As demand grows for high-capacity batteries in electric vehicles, unmanned aerial vehicles, and energy-storage systems, cell sizes have increased accordingly. However, the conventional large-sized parallel configuration suffers from polarization due to the uneven potential distribution, particularly near tab and edge regions. To address this, bipolar stack designs with serial anode/cathode connections offer a promising solution for achieving uniform electrochemical reactions and high-power performance. In this study, a bipolar stack battery incorporating a quasi-solid-state gel polymer electrolyte (GPE) is successfully demonstrated, enabled by an effective edge-masking electrode sealing strategy to prevent shunt current between adjacent stacks. To enhance the oxidative stability of the GPE, we design a novel copolymer based on poly(ethylene glycol) diacrylate (PEGDA) and 2-(perfluorohexyl) ethyl acrylate (C6FA), and its molecular-level stability is investigated through density functional theory calculations. The quasi-solid-state 5-stack bipolar Li||NCM90 battery demonstrates 85.9 % capacity retention after 100 cycles and delivers an output voltage five times higher than that of a single cell, while maintaining non-flammability even under a nail penetration test. This novel design demonstrates the feasibility of bipolar stacking for Li-metal and Li-ion batteries using a quasi-solid-state GPE, enabling higher energy density, increased output voltage, and enhanced safety.

All-solid-state batteries (ASSBs) employing sulfide solid electrolytes (SEs) are widely recognized as promising candidates for future energy storage owing to their excellent ionic conductivity, facile processability, and compatibility with high-energy electrodes. When integrated with Ni-rich layered oxides and Li metal, sulfide SEs enable energy densities and safety margins beyond those of conventional lithium-ion batteries. Yet their practical application is hindered by complex electrochemo-mechanical degradation that originates from intertwined electrochemical reactions and mechanical instability. Electrochemical reactions such as SE oxidation and interfacial decomposition can both induce and be exacerbated by mechanical degradation, e.g., active material cracking and interfacial contact loss. These coupled processes highlight that sustainable interfacial stability is not simply a matter of chemical passivation or mechanical reinforcement, but requires strategies that address both issues simultaneously. In this Feature Article, we review the origins and evolution of electrochemo-mechanical degradation in sulfide-based ASSBs, elucidate its detrimental impact on cell performance, and propose potential strategies for its mitigation. By providing a unified view of electrochemo-mechanical challenges, this work outlines a roadmap toward practical and reliable sulfide-based ASSBs.

All-solid-state batteries employing sulfide solid electrolytes promise high energy density and safety but suffer from poor cycling stability and rate performance due to fundamental shortcomings in composite electrode architectures. To address challenges, this study introduces bimodal composite cathodes formed by blending large polycrystalline and small single-crystalline cathode active materials (CAMs). This bimodal configuration optimizes particle packing and porosity, thereby reducing ionic tortuosity and enhancing Li+ transport. At an extreme CAM loading of 90 wt%, a bimodal composition with a 7:3 mass ratio of polycrystalline to single-crystalline CAM exhibited enhanced rate performance and 87.8% capacity retention after 200 cycles, outperforming unimodal composite cathodes. Distribution-of-relaxation-times analysis, operando X-ray diffraction, operando electrochemical pressiometry, and three-dimensional simulations revealed that the enhanced mechanical performance of densely packed electrode structures originates not from stress relaxation but from uniform stress dispersion. These findings establish a comprehensive framework for advancing the design and optimization of complex composite cathodes.

Practical implementation of Li metal anodes has been hindered by non-uniform, dendritic growth of Li, which causes continuous side reactions, internal short-circuiting, and early cell failure. Although applying external pressure has been reported to promote dense Li plating to some extent, the practical application of this approach remains limited. Herein, a carbon framework-integrated separator to regulate the plating-stripping behavior of Li at reduced external pressure is proposed. To ensure both high porosity and mechanical integrity, carbon nanofibers (CNFs) are employed as a model material for realizing the framework-integrated separator structure. CNFs are electrophoretically deposited onto the separator to achieve a uniform and mechanically robust layer, while preserving the intrinsic porous structure of the separator. Combined experimental and computational studies show that when assembled with a Li metal anode, the carbon framework-integrated separator enables kinetics-controlled "in-cavity" deposition, effectively guiding dense Li plating and accommodating plating-induced volume changes. As a result, a high-voltage (4.25 V) and high-capacity (4.0 mAh cm-2) full cell exhibits stable cycling under low external pressure (0.26 MPa). This work provides a promising strategy for designing functional separators to realize practical high-energy-density Li metal batteries.

To accommodate the escalating demand for high-energy-density batteries, Li metal has received considerable attention as a promising anode material owing to its low electrochemical potential and high specific capacity. Despite their desirable characteristics, the practical applications of Li metal anodes have been hindered by remaining issues that cause early cell failure and hazardous thermal runaway, such as the growth of Li dendrites and large volume changes during battery cycling. Three-dimensional (3D) porous framework electrodes capable of hosting Li metal in their free spaces have been studied to resolve the technical issues associated with Li metal anodes. However, 3D framework electrodes still suffer from uneven Li plating: namely, Li preferentially nucleates and grows on top of the framework electrode. In contrast to the general expectations, therefore, the 3D framework electrodes tend to exhibit poor cycling stability and early cell failure. This talk deals with multiple reaction kinetics of Li plating in 3D framework electrodes, which provides a critical scientific foundation for developing a strategy to resolve top growth problems. A combined modeling and experimental study on a model architecture is presented to demonstrate the manipulation of the Li storage behavior in the 3D framework electrode via microstructural and interfacial engineering. Then, an effective strategy is proposed to design reversible framework electrodes, followed by the introduction of exemplary studies on porous carbon electrodes for practical applications in Li metal batteries.

Dry coating of solid electrolytes (SEs) onto cathode materials is a promising strategy for promoting homogeneous interfacial reactions in all-solid-state batteries (ASSBs). While electrochemical properties are considered a key criterion, the coating process fundamentally depends on the mechanics of SE particles. Herein, we demonstrate that the mechanical properties of sulfide SEs govern coating quality and, consequently, the performance of ASSB cathodes. Argyrodites with controlled Cl/Br compositions are synthesized to tune their electrochemical and mechanical properties. Atomic force microscopy-based force spectroscopy and nanoindentation measurements reveal that halogen substitution systematically governs the Young's modulus, yield strength, and adhesion energy in accordance with the nature of the halogen substituent and compositional ratio. Quantitative analysis of unbound SE fragments shows a strong correlation between the mechanical parameters and coating quality. Finite element method simulations indicate that particle fracture occurs readily, suggesting that fracture is unlikely to be a limiting factor, while density functional theory calculations identify interfacial adhesion as the key factor governing coating quality. Electrochemical analysis combined with ultraviolet photoelectron spectroscopy suggests that coating quality, beyond ionic conductivity and oxidative stability, critically governs interfacial kinetics. Accordingly, Li5.4PS4.4Cl0.8Br0.8-coated LiNi0.8Co0.1Mn0.1O2 (NCM) exhibits superior coating quality and reduced interfacial resistance, resulting in enhanced capacity and cycle stability compared to Li6PS5Cl0.5Br0.5-coated NCM. This study offers a design guideline for high-performance ASSBs through mechanical tuning of coating materials.

Sulfide-based all-solid-state lithium-metal batteries (ASSLMBs) offer enhanced safety compared to conventional liquid electrolyte systems. However, fast and stable cycling remains challenging due to dendrite growth and the formation of resistive by-products at multi-layer interfaces. Here, we propose a site-specific electrolyte customization strategy to enable high-rate stable operation through sequential modifications of the composite cathode, separator layer, and Li-metal interface. Oxygen-substituted argyrodite (Li6PS4OCl) synthesized via highenergy ball milling serves as the catholyte for Ni-rich cathodes, exhibiting superior oxidative and interfacial stability compared to conventional Li6PS5Cl, as confirmed by impedance spectroscopy and X-ray photoelectron spectroscopy. A comparative analysis reveals that Cl-rich Li5.4PS4.4Cl1.6 becomes critical for the separator at rates above 1C, where ionic conductivity limits the cell performance. A mixed solid electrolyte interlayer combining Li5.4PS4.4Cl1.6 and Li6PS4OCl at the Li-metal anode provides high ionic conductivity while promoting the formation of a robust Li3PO4-based interphase, establishing a dendrite-tolerant interface confirmed by microstructural characterizations. The optimized ASSLMB demonstrates stable cycling over 500 cycles at 1C under controlled conditions (20 MPa, 45 degrees C) without short-circuiting, while also sustaining over 100 cycles at room temperature. The design principles presented in this research provide valuable insights into critical factors for developing high-performance ASSLMBs with increased energy density and long cycle life.

Despite the rapid growth of the electric vehicle market, the long charging time of commercial Li-ion batteries (LIBs) remains a major obstacle to expanding customer acceptance of electric vehicles. However, the realization of fast-charging LIBs has been hindered by Li plating on the anode surface, which causes severe capacity decay and raises safety concerns. For safe utilization of fast-charging LIBs, in this study, we present an electrochemical method for determining Li plating-induced degradation based on the transient cell current during constantvoltage (CV) charging. A three-dimensional electrochemical model with a stochastically generated anode is constructed and utilized to find any characteristic signals specific to Li plating under fast-charging conditions. The electrochemical modeling shows that after high-rate charging, a potential variation over a plateau region in the potential profile during CV charging causes the appearance of an inflection point in the current profile, which can be characterized as a peak in the differential current profile. In case that Li plating proceeds continuously on the anode, thus consuming active Li and blocking Li+ transport, the characteristic peak in the differential current profile shifts gradually toward a higher normalized CV capacity. Based on computational and experimental studies, we confirm that the characteristic electrochemical signal can be used to in-situ monitor the Li platinginduced degradation during fast-charging cycling, which is distinguished from the degradation due to the loss of cathode active materials. This study provides an effective strategy for developing diagnostic methods to analyze degradation behaviors of fast-charging LIBs.

A duplex electrode architecture (double-layer electrode, DLE) is constructed to alleviate concentration polarization during the lithiation of the negative electrode. A smaller local voltage deviation in the electrode after lithiation and a reduced probability of Li plating on the top surface of the electrode during high-current-density applications are benefits of the modulated tortuosity and porosity of the upper electrode layer. By reducing the Li-ion concentration polarization in the DLE, the delivered capacity at the C-rate charging step is significantly increased; consequently, the quick charge cycleability is improved. The electrode thickness after cycling and the degree of failure of the electrode due to Li plating and polarization growth were reduced by the uniform utilization of the active materials in the DLE. Given the alleviated concentration polarization after lithiation, the DLE structure exhibited promising electrochemical characteristics that significantly improved its quick-charging performance.

Stack pressure significantly influences the performance of pouch type batteries, particularly those experiencing substantial volume changes, such as Li-metal batteries (LMBs). To gain a deeper understanding of the effects of pressure, it is important to examine how varying pressure conditions influence cell behavior and overall performance. In this study, Li||LiNi0.90Co0.05Mn0.05O2 (Li||NCM90) pouch cells is constrained by static or springbased adjustable-tension compression jigs at initial pressures of 0.25, 0.78, and 1.4 MPa. A novel in situ cellswelling measurement system is employed to capture real-time pressure distribution on the Li metal surface during cycling, providing unique insights into pressure-induced electrochemical "hotspots." This approach leverages mechanical compression to achieve uniform pressure distributions and promote homogeneous electrochemical reactions across the electrode. Furthermore, COMSOL simulations are used to analyze the uniformity of pressure distribution and the deformation of the separator's pore structure at different pressure levels, offering a comprehensive understanding of the pressure-performance relationship. Overall, this study presents a novel perspective on the critical role of pressure in mitigating cell degradation and improving the performance of lithium metal batteries.

Severe interfacial degradation occurs in sulfide-based all-solid-state batteries (ASSBs) at high voltages, due to the parasitic reaction between the solid electrolyte (SE) and Ni-rich layered oxide. Herein, we show that a conformal nanoscale coating of Li6PS5Cl (LPSCl) on LiNi0.8Co0.1Mn0.1O2 (NCM) promotes the homogeneous parasitic reaction and improves the high-voltage stability, enabling durable cell operation, even after extended storage at 4.25 V vs. Li/Li+.

During fast-charging, uneven lithium plating on the surface of commercial graphite anode impedes the electrochemical performance of lithium-ion batteries, causing a safety issue. The formation of a passivation layer, the solid-electrolyte interphase (SEI), due to side reactions with the organic electrolyte, correlates with long-term cycling performance under fast-charging conditions, necessitating comprehensive analysis. Herein, it is demonstrated that a molybdenum disulfide (MoS2) coating on natural graphite (NG) modulates the properties of the SEI layer, enabling reduction of the charging time and the enhancement of long-term cycling performance. MoS2 spontaneously transforms into Li2S and Mo nanoclusters through intercalation and conversion with Li+, altering the chemical composition and stability of the SEI layer on the NG, promoting faster Li+ transport, and reducing interfacial resistance. The MoS2-NG anode shows improved fast-charging capability and cycling performance under 3.0 C-charging and 1.0 C-discharging over 300 cycles without compromising energy density. In the full-cell configuration, a charging time of 14.7 min at 80% state of charge is achieved, making it suitable for electric vehicle applications.

Li ion batteries, widely used in electric vehicles and portable electronics, are now confronting theoretical thresholds in energy density due to low specific capacity of graphite anodes. One promising approach to boost energy density (> 400 Wh kg −1 ) is Li metal batteries (LMBs) paired with commercially available Ni-rich cathodes (LiNi x M 1−x O 2 , M=Mn, Co and x ≥ 0.6). Li metal anodes (LMAs) are regarded as an attractive candidate for next-generation anodes for high-energy-density energy storage because of their high specific capacity (3860 mAh g −1 ) and low electrochemical potential (−3.04 V vs. standard hydrogen electrode). However, the practical deployment of LMAs is hindered by their intrinsic high reactivity and uncontrollable growth of Li dendrites, which consequently lead to excessive parasitic reactions and short lifespan of batteries. Recent studies have demonstrated that applying external mechanical pressures to LMAs effectively suppresses dendritic Li growth, promoting dense and uniform Li deposition. Nevertheless, excessively high pressures (>10 MPa) inevitably lead to detrimental effects such as pore collapse in polyolefin separators and even mechanical tearing, ultimately causing internal short circuits. Three-dimensional (3D) frameworks, which have been extensively studied to resolve the critical issues of LMAs, can improve the cell performance of LMBs under low-pressure operation by providing abundant pore volume to accommodate volume expansion and regulate Li deposition behavior. Herein, we present a porous 3D framework of vapor-grown carbon fibers (VGCFs) integrated with the separator via electrophoretic deposition (EPD) to guide uniform Li + flux. By optimizing the EPD parameters, a mechanically robust and uniformly porous VGCF layer is combined with a commercial polypropylene (PP) separator. 3D electrochemical simulations reveal that the abundant Li⁺ transport pathways in the VGCF layer enable homogeneous Li⁺ distribution, which could inhibit formation and growth of Li dendrites. This prediction is validated through microstructural analysis of Li deposition, which confirms that Li metal is densely and uniformly deposited within the VGCF layer, gradually filling the pores in the framework from bottom to top. Electrochemical properties under reduced external pressure conditions further confirm the efficacy of the VGCF-integrated separator. Compared to bare PP, symmetric cells and half cells with VGCF-integrated separators exhibit more stable Li plating/stripping, featuring reduced hysteresis and improved reversibility. Notably, full cell employing high-voltage NCM cathode and VGCF-integrated separator maintains a capacity retention of 87.3% after 200 cycles, outperforming cells using bare PP. These results demonstrate that the VGCF-integrated separator enables reliable operation of LMBs under practical low-pressure conditions. This work provides a new approach for the design of advanced 3D frameworks for high-energy-density LMBs.for the design of advanced 3D frameworks for high-energy-density LMBs.

Anode-less all-solid-state batteries (ASSBs) with thin interlayers have emerged as a promising solution capable of addressing the dendrite issues of Li metal anodes and considerably enhancing the energy density. However, only a few studies have investigated the calendar life of anode-free ASSBs. Herein, we reveal the degradation of an anode-less ASSB with a LiNi0.88Co0.09Al0.03O2 (NCA) cathode, a Li6PS5Cl (LPSCl) electrolyte, and an Ag-C interlayer during storage and provide mechanistic insights into the possible calendar aging process. The cell shows a decline in discharge capacity after long-term storage, depending on the storage conditions and, more importantly, exhibits the reduced capacity retention upon subsequent cycling. No microstructural and electrochemical degradation is observed on the anode side; however, the composite cathode stored at a high state of charge (SOC) suffers from severe degradation upon storage. In-depth chemical and structural analyses, coupled with impedance decoupling, reveal that the high-SOC storage facilitates the detrimental interfacial side reactions between NCA and LPSCl, which are accelerated at elevated temperatures. As a strategy to address this issue, we further demonstrate that increasing the external pressure to tens of MPa during storage facilitates the chemical lithiation of NCA, which can effectively alleviate the calendar aging of anode-less ASSBs.

The sectional utilization of the Si negative electrode resulted from the appropriate physical treatment of the pouch cell based on the distribution of electrical resistance. Active materials loaded near the tab have low electrical resistance, leading to a higher degree of lithiation in the Si near the tab. This localized utilization in large pouch cells causes significant polarization growth of the electrode due to mechanical and interphasial degradation. In contrast, the active material loaded farther from the tab does not participate in the electrochemical reaction due to its high electrical resistance. Li plating on near-tab-loaded particles arises from the inhomogeneous failure of the Si negative electrode in a large electrode, causing abrupt discharge capacity fading after cycling. However, the application of external pressure increases the overpotential of near-tab-loaded active materials by constraining their volumetric expansion. Therefore, applying external pressure equalizes the Si utilization across the pouch cell footprint through external stress-induced overpotential modulation, thereby mitigating the sectional failure of the Si negative electrode.

All-solid-state batteries (ASSBs) employing composite electrodes require a significant fraction of heavy solid electrolytes (SEs), which poses a challenge to improving their energy density. In this context, a bimodal cathode design, incorporating mixed cathode active materials of different particle sizes, is proposed to enhance the packing density of the cathode layer. This study reveals the mechanism of fracture-induced failure in bimodal cathodes, triggered by interfacial heterogeneity, and discusses the fundamental requirements for achieving high-performance, long-cycling ASSBs. The cycling performance of polycrystalline LiNi0.88Co0.09Al0.03O2 (NCA)|Li6PS5Cl (LPSCl)|Li-In full cells is evaluated using two cathode configurations: a unimodal cathode composed solely of 3 μm polycrystalline NCA (U-NCA) and a bimodal cathode comprising a mixture of 3 and 10 μm NCA particles (B-NCA). Although B-NCA offers improved packing density and electronic conductivity, it suffers from rapid capacity decline under external pressures. Comprehensive impedance analysis and microstructural characterization combined with mechanical simulations reveal that the accelerated degradation of B-NCA arises from cracking in the larger NCA particles: the reaction heterogeneity at the NCA/LPSCl interface incurs the grain boundary damage of NCA, which is more severe in larger particles compared to smaller ones. Introducing a Li2ZrO3 nanolayer to mitigate the interfacial heterogeneity effectively prevents the mechanical failure of the NCA particles, leading to stable cycling performance with B-NCA. This study provides an in-depth understanding of the degradation characteristics of bimodal cathodes for sulfide-based ASSBs with high energy densities and elucidates the critical factors for their design.

The grain sizes of solid electrolyte interphase (SEI) and solvation structure of electrolytes can affect Li+ ion transport across SEI and control the desolvation kinetics of solvated Li+ ions during fast-charging of Li-ion batteries (LIBs). However, the impact of the geometric structure of SEI grains on the fast charging capability of LIBs is rarely examined. Here, the correlation between the SEI grain size and fast charging characteristics of cells is explored, and the desolvation kinetics is controlled by replacing the strongly binding ethylene carbonate (EC) solvent with a weakly binding nitrile-based solvent under fast charging conditions. The evolution of small grains of SEI to provide sufficient paths for Li+ ion supply can be achieved by the modification of solvation structure in the electrolyte. Additionally, the less resistive SEI composition and low viscosity of isoBN-containing electrolyte enable a more rapid charging of LiNi0.8Co0.1Mn0.1O2/graphite full cells by facilitating the SEI crossing of Li+ ions with less Li plating at a charging rate of 4 C at 25 °C. This work sheds light on solvation structure and interface engineering to enhance the fast charging cycle stability of LIBs for tailorable adoption in transportation sectors.

The continuous pursuit of batteries with higher energy densities and longer lifespans has exposed the inherent limitations of lithium-ion batteries, including their capacity ceiling and safety concerns arising from flammable liquid electrolytes. These issues have encouraged the exploration of next-generation energy storage solutions, and all-solid-state batteries (ASSBs) emerged as a promising alternative. By replacing liquid electrolytes with solid electrolytes (SEs), ASSBs offer the dual advantages of enhanced safety and the potential for higher energy density. In particular, sulfide-based ASSBs incorporating highly conductive sulfide SEs have attracted significant attention. Recently, methods to enhance the energy density of ASSBs have been extensively studied, such as reducing the thickness of the bulk electrolyte layer or incorporating high-energy-density anode materials such as Li metal and Si. Improving the energy density of the composite cathode, which accounts for the largest volume fraction in the cell, is also crucial for boosting the overall effectiveness of sulfide-based ASSBs. In this context, the bi-modal cathode design, incorporating mixed cathode active materials of different particle sizes, has been proposed to enhance the packing density of the cathode layer. In this study, we systematically investigate the degradation mechanisms of bi-modal cathodes and discuss the fundamental requirements for achieving high performance bi-modal cathodes. The cycling performances of polycrystalline LiNi 0.88 Co 0.09 Al 0.03 O 2 (NCA) | Li 6 PS 5 Cl (LPSCl) | Li-In full cells are tested using two cathode configurations: a uni-modal cathode composed solely of 3 μm polycrystalline NCA (U-NCA) and a bi-modal cathode comprising a mixture of 3 μm and 10 μm NCA particles (B-NCA). While B-NCA offers improved packing density and electronic conductivity, it exhibits rapid capacity decline after 80 cycles. Comprehensive impedance analysis and microstructural characterization reveal that the accelerated degradation in B-NCA arises from cracking in the larger NCA particles, significantly increasing the interfacial and diffusion resistances. Mechanical simulations further confirm that larger particles experience greater stress compared to smaller ones. Introducing Li 2 ZrO 3 coating layer to address the mechanical degradation of 10 μm particles results in stable cycling performance at 0.5C for over 120 cycles for B-NCA, with a significant reduction in interfacial side reactions at NCA/LPSCl interfaces and effective prevention of active material failure. This study provides an in-depth understanding of the degradation characteristics of bi-modal cathodes for sulfide-based ASSBs with high energy density and elucidates the critical factors for their design.

Despite the great potential of Li-metal anodes, the high reactivity of Li metal and dendritic Li growth hinder the stable operation of Li-metal batteries. Artificial Li protective layers have been introduced as a solution to stabilize the interface between the electrolyte and the Li-metal anode. In this study, we propose a functionally designed polymeric ionic liquid (PIL) for the interfacial stabilization of Li-metal anodes in quasi-solid-state batteries. Polycationic PILs are designed to form conductive and robust interphases at the PIL/Li while serving as an effective electrostatic shield to suppress dendrite growth. In addition to the optimized composition for facile Li+ transport kinetics in the PIL, the anion configurations in the PIL are engineered to produce highly ionic-conductive Li3N and to increase the concentration of LiF in the solid-electrolyte interphase. A PIL-coated Li-metal electrode (PIL thickness similar to 5 mu m) exhibits reduced interfacial resistance and enhanced cycling performances for the Li symmetric cell and full cell with a quasi-solid-state electrolyte and a high-loading LiNi0.8Co0.1Mn0.1O2 cathode (4 mAh cm-2). These findings provide insights into the design of protective PIL layers for constructing a stable interface between the electrolyte and the Li-metal anode.

The realization of lithium (Li) metal batteries, generally hindered by the high reactivity of Li metal with liquid electrolytes and the formation of Li dendrites, can be facilitated using solid electrolytes (SEs). Among the various types of SEs, succinonitrile (SN)-based SEs have attracted considerable attention owing to their high ionic conductivities at room temperature and oxidative stabilities at high voltages. However, the use of SN-based SEs in solid-state Li metal batteries (SSLMBs) is limited by severe side reactions (i.e., the polymerization of nitrile groups in SN catalyzed by Li metal). To overcome this problem, we propose a strategy to stabilize the interface between the Li anode and SN-based SE via a polymeric interlayer with a high salt concentration. The high salt concentration polymer (HSCP) interlayer inhibits the side reactions of SN with Li metal by blocking direct contact between them while also promoting the formation of a LiF-rich solid-electrolyte interphase (SEI), thereby mitigating the growth of Li dendrites during repeated charge-discharge cycling. The SSLMB cell assembled with the HSCP interlayer and high-voltage LiNi0.8Co0.1Mn0.1O2 cathode shows enhanced cycling performance compared to the cell with bare Li, demonstrating the beneficial role of the HSCP interlayer in stabilizing the Li/ SN-based SE interface. Hence, this study provides an essential understanding of the design and construction of stable Li metal anodes for high-performance and long-cycling SSLMBs.