LiF Layer Research Articles

On the Surface Modification of LLZTO with LiF via a Gas-Phase Approach and the Characterization of the Interfaces of LiF with LLZTO as Well as PEO+LiTFSI.

In this study we present gas-phase fluorination as a method to create a thin LiF layer on Li6.5La3Zr1.5Ta0.5O12 (LLZTO). We compared these fluorinated films with LiF films produced by RF-magnetron sputtering, where we investigated the interface between the LLZTO and the deposited LiF showing no formation of a reaction layer. Furthermore, we investigated the ability of this LiF layer as a protection layer against Li2CO3 formation in ambient air. By this, we show that Li2CO3 formation is absent at the LLZTO surface after 24 h in ambient air, supporting the protective character of the formed LiF films, and hence potentially enhancing the handling of LLZTO in air for battery production. With respect to the use within hybrid electrolytes consisting of LLZTO and a mixture of polyethylene oxide (PEO) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), we also investigated the interface between the formed LiF films and a mixture of PEO+LiTFSI by X-ray photoelectron spectroscopy (XPS), showing decomposition of the LiTFSI at the interface.

Conformal LiF Stabilized Interfaces via Electrochemical Fluorination on High Voltage Spinel Cathodes (≈4.9 V) for Lithium‐Ion Batteries

AbstractThe high voltage LiNi0.5Mn1.5O4 (LNMO) spinel is one of the promising cathodes for the lithium‐ion batteries due to its high energy densities, good rate performance. However, its high operating potential (≈4.75 V) causes extensive oxidation of conventional carbonate electrolytes, resulting an unstable and thick cathode electrolyte interphase (CEI) layer with a large irreversible capacity and low coulombic efficiency. Herein, this work reports the formation of thin LiF stabilized interfaces on LNMO via electrochemical fluorination that significantly improves the cycling stability and enhanced the capacity. An electrochemically induced conformal LiF layer acts as a part of a robust CEI by reducing the leakage of electrons and allowing the conduction of Li ions through it. Because of the robust LiF stabilized CEI, LNMO delivers a discharge capacity of ≈148.5 and ≈117.1 mAh g−1 at 0.1 and 1 C rate, respectively. It exhibits excellent cyclability with 80% capacity retention (CR) after 600 cycles in lithium‐half cell and ≈90% CR after 200 cycles in full cell with only 0.03% and 0.05% capacity decay per cycle in conventional carbonate electrolytes without additives. Such an excellent electrochemical performance could lead to the potential development of high energy density batteries with high voltage cathodes for grid‐based applications.

Constructing LiF-rich artificial SEI at a two-dimensional copper net current collector in anode-free lithium metal batteries

Anode-Free lithium metal batteries (AF-LMBs) show the advantage in reducing the volume change of lithium metal anode, however also suffer from the obstacles of lacking active sites and uneven deposition of lithium. Herein, employing the silver coated two-dimensional (2D) copper net with artificial LiF-rich solid electrolyte interphase (SEI) as the current collector is proposed to address these issues. The 2D copper net has high chemical and volume stability, and the coated silver nanoparticles can provide active sites for lithium deposition. LiF layer can homogenize Li-ion flux and improve the stability of the interface between electrode and electrolyte. By combining the above-mentioned superiorities, compared with the initial copper net, LiF@Li-Ag@Cu maintains higher coulombic efficiencies and enhanced stable cycling over 250 h at a current density of 1 mA cm−2 in the asymmetric cell with Li foil as counter electrode. A good cycling stability can be also observed in a full cell with LiNi0.8Co0.1Mn0.1O2 as positive electrode material.

Collaborative Assembly of a Fluorine-Enriched Heterostructured Solid Electrolyte Interphase for Ultralong-Life Lithium Metal Batteries.

Lithium metal batteries have become potential high-energy storage devices because lithium metal has excellent theoretical capacity and low reduction potential. Unfortunately, the reckless growth of lithium dendrites leads to the decrease in Coulombic efficiency and the attenuation of cycle performance. Herein, we propose a collaborative assembly approach for a fluorine-enriched heterostructured solid electrolyte interphase (SEI) on lithium metal to enable stable and ultralong-life lithium metal batteries. The fluorine-enriched heterostructured SEI consists of an artificial precursor substrate K2ZrF6 and an epigenetically assembled LiF layer, and the composite structure cooperatively realizes the rapid conduction of Li+ ions and inhibits the formation of lithium dendrites. Benefiting from the heterostructured SEI, the symmetric cell exhibits an ultralong-time stable cycle of more than 7000 h at a high current and capacity density (4 mA cm-2 and 4 mA h cm-2, respectively), much longer than that of the lithium cell. Besides, the LiFePO4 full battery (LFP||Li-Zr) enables substantially enhanced cyclability over 800 cycles at 1 C. This work paves the way for dendrite-free and long-life lithium metal batteries with well-balanced heterostructured SEI engineering.

Constructing interfacial gradient layers and enhancing lithium salt dissolution kinetics for high-rate solid-state batteries

The stability of the interfacial layers depends mainly on the composition and distribution of the decomposition products from solid-state electrolytes (SSEs) in lithium metal batteries. Therefore, the design of SSEs becomes an attractive way to construct a homogeneous stable interfacial layer. Herein, pentafluorostyrene (PFS) as a block is used to generate robust interfacial layers for solid-state batteries. Meanwhile, PFS facilitates the dissociation of lithium salts to produce more free Li-ions which can enhance the ionic conductivity from the results of 7Li solid-state NMR spectra, density functional theory, and molecular dynamics calculations. Subsequently, XPS depth etching and TOF-SIMS characterizations together show that the gradient interfacial layer is composed of a rich C-F bond surface layer and a rich–LiF&Li3N bottom layer, enabling rapid transport and uniform deposition of lithium ions. As a result, the Li/Li symmetric cell can achieve a stable ultra-long cycle time of more than 3000 h at 0.2 mA cm−2 and a critical current density of 2.4 mA cm−2. The as-prepared SSE exhibits a high ionic conductivity of 4.3 × 10−4 S cm−1 at 25 °C and remarkable cycling stability at 0 °C and − 20 °C. Moreover, the lithium metal batteries based on as-prepared SSEs deliver high-rate (2 C) capability and high-voltage (NCM811) stability at room temperatures.

An FPGA Accelerator for High-Speed Moving Objects Detection and Tracking With a Spike Camera.

Ultra-high-speed object detection and tracking are crucial in fields such as fault detection and scientific observation. Existing solutions to this task have deficiencies in processing speeds. To deal with this difficulty, we propose a neural-inspired ultra-high-speed moving object filtering, detection, and tracking scheme, as well as a corresponding accelerator based on a high-speed spike camera. We parallelize the filtering module and divide the detection module to accelerate the algorithm and balance latency among modules for the benefit of the task-level pipeline. To be specific, a block-based parallel computation model is proposed to accelerate the filtering module, and the detection module is accelerated by a parallel connected component labeling algorithm modeling spike sparsity and spatial connectivity of moving objects with a searching tree. The hardware optimizations include processing the LIF layer with a group of multiplexers to reduce ADD operations and replacing expensive exponential operations with multiplications of preprocessed fixed-point values to increase processing speed and minimize resource consumption. We design an accelerator with the above techniques, achieving 19 times acceleration over the serial version after 25-way parallelization. A processing system for the accelerator is also implemented on the Xilinx ZCU-102 board to validate its functionality and performance. Our accelerator can process more than 20,000 spike images with 250 × 400 resolution per second with 1.618 W dynamic power consumption.

Design of inorganic/organic bi-layered Li protection layer enabled dendrite-free practical Li metal battery

In this work, we report an inorganic/organic bi-layered, composed LiF, Li3N, Li2S, and porous polymer layer (LiFNS-PPL), Li protection layer for practical Li metal application toward high energy density Li metal batteries. The LiFNS-PPL layer, formed by a facile and scalable roll-pressing between Li metal and LiTFSI and PTFE complex film, is composed of an inside (lithium side) robust inorganic layer with 200 nm thick and outside (electrolyte side) porous polymer layer with over 20 μm thick. The robust inorganic layer prohibits dendritic Li growth. The flexible and porous polymer layer retains the protection layer structure with high Li-ion flux. This novel LiFNS-PPL protection layer enables in-plane Li growth underneath the protection layer without Li dendrites, resulting in high electrochemical performance. Even in the carbonate-based electrolyte and high areal capacity, cycle retention showed over 600 h under 1 mA∙cm−2 with 5 mAh∙cm−2 condition in the Li||Li symmetric cell. Full cells paired with high-nickel contented nickel manganese oxide (NCM811) are prepared with a high areal capacity of 5 mA h·cm−2 NCM cathode and a limited Li reservoir of 4.1 mA h·cm−2 (20 μm-thick) with 0.8 N/P ratios. The Li||NCM full cell with the protection layer presents stable cycle performance over 200 cycles with the Li anode efficiency of 99.6% calculated by average Coulombic efficiency. Our facile and scalable process for introducing multi-functional Li protection layer delivers good insight into the practical implementation of high energy density Li metal batteries.

Highly conductive and transparent thin metal layer for reducing microcavity effect in top-emitting white organic light-emitting diode

The optical and electrical properties of the top electrode are crucial for the structural design of top-emitting organic light-emitting diodes (OLEDs). A uniform metal layer, if obtainable, can be electrically excellent and optically well-tuned. In this study, Ag deposited with Mg at a concentration of 9:1 to form a metal thin film exhibits higher conductivity and higher transmittance than those of a neat Ag thin film within a thickness of 10 nm or less. In addition, the thin Mg:LiF (1:1) layer renders the Mg:Ag metal film more uniform and enhances its electron injection property. If a Mg:LiF/Mg:Ag thin film is applied to top-emitting white OLEDs, the driving voltage is lowered and the efficiency is improved. In addition, color shifts for viewing angles are reduced, and the emission characteristics are close to Lambertian. • 10-nm-thick Mg:Ag (1:9) metal forms a more uniform film compared with neat Ag thin metal of the same thickness. • Thin Mg:LiF (1:1) layer improves the optical and electrical properties of the Mg:Ag thin film. • Top-emitting white OLED device with thin Mg:Ag shows higher efficiency and superior angular emission characteristics.

Enhancing Cycling Stability and Capacity Retention of NMC811 Cathodes by Reengineering Interfaces via Electrochemical Fluorination (Adv. Mater. Interfaces 18/2022)

Reengineering Cathode Interfaces Via Electrochemical Fluorination In article number 2200035, Bishnu P. Thapaliya, Sheng Dai, and co-workers develop electrochemical fluorination (ECF) to reengineer the interface of high-capacity cathodes by forming conformal LiF layer. The ECF can tune the LiF layer thickness, resulting in a robust cathode electrolyte interphase (CEI), which in turn results in enhanced electrochemical performance. Additionally, ECF is cost-effective and free from all the hazards associated with state-of-the-art fluorination that ensure its easy industrial upscaling.

Building a stable artificial solid electrolyte interphase on lithium metal anodes toward long-life Li–O2 batteries

Rechargeable Li–O2 batteries (LOBs) are considered as a promising battery technology due to their high energy density. The performance of the batteries, however, is limited by inevitable chemical/electrochemical corrosion and uncontrollable Li dendrite growth. Here, a uniform and dense LiF artificial solid electrolyte interphase (SEI) is introduced to address these issues. This LiF layer with rich and uniform crystal boundary can homogenize the Li-ion flux on Li metal anodes (LMAs) surface and thus accomplish planar Li deposition under the LiF layer, improving the interfacial stability of LMAs. In addition, the dense LiF layer enables high corrosion resistance against the electrolyte and air. As a result, the symmetric cells with LiF layer coated Li anodes (LiF@Li) show stable polarization voltage and long cycle life up to 1000 h. Moreover, the Li–O2 battery with LiF@Li shows excellent cycle stability up to 150 cycles at an ultrahigh current density of 4.50 mA cm−2. This work illustrates a promising way for the unfettered development of advanced LOBs.

One-Pot Preparation of Lithium Compensation Layer, Lithiophilic Layer, and Artificial Solid Electrolyte Interphase for Lean-Lithium Metal Anode.

Lithium metal is an ideal anode for high-energy-density batteries. However, the low Coulomb efficiency and the generation of dendrites pose a significant limitation to its practical application, while the excess lithium in the battery also generates serious safety concerns. Herein, a layer-by-layer optimized multilayer structure integrating an artificial solid electrolyte interphase (LiF) layer, a lithiophilic (LixAu alloy) layer, and a lithium compensation layer is reported for a lean-lithium metal battery, where each layer acts synergistically to stabilize the lithium deposition behaviors and enhances the cycling performance of the battery. The optimized anode could effectively induce homogeneous reversible lithium deposition under the synergistic effect of multilayer films and keep the integrity of the morphological structure unbroken during the deposition. The presence of the lithium compensation layer allows the half-cell to have a high initial CE of 158.9%, and the action of the LiF layer and lithiophilic layer maintains an average CE of 98.8% over 160 cycles, which further demonstrates the stability of the structure. As a result, when combined with LiFePO4 cathode, an initial capacity of 148 mAh g-1 and a retention rate of 97.5% over 130 cycles were achieved.

Multiscale Simulation of Solid Electrolyte Interface Formation in Fluorinated Diluted Electrolytes with Lithium Anodes.

Lithium metal batteries (LMBs) hold great promise in facilitating high-energy batteries due to their merits such as high specific capacity, low reduction potential, and so forth. However, the realizations of practical LMBs are hindered by severe problems such as undesirable dendrite growth, poor Coulombic efficiency, and so forth. A recently proposed fluorinated electrolyte based on 1 M lithium bis(fluorosulfonyl)imide (LiFSI) dissolved in designed fluorinated 1,4-dimethoxybutane (FDMB) solvent has attracted significant attention because of its excellent electrochemical performance that origins from its superior physical and chemical properties, especially its unique ability in forming a robust, stable solid electrolyte interphase (SEI). However, the detailed structure and reaction mechanism of the SEI formation in such a novel electrolyte remains unclear. In this work, we carry out a hybrid ab initio and reactive molecular dynamics (HAIR) simulation to investigate the elementary reactions that regulate the formation of the primitive SEI, paying special attention to the process that involves FDMB, the fluorinated solvent. HAIR simulation reveals that both FSI- anion and FDMB provide F that is adequate to form a uniformed LiF layer that resembles the inorganic inner layer (IIL) of the SEI. N and S radicals from the FSI- anion, which do not deposit on the electrode interface to form lithium-containing inorganic substances, promote the polymerization reaction of unsaturated carbon chains produced by FDMB defluorination, forming the organic outer layer (OOL) of the SEI. The combination of the LiF-rich IIL and polymer-rich organic OOL explains the superior performance of the FDMB-based electrolyte in the device. The detailed reaction mechanism and SEI observed in this work provide insights into the atomic scale for the rational design of F-rich electrolytes in the near future.

Enhancing the interfacial perpendicular magnetic anisotropy and tunnel magnetoresistance by inserting an ultrathin LiF layer at an Fe/MgO interface

Perpendicular magnetic anisotropy (PMA) is becoming increasingly important in spintronics research, especially for high-density magnetoresistive random access memories (MRAMs). The PMA induced at an Fe/MgO interface is widely used in magnetic tunnel junctions. Here, we propose inserting an ultrathin LiF layer at the interface in an epitaxial Fe/MgO junction. With a 0.3 nm-thick LiF layer, a large intrinsic interface PMA energy, Ki,0, of 2.8 mJ/m2 was achieved. We also found that the LiF/MgO bilayer tunneling barrier exhibited a large tunnel magnetoresistance (TMR) effect, suggesting that a coherent spin-dependent tunneling process was maintained in the ultrathin LiF layer. Atomic-scale interface engineering using fluoride can further improve the PMA and TMR properties of spintronic devices.

Numerical study of aluminum doped zinc oxide anode based fluorescent bilayer organic light-emitting diode

The simulation study is carried out to investigate the performance of organic light-emitting diode (OLED), AZO/NPB/Alq3: Ir(ppy)3/LiF/Al configuration. To minimize the turn-on (knee) voltage, the LiF layer is staked with the organic emissive layer's (OEL's) and cathode. This interface enhances hysteresis of recombination prefactor due to the higher hopping effect of OEL with bilayer cathode unit (LiF/Al). To counteract such improvements, an electron injecting layer (EIL) free OLED is considered to nullify the impact under the thickness optimization of OEL. The maximum light flux of 9.5 × 106 Wm−2 has been achieved for 20 nm thickness of electron emission layer/electron transport layer (EML/ETL) and 10 nm thickness of hole transport layer (HTL). Thus, portrayed different characteristics curve implies the charge density and mean current density is 3 × 1024 m−3, and 1.2 × 106 Am−2 at 1.75 V turn-on (knee) voltages, respectively. The maximum recombination prefactor of 4 × 10−17 m−6 s−1 is found at 300 K for different optoelectronic parameters. This study also offers an alternative way to optimize further the efficiency of the Aluminium doped zinc oxide (AZO) anode contact OLED devices.

Coordinating ionic and electronic conductivity on 3D porous host enabling deep dense lithium deposition toward high-capacity lithium metal anodes.

Engineering composite lithium (Li) metal within three-dimensional (3D) porous skeleton hosts is a feasible strategy to tackle issues of uncontrollable dendrite growth and enormous volume change on Li metal anodes. Nevertheless, the accumulative Li deposition on the top surface of the 3D skeleton remains a harsh challenge that still requires effort. Herein, we develop a rational design involving an enriched-sparse LiF gradient on a Cu foam via facile magnetron sputtering to coordinate ionic and electronic conductivity. The Li ion-conductive LiF gradient guides deep, dense Li deposition within the Cu foam framework, safely preventing surface Li accumulation. As a result, the Cu foam with optimal LiF sputtering time for 40 min (Cu foam/LiF(40)) renders the best synergy of ionic and electronic conduction. Such composite Li anode in the symmetric cell achieves an ultra-long lifespan up to 1700 h at the current density of 2 mA cm-2 with the capacity of 2 mA h cm-2. This work certifies the decisive significance of coordinating ionic and electronic conductivity for uniform Li deposition on 3D porous hosts and provides a simple and effective avenue to controllably deposit Li in suitable locations for long-term and high-capacity 3D Li metal anodes.

Enhanced Electrochemical Performance of Ni-Rich Cathodes by Neutralizing Residual Lithium with Acid Compounds.

Surficial residual LiOH and/or Li2CO3 on Ni-rich cathodes arouse troubles for their practical applications, such as slurry gelling and durability degrading. To assure acceptable performance, the strategy of "washing and heat treatment" is generally utilized to remove them in industry, which is unavoidable to generate plenty of wastewater. In this work, we investigated the mechanism of slurry gelling caused by residual lithium on Ni-rich materials and then proposed a simple and efficient method to convert the detrimental residual lithium to the useful surface layer of LiF or LiBOB at 220 °C without water washing. As a result, the basicity of modified samples is lowered to 11.48 and 11.60 from 12.05 of the pristine, respectively. Owing to the beneficial effect of the surface layer, the treated samples deliver a discharge capacity of 189.5 and 187.9 mA h g-1 and retain 84.1 and 82.8% of the initial capacity under 1 C after 300 cycles, which is much better than that of the untreated material (57.8%). The comprehensive performances of the modified samples in this work are very close to those of the material treated with the industrial method, demonstrating the advantage of this strategy to further reduce the cost of material production.

Exploring the performance of carbonate and ether-based electrolytes for anode-free lithium metal batteries operating under various conditions

An anode-free lithium metal battery (AFLMB) configuration can be used to develop electrolytes for wide-temperature applications. The charge/discharge performance of an electrolyte consisting of lithium hexafluorophosphate (LiPF 6 ) in a mixture of fluoroethylene carbonate (FEC), 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE), and ethyl methyl carbonate (EMC) has been is reported as an electrolyte for lithium metal batteries. It has a good passivating capability and wide electrochemical windows relative to the commercial electrolyte. Conversely, its lower ionic conductivity and high viscosity impede practical application. Hence, an electrolyte of 1 M LiPF 6 in EA/FEC/TTE/EMC (2:1:5:2 by vol.) is developed by adding a quaternary solvent of ethyl acetate (EA). The electrolyte exhibits a lower viscosity and higher ionic conductivity than 1 M LiPF 6 in FEC/TTE/EMC (3:5:2 by vol.). At 0 °C, 1 M LiPF 6 in EA/FEC/TTE/EMC (2:1:5:2 by vol.) provides capacity retention of 30 % and the average Coulombic efficiency (av. CE) of 95 % using the Cu||NMC111 after 40 cycles at a current density of 0.2 mA/cm 2 . The synergy of higher ionic conductivity and formation of LiF layer in the developed electrolyte extends the service-temperature range of AFLMB. This study opens an avenue in developing low-temperature electrolytes using an AFLMB. • The cycling performance of an anode-free battery is extended under various conditions. • 1 M LiPF 6 in EA/FEC/TTE/EMC (2:1:5:2 by vol.) electrolyte is developed. • At 0 °C, it provides capacity retention of 30% using Cu.||NMC111 after 40 cycles. • The high solvation power of EA gives lower viscosity and higher ionic conductivity. • The developed electrolyte has stable cycling compared to EC/DEC electrolyte.

Multiscale Simulations to Study the Atomic Structure of Solid Electrolyte Interfaces

The Solid Electrolyte Interface (SEI) is the "most important but least understood" area of research in batteries. A deeper understanding of the atomic structure of SEI can provide a theoretical basis for the development of high energy density batteries. Based on the available experimental results, four generations of SEI models have been developed. However, the above-mentioned SEI models lack atomic details and cannot reasonably explain important experimental phenomena and guide experimental synthesis. Quantum chemistry (QM)-based multi-scale theoretical simulations are a powerful tool to study the atomic structure of interfaces. The authors' group has developed a series of computational methods for SEI simulations in recent years,1 including the Hybrid ab initio molecular dynamics combined with reactive force fields (HAIR)2, the Kinetic Monte Carlo method for simulating lithium dendrite Kinetic Monte Carlo (KMC) method for simulating the growth of lithium dendrites, etc. Applying these methods, we have performed detailed theoretical simulations of the formation of the SEI interface and achieved some milestones, including (1) elucidation of the important initial decomposition reaction mechanism of solute and solvent (Fig. 1a);2 (2) revealing the formation process and structure of the initial inorganic LiF layer of SEI (Fig. 1b);3 (3) resolving the SEI solid-solid phase transition in all-solid-state batteries (Fig. 1b).4 The above theoretical simulation progress provides important theoretical guidance for the development of high energy density and high safety batteries, such as Li-Metal batteries, Li-Sulfur batteries, and all-solid-state batteries. Currently, the Battery open source package developed by the group has implemented most of the above functions.Reference[1] Cheng T; Jaramillo-Botero A; An Q; Ilyin DV; Naserifar S; Goddard WA*;Proc. Natl. Acad. Sci. U.S.A. 2019, 116, 18193.[2] Liu Y; Yu PP; Wu Y; Yang H; Miao X; Huai LY; Goddard WA*; Cheng T*; J. Phys. Chem. Lett. 2021, 12, 1300.[3] Liu Y; Sun QT; Yu PP; Wu Y; Xu L; Yang H; Xie M; Cheng T*; Goddard III WA; J. Phys. Chem. Lett. 2021,12, 2922.[4] Cheng T; Merinov BV*; Morozov S; Goddard WA; ACS Energy Lett. 2017, 2, 1454. Figure 1

Achieving high-performance in situ fabricated FAPbBr3 and electroluminescence.

Currently, metal halide perovskite films still encounter the issues of inferior film quality and interfacial electrical properties when they were constructed electroluminescence devices. Herein, efficient and pinhole-free perovskite emissive film was obtained on the poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) layer modified by an ultrathin LiF layer. Owing to the synergetic effect of the LiF interlayer, including better regulation of the perovskite film and a more balanced charge injection capability, an efficient green light-emitting diode based on the perovskite film was achieved with a maximum current efficiency of 25.6 cd/A, which is 58% higher than that of the control device with a plasma-treated PEDOT:PSS layer. Our results not only provide a facile strategy for acquiring efficient perovskite films but also circumvent the expensive and time-consuming plasma treatment process commonly used to improve the wetting properties of the underlying films.

High Interfacial-Energy and Lithiophilic Janus Interphase Enables Stable Lithium Metal Anodes.

The stability of solid electrolyte interphase (SEI) layers is critical for developing lithium (Li) metal batteries. However, the fabrication of stable SEI layers is plagued by un-controlled structures, properties, and functions. Here a controllable design of an ordered LiF-rich and lithiophilic hybrid Janus interphase (LiF-HJI) is reported using organic fluorination reagent as a functional SEI precursor. The LiF-HJI with a lower crystalline LiF layer and an upper Li organosulfide layer provides high interfacial energy with the Li metal and strong Li-ion affinity, allows homogenous Li-ion distribution, fast and uniform Li-ion transport, and excellent mechanical and passivation properties, enabling stable Li metal anodes under harsh conditions, such as high deposition capacities (6mAhcm-2 ), current densities (10mAcm-2 ), and rates (5 C). Stable LiF-HJI@Li greatly improves cycling stability and capacity retention (80.1% after 300 cycles) of Li||LiNi0.8 Co0.1 Mn0.1 O2 cells at a commercial-level areal capacity (≈4.2mAhcm-2 ). Even under a lean-electrolyte condition of 3gAh-1 , 80% capacity retention can be maintained after 100 cycles, demonstrating excellent cycling performance under such harsh conditions.