unfavorable phase transition, lattice oxygen release and interfacial strain. Traditional high-temperature carbonization processes exacerbate the loss of lattice oxygen and reduction of highvalence metal, while low-energy routes result in nonconformal coating with low conductivity. Herein, we resolve this dilemma by developing a novel solid-source plasma technology to realize a breakthrough in high-quality N-doped carbon (NC) coating for ternary cathodes at low temperature. Typically, 2,2' bipyridyl plasma enables controllable uniform encapsulation of NC on LiNi0.8 Co0.1 Mn0.1 O2 (NCM811) at lower than 300 degrees C. The electrochemically adaptive NC layer establishes efficient conductive pathways while demonstrating exceptional mechanical flexibility. This compliant architecture likely alleviates strain coupling between Faradaic reactions and lattice stress evolution, suppressing microcrack initiation at primary particle boundaries. Additionally, synchrotron technology reveals that lattice oxygen release and phase transition can be effectively suppressed by the NC. Consequently, the modified cathode achieves a capacity retention of 92.7% after 100 cycles at 1 C and demonstrates remarkable ambient stability so that samples exposed to air for one month retain 83.7% capacity after 200 cycles at 1 C, much better than bare NCM811 (29.9%). This work establishes a new interfacial paradigm for advanced cathodes. (c) 2026 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.

Poly(ethylene oxide) (PEO) electrolytes present a promising option for next-generation solid-state highenergy-density batteries. However, the poor ionic conductivity and inefficiency transference number pose significant barriers to its broader application. Herein, an in-built synthesis of poly(ethylene oxide) with zwitterionic poly(ionic liquid) composite electrolyte (PEO/Zwit PIL) is employed by a thio-lene click reaction. The introduction of Zwit PIL can help the composite electrolyte fully dissociation lithium salts and optimize the solvation structure. Molecular dynamics simulations elucidate fast Li+ transport through a structural diffusion mechanism upon the addition of Zwit PIL to the composite electrolyte, simultaneously facilitating a high ionic conductivity and transference number. The composite electrolyte also demonstrates a high self-adhesive to construct a robust and tough electrode-electrolyte interface. The assembled full cell (LiFePO4||PEO-Zwit PIL||Li) exhibits a discharge capacity of 153 mAh/g at 60 degrees C and highly stable cyclic performance up to 200 cycles at 0.2 C. The employment of Zwit PIL within PEO for novel solid-state electrolytes furnishes an alternative approach to the design of high-performance, nextgeneration, sustainable batteries. (c) 2026 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.

Solid-state lithium metal batteries (SSLMBs) hold great promise for safe and high-energy-density storage. Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based composite polymer electrolytes (CPEs) with garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO) fillers are attractive but suffer from the detrimental Li2CO3 layer on LLZTO, which hinders ion transport and triggers polymer decomposition. Herein, we introduce a plasma-assisted strategy to in situ convert the Li2CO3 layer into a uniform 15 nm LiF coating. This LiF interphase not only mitigates the alkalinity to suppress dehydrofluorination but also promotes the transformation of PVDF-HFP from the α-phase to the electroactive β-phase, enhancing Li salt dissociation and creating robust ion transport pathways across the PVDF-HFP/LLZTO interface. Consequently, the LiF coating increases the intrinsic ionic conductivity contribution of the LLZTO filler by 12.6%–17.5% (semi-quantitative results from 6Li solid-state nuclear magnetic resonance analysis). The optimized CPE exhibits a high ionic conductivity of 6.65×10−4 S cm−1 and enables stable lithium plating/stripping for 3000 h. The corresponding SSLMB delivers excellent cyclability with 88.5% capacity retention after 140 cycles at 2 C, highlighting the efficacy of this interfacial engineering approach.

Atomically dispersed noble metal single-atoms (SAs) catalysts offer near-100% atom utilization and exceptional catalytic activity, yet achieving high loading and controlled synthesis remains challenging. Herein, we present a novel and rapid plasma technique for the simultaneous synthesis of Ru SAs anchored on cobalt nitride (Ru CoN). The uniform dispersion of Ru atoms modulates the electronic structure of CoN, promoting in situ surface reconstruction and leading to exceptional oxygen evolution reaction (OER) performance with an overpotential of only 226 mV at 10 mA cm-2 . In an alkaline anionexchange membrane water electrolyzer (AEMWE), Ru-CoN achieves 0.5 A cm-2 at 1.86 V, operating stably for over 100 hat 60 degrees C. Experimental and theoretical analyses show that Ru incorporation downshifts the Co 3d band center, upshifts the O 2p band, and enhances metal-oxygen covalency, thereby activating the lattice oxygen mechanism (LOM) and surpassing the conventional OER pathway. This work offers an efficient strategy for atomically doped, high-performance OER catalysts toward sustainable energy applications. (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.

Although microporous metal-organic frameworks (MOFs) are demonstrated to be advantageous for light hydrocarbons (HCs) separation and biogas upgradation to biomethane, 2D 'flexible-robust' MOFs can show great potential in selective capture and separation performances via the guest-dependent gate-opening phenomenon due to their ability to undergo stimulated structural transformations. Herein, we report a 2D 'flexible-robust' MOF, IITKGP-35 with phenyl ring-decorated one-dimensional microporous channels showing an impressive capability for C2s/CH4 and CO2/CH4 separations benefiting from multi-step adsorption, while maintaining tradeoff between high sorption capacity (C2 HCs and CO2) and excellent separation selectivity. Dynamic breakthrough study unveiled an impressive C2H6/CH4 and CO2/CH4 separations with the breakthrough retentions of 46.4 min g- 1 and 38.6 min g- 1 for C2H6 (with the pure CH4 productivity of 51.0 L kg- 1 for a given cycle, >= 99 % purity) and CO2 (pure CH4 productivity of 40.6 L kg- 1 for a given cycle, >= 99 % purity), respectively. The theoretical calculations revealed that the primary adsorption sites are the aromatic it surfaces, decorated within the optimal pore space, facilitating enhanced host-guest noncovalent interactions (C - H center dot center dot center dot it and it-it stacking) for C2 HCs and CO2 gas molecules.

Carbon-based supercapacitor electrodes face critical challenges, including disordered pore architecture, surface inertness, and insufficient graphitization, leading to compromised electron transport and interfacial reactivity. This study systematically investigates the effects of physical or chemical activation strategies on the structural and electrochemical properties of carbon electrode materials. Comparative analysis reveals that physical activation (N2/CO2 annealing) primarily induces partial graphitization and moderate particle refinement, while chemical activation involving melamine-assisted heteroatom doping followed by NaOH etching enables comprehensive structural reorganization. The optimized process converts the particle structure into three-dimensional interconnected porous frameworks with enhanced surface functionality. The chemically activated N doped hierarchical porous carbon frameworks (N-CNFs) exhibit (1) hierarchical porosity with optimized meso/micropore coexistence, (2) effective nitrogen incorporation generating redox-active sites, (3) improved charge transfer kinetics through structural graphitization, (4) electrochemical evaluation demonstrates exceptional performance metrics with high specific capacitance of 443 F g-1 at 1 A g-1, outstanding cycling stability with 100% capacitance retention after 10,000 cycles at 10 A g-1 and maximum energy/power density of 21.25 Wh kg-1 and 15.0 kW kg-1. This work establishes a paradigm for developing advanced carbon electrodes through coordinated microstructure engineering and surface chemistry modulation, providing critical insights into structure-property relationships for energy storage applications.

Polar solvent molecules often participate in the formation of hydrogen-bonded organic frameworks (HOFs) as building blocks, but the fragile nature of hydrogen bonds means that most HOFs collapse after activation, limiting their broad applications in gas separation. Herein, we report a strategy of solvent-induced structural rearrangement to eliminate the negative effects of polar solvent molecules for achieving efficient C2H6/C2H4 separation. Single-crystal X-ray diffraction (SCXRD) studies identified that a structural rearrangement was achieved from nonporous HOF-BPTC(MeOH) to porous ZJU-HOF-20 by soaking in low-polarity solvents such as n-hexane. This solvent-induced rearrangement not only removes the bonded methanol molecules from the framework, but also enables it to reversibly transform into a new threefold interpenetrated structure with highly enhanced framework stability. As a result, the activated ZJU-HOF-20a exhibits a largely improved BET surface area of 856 m2 g-1 compared to that of HOF-BPTC(MeOH), affording both high C2H6 uptake (2.35 mmol g-1 at 298 K and 0.5 bar) and C2H6/C2H4 selectivity (2.0). The SCXRD studies on gas-loaded ZJU-HOF-20a reveal that the inherent nonpolar pore surfaces combined with suitable pore sizes provide much stronger multipoint interactions with C2H6 than C2H4, thus accounting for the preferential binding of C2H6 over C2H4. Breakthrough experiments confirm that ZJU-HOF-20a can efficiently separate actual 50/50 and 10/90 (v/v) C2H6/C2H4 mixtures to directly produce pure C2H4, affording high C2H4 productivities of 8.3 L kg-1 and 15.7 L kg-1, respectively.

Conventional binders fail to simultaneously provide efficient ion transport channels and three-dimensional (3D) mechanically robust networks, hindering optimal prelithiation and stable solid electrolyte interphase (SEI) formation in Si anodes. This work develops a carboxymethyl cellulose (CMC)-iminodiacetic acid (IA) binder featuring a 3D covalent-hydrogen bond crosslinked network, synthesized via one-step in-situ thermal condensation to regulate ion/electron transport during contact prelithiation. The prelithiated Si electrode (p-Si@CMC-c-IA) achieves a high initial Coulombic efficiency (ICE) of 109.63 % and a reversible specific capacity of 611.5 mAh g-1 sites, which can provide a fast ion transport channel for prelithiation. Furthermore, CMC-c-IA binder can induce the decomposition of lithium salt on the surface of Si anodes to form a dense and stable LiF-rich SEI film. The full-cell with a p-Si@CMC-c-IA anode achieves a high ICE of 86.99 %, and its capacity retention rate is still as high as 91 % after 100 cycles at 0.2 C. As a result, the in-situ electrochemical stress analysis confirmed that the combination of prelithiation strategy and binder design effectively enhances both ICE and cycling stability in Si anodes. after 250 cycles at 0.5 A g-1. The main reason is that the CMC-c-IA binder has abundant Li+ complexation

The uncontrolled deposition behavior, sluggish reaction kinetics and inefficient utilization of Al derived from unstable anode/electrolyte interface have severely impeded the development of aluminum-ion batteries. Here, we discuss the impact of interfacial electron/ion transfer on the electrochemical performance, and as an illustration, propose the construction of Cu@MXene as anodic current collector through work function engineering to simultaneously achieve homogeneous deposition morphology and rapid plating/stripping rate. The difference in work function between Cu nanoparticles and Ti3C2 MXene facilitates charge redistribution in the anode/electrolyte interface and enhances the electron availability, optimizing the interfacial electron/ion transfer behavior. This, in turn, endows Cu@MXene with elevated catalytic efficiency for desolvation reactions and robust reduction ability for the Al plating process. As a result, Cu@MXene enables a high coulombic efficiency of 99.87 % even at a high current density of 10 mA cm-2, and sustains reversible Al plating/stripping cycles for over 3200 h at a typical current density of 1 mA cm-2. Notably, by coupling graphite cathode and Cu@MXene-Al anode under a limited N/P ratio of 2.2, the full cell exhibits durable lifetime for 2000 cycles with an impressive energy density of 119.6 Wh kg-1 (based on the total mass of cathode and anode). This work highlights a fundamental understanding of interfacial interactions in the Al deposition process and offer sustainability motivations in designing highly reversible anodes for high-energy-density aluminum-ion batteries.

Design and optimization of the solid electrolyte interphase (SEI) is extremely important for the construction of advanced lithium metal anodes. Herein, we pioneer a novel SnCl4/trifluorotoluene hybrid plasma technology to construct a Li-Sn alloy-based gradient SEI on lithium metal anodes to synergistically regulate reaction kinetics, structure, and crystal orientation of lithium deposition. Notably, the designed SEI displays a gradient layered structure, with a Li-Sn alloy constituting the bottom layer, LiF occupying the middle layer, and a composite layer of LiCl and organic lithium compounds forming the top layer. The formation mechanism is primarily attributed to the differential acceleration effects exerted by the plasma shell's electric field on different plasma ions. The gradient SEI exhibits multifunctionality, featuring not only high Young's modulus (13.9 GPa) and enhanced interfacial structural stability, but also enabling the Li-Sn alloy component within the SEI to facilitate the preferential growth of the (110) crystal plane with a low migration barrier, thereby achieving the uniform deposition of Li without dendrite growth. Consequently, the modified Li anode exhibits a low overpotential and high coulombic efficiency, and the corresponding pouch cell shows improved cycling stability. This research provides a pioneering interfacial modification strategy for the fabrication of high-performance lithium metal anodes.

Component leaching plays a pivotal role in enhancing the activity and stability of high-entropy-based catalysts by triggering structural reconstruction during the oxygen evolution reaction（OER）.In this study,we employed soluble V and Mo as sacrificial components alongside a Co stabilizer to synthesize NiFeCoVMo high-entropy catalysts,aiming to simultaneously modulate the reconstruction behavior and optimize catalytic performance.The synergistic interplay between dual-component dissolution and in situ deposition/adsorption mechanisms accelerates structural evolution,ultimately yielding MoO 4 2- -modified NiFeCo oxyhydroxide(NiFeCoOOH-MoO 4 2- ).Mechanistic studies reveal that the NiFeCo-based system is particularly conducive to the reconstruction process,while adsorbed MoO 4 2- function as electronic modulators that redistribute charge densities within the reconstructed layers and reduce surface energy.As a result,this reconstructed catalyst demonstrates exceptional OER activity,achieving an overpotential of 172 mV at 10 mA cm -2 ,along with remarkable long-term durability(up to500 h at 50 mA cm -2 ).This study provides fundamental insights into the origins of the superior electrocatalytic performance of high-entropy materials,paving the way for further exploration and optimization of these advanced catalysts.