Compressible and Elastic Reduced Graphene Oxide Sponge for Stable and Dendrite-Free Lithium Metal Anodes.

Dendritic Li deposition, an unstable solid-electrolyte interphase (SEI), and a nearly infinite relative volume change during cycling are three major obstacles to the practical application of Li metal batteries. Herein, we introduce a compressible and elastic reduced graphene oxide sponge (rGO-S) to simultaneously eliminate Li dendrite growth, stabilize the SEI, and accommodate the volume change. The volume change is contained by compressing and expanding the rGO-S anode, which effectively releases the Li plating-induced stress during cycling. The smooth and dense Li metal is deposited on rGO-S without dendrites, which preserves the SEI, reduces consumption of the electrolyte, and prevents the formation of Li debris. The half-cells employing rGO-S show a steady and high Coulombic efficiency. The Li@rGO-S symmetric cells demonstrate excellent cycling stability over 1200 cycles with a low overpotential. When paired with LiFePO4 (LFP), the Li@rGO-S||LFP full cells exhibit a high specific capacity (150.3 mAh g-1 at 1C), superior rate performance, and good capacity retention.

Balancing the Ion/Electron Transport of Graphite Anodes by a La-Doped TiNb2O7 Functional Coating for Fast-Charging Li-Ion Batteries.

A functional coating layer (FCL) is widely applied in fast-charging lithium-ion batteries to improve the sluggish Li+ transport kinetics of traditional graphite anodes. However, blindly increasing the Li+ conductivity for FCL reduces the overall electron conductivity of the anodes. Herein, we decoupled the effect of La-doping on TiNb2O7 (TNO) in terms of the phase evolution, Li+/electron transport, and lithiation behavior, and then proposed a promising La0.1TNO FCL with balanced Li+/electron transport for a fast-charging graphite anode. By optimizing the doping concentration of La, more holes are introduced into the TNO as electron carriers without causing lattice distortion, thus maintaining the fast Li+ diffusion channel in TNO. As a result, the graphite with La0.1TNO FCL delivers an excellent capacity of 220.2 mAh g-1 (96.3% retention) after 450 cycles at 3 C, nearly twice that of the unmodified one.

Multifunctional Catalytic Hierarchical Interfaces of Ni12 P5 -Ni2 P Porous Nanosheets Enabled Both Sulfides Reaction Promotion and Li-Dendrite Suppression for High-Performance Li-S Full Batteries.

The development of lithium-sulfur (Li-S) batteries is very promising and yet faces the issues of hindered polysulfides conversion and Li dendrite growth. Different from using different materials strategies to overcome these two types of problems, here multifunctional catalytic hierarchical interfaces of Ni12 P5 -Ni2 P porous nanosheets formed by Ni2 P partially in situ converted from Ni12 P5 are proposed. The unique electronic structure in the interface endows Ni12 P5 -Ni2 P effective electrocatalysis effect toward both sulfides' reduction and oxidation through reducing Gibbs free energies, indicating a bidirectional conversion acceleration. Importantly, Ni12 P5 -Ni2 P porous nanosheets with hierarchical interfaces also reduced the Li nucleation energy barrier, and a dendrite-free Li deposition is realized during the overall Li deposition and stripping steps. To this end, Ni12 P5 -Ni2 P decorated carbon nanotube/S cathode showing a high capacity of over 1500 mAh g-1 , and a high rate capability of 8 C. Moreover, the coin full cell delivered a high capacity of 1345 mAh g-1 at 0.2 C and the pouch full cell delivered a high capacity of 1114 mAh g-1 at 0.2 C with high electrochemical stability during 180° bending. This work inspires the exploration of hierarchical structures of 2D materials with catalytically active interfaces to improve the electrochemistry of Li-S full battery.

Piezoelectric Polymer Solid Electrolyte Integrating Electromechanical Coupling and Ferroelectric Polarization Effects.

The unsatisfactory lithium-ion conductivity (σ) and limited mechanical strength of polymer solid electrolytes hinder their wide applications in solid-state lithium metal batteries (SSLMBs). Here, a thin piezoelectric polymer solid electrolyte integrating electromechanical coupling and ferroelectric polarization effects has been designed and prepared to achieve long-term stable cycling of SSLMBs. The ferroelectric Bi4Ti3O12 nanoparticle (BIT NPs) loaded poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)) piezoelectric nanofibers (B-P NFs) membranes are introduced into the poly(ethylene oxide) (PEO) matrix, endowing the composite electrolyte with unique polarization and piezoelectric effects. The piezoelectric nanofiber membrane with a 3D network structure not only promotes the dissociation of lithium (Li) salts through the polarization effect but also cleverly utilizes the coupling effect of a mechanical stress-local electric field to achieve dynamic regulation of the Li electroplating process. Through the corresponding experimental tests and density functional theory calculations, the intrinsic mechanism of piezoelectric electrolytes improving σ and suppressing Li dendrites is fully revealed. The obtained piezoelectric electrolyte has achieved stable cycling of LiFePO4 batteries over 2000 cycles and has also shown good practical application potential in flexible pouch batteries.

Trinitarian Design of Gradient Artificial Interphase Enables Colossal Granular Li Deposits for Stable Li-Metal Batteries.

The cycling lifespan of Li-metal batteries is compromised by the unstable solid electrolyte interphase (SEI) and the continuous Li dendrites, restricting their practical implementations. Given these challenges, establishing an artificial SEI holds promise. Herein, a trinitarian gradient interphase is innovatively designed through composite coatings of magnesium fluoride (MgF2), N-hexadecyltrimethylammonium chloride (CTAC), and polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP) on Li-metal anode (LMA). Specifically, the MgF2/CTAC/PVDF-HFP SEI spontaneously forms a lithium fluoride (LiF)-rich PVDF-HFP-based SEI, along with lithium-magnesium (Li-Mg) alloy substrate as lithiophilic electronic conductor and positively charged CTAC during plating. Noticeably, the Li-Mg alloy homogenizes the distribution of electric field and reduce the internal resistance, while the electronically insulated LiF/PVDF-HFP composite SEI offers fast ion-conducting and mechanical flexibility, accommodating the volumetric expansion and ensuring stable Li-ion flux. Additionally, CTAC at the dendritic tip is pivotal for mitigating dendrites through its electrostatic shield mechanism. Innovatively, this trinitarian synergistic mechanism, which facilitates colossal granular Li deposits, constructs a dendrite-free LMA, leading to stable cycling performances in practical Li||LFP, popular Li||NCM811, and promising Li||S full cells. This work demonstrates the design of multifunctional composite SEI for comprehensive Li protection, thereby inspiring further advancements in artificial SEI engineering for alkali-metal batteries.

Trace Fluorinated Carbon dots driven Li-Garnet Solid-State Batteries.

Garnet solid-state electrolyte Li6.5La3Zr1.5Ta0.5O12 (LLZTO) holds significant promise. However, the practical utilization has been seriously impeded by the poor contact of Li|garnet and electron leakage. Herein, one new type garnet-based solid-state batteries is prososed with high-performance  through the disparity in interfacial energy, induced by the reaction between trace fluorinated carbon dots (FCDs) and Li. The work of adhesion of Li|garnet is increased by the acquired Li-FCD composite, which facilitates an intimate Li|garnet interface with the promoted uniform Li+ deposition, revealed by density functional theory (DFT) calculations. It is futher validated that a concentrated C-Li2O-LiF component at the Li|garnet interface is spontaneously constructed, due to the the significant disparity in interfacial energy between C-Li2O-LiF|LLZTO and C-Li2O-LiF|Li. Furthermore, The electron transport and Li dendrites penetration are effectively hindered by the formed Li2O and LiF. The Li-FCD|LLZTO|Li-FCD symmetrical cells demonstrate stable cycling performance for over 3000 hours at 0.3 mA cm-2 and 800 hours at 0.5 mA cm-2. Furthermore, the LFP|garnet|Li-FCD full cell exhibit remarkable cycling performance (91.6% capacity retention after 500 cycles at 1 C). Our research has revealed a novel approach to establish a dendrite-free Li|garnet interface, laying the groundwork for future advancements in garnet-based solid-state batteries.

Suppressing Dendrite Growth with Eco-Friendly Sodium Lignosulfonate Additive in Quasi-Solid-State Li Metal Battery.

The application of lithium metal batteries is limited by the drawbacks of safety problems and Li dendrite formation. Quasi-solid-state electrolytes (QSSEs) are the most promising alternatives to commercial liquid electrolytes due to their high safety and great compatibility with electrodes. However, Li dendrite formation and the slow Li+ diffusion in QSSEs severely hinder uniform Li deposition, thus leading to Li dendrite growth and short circuits. Herein, an eco-friendly and low-cost sodium lignosulfonate (LSS)-assisted PVDF-based QSSE is proposed to induce uniform Li deposition and inhibit Li dendrite growth. Li symmetric cells with 5%-LSS QSSE possess a high Li+ transfer number of 0.79, and they exhibit a long cycle life of 1000 h at a current density/areal capacity of 1 mA cm-2/5 mAh cm-2. Moreover, due to the fast electrochemical dynamics endowed by the improved compatibility of the electrodes and fast Li+ diffusion, the LFP/5%-LSS/Li full cells still maintain a high capacity of 110 mAh g-1 after 250 cycles at 6C. This work provides a novel and promising choice that uses eco-friendly LSS as an additive to PVDF-based QSSE in Li metal batteries.

Lithium Deposition-Induced Fracture of Carbon Nanotubes and Its Implication to Solid-State Batteries.

The increasing demand for safe and dense energy storage has shifted research focus from liquid electrolyte-based Li-ion batteries toward solid-state batteries (SSBs). However, the application of SSBs is impeded by uncontrollable Li dendrite growth and short circuiting, the mechanism of which remains elusive. Herein, we conceptualize a scheme to visualize Li deposition in the confined space inside carbon nanotubes (CNTs) to mimic Li deposition dynamics inside solid electrolyte (SE) cracks, where the high-strength CNT walls mimic the mechanically strong SEs. We observed that the deposited Li propagates as a creeping solid in the CNTs, presenting an effective pathway for stress relaxation. When the stress-relaxation pathway is blocked, the Li deposition-induced stress reaches the gigapascal level and causes CNT fracture. Mechanics analysis suggests that interfacial lithiophilicity critically governs Li deposition dynamics and stress relaxation. Our study offers critical strategies for suppressing Li dendritic growth and constructing high-energy-density, electrochemically and mechanically robust SSBs.

Lithium Ion Repulsion-Enrichment Synergism Induced by Core-Shell Ionic Complexes to Enable High-Loading Lithium Metal Batteries.

A core-shell additive with anionic Keggin-type polyoxometalate (POM) cluster as core and N-containing cation of ionic liquid (IL) as shell is proposed to stabilize Li-metal batteries (LMBs). The suspended POM derived complex in ether-based electrolyte is absorbed around the protuberances of anode and triggers a lithiophobic repulsion mechanism for the homogenization of Li+ redistribution. The gradually released POM cores with negative charge then enrich Li+ and co-assemble with Li. The Li+ repulsion-enrichment synergism can compact Li deposition and reinforce solid electrolyte interphase. This sustained-release additive enables Li∥Li symmetric cells with a long lifetime over 500 h and 300 h at high current densities of 3 and 5 mA cm-2 respectively. The complex additive is also compatible with high-voltage Li∥LiNi0.8 Co0.15 Al0.05 O2 (NCA) cells. Even with a NCA loading as high as ca. 20 mg cm-2 , the additive contained Li∥NCA cell can still cycle for over 100 cycles at 2.6 mA cm-2 .

Consecutive Nucleation and Confinement Modulation towards Li Plating in Seeded Capsules for Durable Li-Metal Batteries.

A dual modulation strategy of consecutive nucleation and confined growth of Li metal is proposed by using the metal-organic framework (MOF) derivative hollow capsule with inbuilt lithiophilic Au or Co-O nanoparticle (NP) seeds as heterogeneous host. The seeding-induced nucleation enables the negligible overpotential and promotes the inward injection of Li mass into the abundant cavities in host, followed by the conformal plating of Li on the outer surface of host during discharging. This modulation alleviates the dendrite growth and volume expansion of Li plating. The interconnected porous host network enables enhancement of cycling and rate performances of Li metal (a lifespan over 1200 h for Au-seeding symmetric cells, and an endurance of 220 cycles under an ultrahigh current density of 10 mA cm-2 for corresponding asymmetric cells). The hollow capsules integrated with lithiophilic seeds solve the deformation problem of Li metal for durable and long-life Li-metal batteries.

Progress on Lithium Dendrite Suppression Strategies from the Interior to Exterior by Hierarchical Structure Designs.

Lithium (Li) metal is promising for high energy density batteries due to its low electrochemical potential (-3.04 V) and high specific capacity (3860 mAh g-1 ). However, the safety issues impede the commercialization of Li anode batteries. In this work, research of hierarchical structure designs for Li anodes to suppress Li dendrite growth and alleviate volume expansion from the interior (by the 3D current collector and host matrix) to the exterior (by the artificial solid electrolyte interphase (SEI), protective layer, separator, and solid state electrolyte) is concluded. The basic principles for achieving Li dendrite and volume expansion free Li anode are summarized. Following these principles, 3D porous current collector and host matrix are designed to suppress the Li dendrite growth from the interior. Second, artificial SEI, the protective layer, and separator as well as solid-state electrolyte are constructed to regulate the distribution of current and control the Li nucleation and deposition homogeneously for suppressing the Li dendrite growth from exterior of Li anode. Ultimately, this work puts forward that it is significant to combine the Li dendrite suppression strategies from the interior to exterior by 3D hierarchical structure designs and Li metal modification to achieve excellent cycling and safety performance of Li metal batteries.

Lithium-Salt Mediated Synthesis of a Covalent Triazine Framework for Highly Stable Lithium Metal Batteries.

A new strategy for the synthesis of a covalent triazine framework (CTF-1) was introduced based on the cyclotrimerization reaction of 1,4-dicyanobenzene using lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) under ionothermal conditions. LiTFSI not only served as a catalyst, but also facilitated the in situ generation and homogeneous distribution of LiF particles across the framework. The hierarchical structure resulting upon integration of CTF-LiF onto an airlaid-paper (AP) offered unique features for lithium metal anodes, such as lithiophilicity from CTF, interface stabilization from LiF, and sufficient lithium storage space from AP. Based on this synergistic effect, the AP-CTF-LiF anode exhibited stable cycling performance even at a current density of 10 mA cm-2 .

Ultrahigh-Capacity and Long-Life Lithium-Metal Batteries Enabled by Engineering Carbon Nanofiber-Stabilized Graphene Aerogel Film Host.

A safe, high-capacity, and long-life Li metal anode is highly desired due to recent developments in high-energy-density Li-metal batteries. However, there are still rigorous challenges associated with the undesirable formation of Li dendrites, lack of suitable host materials, and unstable chemical interfaces. Herein, a carbon nanofiber-stabilized graphene aerogel film (G-CNF film), inspired by constructional engineering, is constructed. As the host material for Li deposition, the G-CNF film features a large surface area, porous structure, and a robust skeleton that can render low local current density. This allows for dendrite-free Li deposition and mitigation of problems associated with large volume change. Importantly, the G-CNF film can keep high Li plating/stripping efficiency at nearly 99% for over 700 h with an areal capacity of 10 mA h cm-2 (the specific capacity up to 2588 mA h g-1 based on the total mass of carbon host and Li metal). The symmetric cells can stably run for more than 1000 h with low voltage hysteresis. The full cell with the LiFePO4 cathode also delivers enhanced capacity and lowered overpotential. As two-in-one host materials for both cathodes and anodes in Li-O2 batteries, the battery exhibits a capacity of 1.2 mA h cm-2 .

Superior Conductive Solid-like Electrolytes: Nanoconfining Liquids within the Hollow Structures.

The growth and proliferation of lithium (Li) dendrites during cell recharge are currently unavoidable, which seriously hinders the development and application of rechargeable Li metal batteries. Solid electrolytes with robust mechanical modulus are regarded as a promising approach to overcome the dendrite problems. However, their room-temperature ionic conductivities are usually too low to reach the level required for normal battery operation. Here, a class of novel solid electrolytes with liquid-like room-temperature ionic conductivities (>1 mS cm(-1)) has been successfully synthesized by taking advantage of the unique nanoarchitectures of hollow silica (HS) spheres to confine liquid electrolytes in hollow space to afford high conductivities (2.5 mS cm(-1)). In a symmetric lithium/lithium cell, the solid-like electrolytes demonstrate a robust performance against the Li dendrite problem, preventing the cell from short circuiting at current densities ranging from 0.16 to 0.32 mA cm(-2) over an extended period of time. Moreover, the high flexibility and compatibility of HS nanoarchitectures, in principle, enables broad tunability to choose desired liquids for the fabrication of other kinds of solid-like electrolytes, such as those containing Na(+), Mg(2+), or Al(3+) as conductive media, providing a useful alternative strategy for the development of next generation rechargeable batteries.

Observation and quantification of nanoscale processes in lithium batteries by operando electrochemical (S)TEM.

An operando electrochemical stage for the transmission electron microscope has been configured to form a "Li battery" that is used to quantify the electrochemical processes that occur at the anode during charge/discharge cycling. Of particular importance for these observations is the identification of an image contrast reversal that originates from solid Li being less dense than the surrounding liquid electrolyte and electrode surface. This contrast allows Li to be identified from Li-containing compounds that make up the solid-electrolyte interphase (SEI) layer. By correlating images showing the sequence of Li electrodeposition and the evolution of the SEI layer with simultaneously acquired and calibrated cyclic voltammograms, electrodeposition, and electrolyte breakdown processes can be quantified directly on the nanoscale. This approach opens up intriguing new possibilities to rapidly visualize and test the electrochemical performance of a wide range of electrode/electrolyte combinations for next generation battery systems.

Dendrite-free lithium deposition with self-aligned nanorod structure.

Suppressing lithium (Li) dendrite growth is one of the most critical challenges for the development of Li metal batteries. Here, we report for the first time the growth of dendrite-free lithium films with a self-aligned and highly compacted nanorod structure when the film was deposited in the electrolyte consisting of 1.0 M LiPF6 in propylene carbonate with 0.05 M CsPF6 as an additive. Evolution of both the surface and the cross-sectional morphologies of the Li films during repeated Li deposition/stripping processes were systematically investigated. It is found that the formation of the compact Li nanorod structure is preceded by a solid electrolyte interphase (SEI) layer formed on the surface of the substrate. Electrochemical analysis indicates that an initial reduction process occurred at ∼ 2.05 V vs Li/Li(+) before Li deposition is responsible for the formation of the initial SEI, while the X-ray photoelectron spectroscopy indicates that the presence of CsPF6 additive can largely enhance the formation of LiF in this initial SEI. Hence, the smooth Li deposition in Cs(+)-containing electrolyte is the result of a synergistic effect of Cs(+) additive and preformed SEI layer. A fundamental understanding on the composition, internal structure, and evolution of Li metal films may lead to new approaches to stabilize the long-term cycling stability of Li metal and other metal anodes for energy storage applications.

Constructing Reversible Li Deposition Interfaces by Tailoring Lithiophilic Functionalities of a Heteroatom-Doped Graphene Interlayer for Highly Stable Li Metal Anodes.

Lithium (Li) metal has been regarded as the ideal anode for rechargeable batteries due to its low reduction potential and high theoretical capacity. However, the formation of fatal Li dendrites during repeated cycling shortens the battery life and causes serious safety concerns. Functionalized separators with electrically conductive and lithiophilic coating layers potentially inhibit dendrite formation and growth on Li metal anodes by providing nucleation sites for reversible Li deposition/stripping. In this work, we propose functionalized separators incorporating heteroatom-doped (N or B) graphene interlayers to modulate the Li nucleation behavior. The electronegative N-doping and electropositive B-doping were investigated to understand their regulation of the Li deposition behavior. With the heteroatom-doped graphene-coated separators, we observe significantly improved cycling stability along with enhanced charge transfer kinetics and low Li nucleation overpotential. This is attributed to the heteroatom-doped graphene interlayer expanding the surface area of the Li metal anode while providing additional space for uniform Li deposition/stripping, thus preventing undesirable side reactions. As a result, the formation of dendrites and pits on the Li metal anode surface is suppressed, demonstrating the protective effect of the Li metal anode. Interestingly, N-doped graphene-coated separators exhibit lower Li nucleation overpotentials than B-doped graphene-coated separators but rather lower average Coulombic efficiencies and reduced cycling stability. This implies that adequate adsorption on B-based sites, as opposed to the strong adsorption on N-based sites, improves the reversibility. Notably, the Li adsorption strength of the lithiophilic functional groups critically affects the reversibility, as observed by Li nucleation barrier measurements and atomistic simulations. This work suggests that interface engineering using conductive and lithiophilic materials can be a promising strategy for controlling Li deposition in advanced Li metal batteries.

Dual-functional Separators Regulating Ion Transport Enabled by 3D-Reinforced Polyimide Microspheres Protective Layer for Dendrite-Free and High-Temperature Lithium Metal Batteries.

High-energy-density lithium metal batteries (LMBs) are confronted with crucial concerns of security and a short cycle lifespan caused by the uncontrollable formation of lithium (Li) dendrites. The poor thermal stability and heterogeneous Li deposition of conventional polyolefin separators often cause battery short circuiting and thermal runaway in LMBs. Herein, a novel dual-functional PE composite separator (PI-COOH/PE) coated by carboxyl polyimide (PI) microspheres is fabricated by an etching-acidification method. The three-dimensional (3D) high-temp PI microsphere with rich carboxyl groups on the surface improve the security of LMBs at extremely high temperatures and facilitate the formation of a stable and uniform SEI layer, which contributes to accelerating the Li+ transport and stabilizing the formation of the SEI layer. Consequently, the Li symmetric cell assembled with the (PI-COOH)/PE separator exhibits stable overpotential over 3000 h, and the corresponding Li//NCM811 full cells also show a high-level discharge capacity of 146.6 mAh g-1 at 5 C. Meanwhile, it also demonstrates outstanding cycling stability and thermal safety, which can survive continuously over 160 min at 140 °C (vs 21 min for PE). The above results indicate the (PI-COOH)/PE separator constructed by a low-cost and industrial-friendly strategy simultaneously addresses high-temperature stability and dendrite resistance.

Lithiophilic Multichannel Layer to Simultaneously Control the Li-Ion Flux and Li Nucleation for Stable Lithium Metal Batteries.

Although the Li metal has been gaining attention as a promising anode material for the next-generation high-energy-density rechargeable batteries owing to its high theoretical specific capacity (3860 mAh g-1), its practical use remains challenging owing to inherent issues related to Li nucleation and growth. This paper reports the fabrication of a lithiophilic multichannel layer (LML) that enables the simultaneous control of Li nucleation and growth in Li-metal batteries. The LML, composed of lithiophilic ceramic composite nanoparticles (Ag-plated Al2O3 particles), is fabricated using the electroless plating method. This LML provides numerous channels for a uniform Li-ion diffusion on a nonwoven separator. Furthermore, the lithiophilic Ag on the Li metal anode surface facing the LML induces a low overpotential during Li nucleation, resulting in a dense Li deposition. The LML enables the LiNi0.8Co0.1Mn0.1O2|| Li cells to maintain a capacity higher than 75% after 100 cycles, even at high charge/discharge rates of 5.0 C at a cutoff voltage of 4.4 V, and achieve an ultrahigh energy density of 1164 Wh kg-1. These results demonstrate that the LML is a promising solution enabling the application of Li metal as an anode material in the next-generation Li-ion batteries.

A Dynamically Stable Mixed Conducting Interphase for All-Solid-State Lithium Metal Batteries.

All-solid-state lithium (Li) metal batteries (ASSLMBs) employing sulfide solid electrolytes have attracted increasing attention owing to superior safety and high energy density. However, the instability of sulfide electrolytes against Li metal induces the formation of two types of incompetent interphases, solid electrolyte interphase (SEI) and mixed conducting interphase (MCI), which significantly blocks rapid Li-ion transport and induces uneven Li deposition and continuous interface degradation. In this contribution, a dynamically stable mixed conducting interphase (S-MCI) is proposed by in situ stress self-limiting reaction to achieve the compatibility of Li metal with composite sulfide electrolytes (Li6 PS5 Cl (LPSCl) and Li10 GeP2 S12 (LGPS)). The rational design of composite electrolytes utilizes the expansion stress induced by the electrolyte decomposition to in turn constrain the further decomposition of LGPS. Consequently, the S-MCI inherits the high dynamical stability of LPSCl-derived SEI and the lithiophilic affinity of Li-Ge alloy in LGPS-derived MCI. The Li||Li symmetric cells with the protection of S-MCI can operate stably for 1500 h at 0.5 mA cm-2 and 0.5 mAh cm-2 . The Li||NCM622 full cells present stable cycling for 100 cycles at 0.1 C with a high-capacity retention of 93.7%. This work sheds fresh insight into constructing electrochemically stable interphase for high-performance ASSLMBs.