Lithiophilic Layer Research Articles

Controlling SnOx Stoichiometry via ALD Deposition on Cu Current Collectors: Investigating Stability and Reversibility Enhancement in Lithium Metal Batteries

Recent advancements in battery technology have led to the emergence of various types of secondary batteries with higher capacities to meet increasing demands. Among these, research on Lithium metal batteries (LMBs) with high capacity potential is actively pursued. However, LMBs face stability issues due to dendrite formation and low reversibility in Li plating-stripping processes. To address these challenges, we have modified the surface of Cu current collectors with lithiatable material, SnOx, to inhibit dendrite formation, enhance the stability and reversibility of LMBs. Furthermore, SnOx films reduce the overpotential of Li and enable stable Solid Electrolyte Interphase (SEI) formation. Therefore, they enhance the reversibility of Li plating/stripping processes. SnOx films were deposited via Thermal Atomic Layer Deposition (ALD) at 200°C with a thickness of 20nm. We have already reported the effectiveness of SnOx in enhancing the efficiency and stability of LMBs.[1] Therefore, in this study, we conducted research on the variation in characteristics of LMBs resulting from the control of stoichiometry in this lithiatable SnOx. Stoichiometry was adjusted through two methods. One method involved post-deposition heat treatment, where treatments were conducted at 400°C for one hour under H2 (H2 4%, Ar 96% gas) and N2 atmospheres. Additionally, we adjusted the injection time of H2O, the reactant in ALD, varying it from 1 to 3sec to create an oxygen deficient environment, and analyzed each characteristic accordingly. We will present our findings on the effect of SnOx stoichiometry on the performance and stability of LMBs.[1] Kim, Junghwan, et al. "Homogeneous Li Deposition guided by Ultra-thin Lithiophilic Layer for Highly Stable Anode-free Batteries." Energy Storage Materials (2023): 102899. Figure 1

Interface engineering enabling thin lithium metal electrodes down to 0.78 μm for garnet-type solid-state batteries

Controllable engineering of thin lithium (Li) metal is essential for increasing the energy density of solid-state batteries and clarifying the interfacial evolution mechanisms of a lithium metal negative electrode. However, fabricating a thin lithium electrode faces significant challenges due to the fragility and high viscosity of Li metal. Herein, through facile treatment of Ta-doped Li7La3Zr2O12 (LLZTO) with trifluoromethanesulfonic acid, its surface Li2CO3 species is converted into a lithiophilic layer with LiCF3SO3 and LiF components. It enables the thickness control of Li metal negative electrodes, ranging from 0.78 μm to 30 μm. Quasi-solid-state lithium-metal battery with an optimized 7.54 μm-thick lithium metal negative electrode, a commercial LiNi0.83Co0.11Mn0.06O2 positive electrode, and a negative/positive electrode capacity ratio of 1.1 shows a 500 cycles lifespan with a final discharge specific capacity of 99 mAh g−1 at 2.35 mA cm−2 and 25 °C. Through multi-scale characterizations of the thin lithium negative electrode, we clarify the multi-dimensional compositional evolution and failure mechanisms of lithium-deficient and -rich regions (0.78 μm and 7.54 μm), on its surface, inside it, or at the Li/LLZTO interface.

Toward High-Energy-Density Initial-Anode-Free Lithium-Metal Batteries via Ultra-Thin Protective Ion-Transport-Promoting Interface Modification and Surface Prelithiation.

Anode-free lithium-metal batteries (AFLMBs) are desirable candidates for achieving high-energy-density batteries, while severe active Li+ loss and uneven Li plating/stripping behavior impede their practical application. Herein, a trilaminar LS-Cu (LiCPON + Si/C-Cu)current collector is fabricated by radio frequency magnetron sputtering, including a Si/C hybrid lithiophilic layer and a supernatant carbon-incorporated lithium phosphorus oxynitride (LiCPON) solid-state electrolyte layer. Joint experimental and computational characterizations and simulations reveal that the LiCPON solid-state electrolyte layer can decompose into an in situ stout ion-transport-promoting protective layer, which can not only regulate homogeneous Li plating/stripping behavior but also inhibit the pulverization and deactivation of Si/C hybrid lithiophilic layer. When combined with surface prelithiated Li1.2Ni0.13Co0.13Mn0.54O2 (Preli-LRM) cathode, the Preli-LRM||LS-Cu full cell delivers 896.1Wh kg-1 initially and retains 354.1Wh kg-1 after 50 cycles. This strategy offers an innovative design of compensating for active Li+ loss and inducing uniform Li plating/stripping behavior simultaneously for the development of AFLMBs.

Constructing a Li–Zn lithiophilic layer by a scalable method of magnetron sputtering for a high-quality Li–B alloy anode

Lithium metal anodes offer high theoretical capacity and low redox potential but face challenges like dendritic growth, fragile solid electrolyte interface (SEI), "dead lithium" formation, and volume expansion. Composite anodes or artificial SEIs can address these issues, but often suffer from poor lithiophilicity and mass burdens. This study presents a Li–Zn–B alloy anode combining a Li–Zn lithiophilic layer with a bulk Li–B alloy. The Li–Zn lithiophilic layer, formed by magnetron sputtering of Zinc oxide (ZnO), improves surface lithiophilicity. Symmetrical cells with this alloy cycled stably for 1300 (1 mA cm−2, 1 mAh cm−2) and 550 h (2 mA cm−2, 2 mAh cm−2) with minimal overpotentials. The LiBZn||NCM811 full cell showed a specific discharge capacity of 130.8 mAh/g and stable Coulombic efficiency of 98.9 % after 300 cycles.

Constructing Sn-Cu2O Lithiophilicity Nanowires as Stable and High-Performance Lithium Metal Anodes.

Lithium (Li) metal batteries (LMBs) have garnered significant research attention due to their high energy density. However, uncontrolled Li dendrite growth and the continuous accumulation of "dead Li" directly lead to poor electrochemical performance in LMBs, along with serious safety hazards. These issues have severely hindered their commercialization. In this study, a lithiophilic layer of Sn-Cu2O is constructed on the surface of copper foam (CF) grown with Cu nanowire arrays (SCCF) through a combination of electrodeposition and plasma reduction. Sn-Cu2O, with excellent lithiophilicity, reduces the Li nucleation barrier and promotes uniform Li deposition. Simultaneously, the high surface area of the nanowires reduces the local current density, further suppressing the Li dendrite growth. Therefore, at 1 mA cm-2, the half cells and symmetric cells achieve high Coulombic efficiency (CE) and stable operation for over 410 cycles and run smoothly for more than 1350 h. The full cells using an LFP cathode demonstrate a capacity retention rate of 90.6% after 1000 cycles at 5 C, with a CE as high as 99.79%, suggesting excellent prospects for rapid charging and discharging and long-term cyclability. This study provides a strategy for modifying three-dimensional current collectors for Li metal anodes, offering insights into the construction of stable, safe, and fast-charging LMBs.

Rapid Growth of Bi2Se3 Nanodots on MXene Nanosheets at Room Temperature for Promoting Sulfur Redox Kinetics.

Li-S batteries are hampered by problems with their cathodes and anodes simultaneously. The improvement of Li-S batteries needs to consider both the anode and cathode. Herein, a Bi2Se3@MXene composite is prepared for the first time by rapidly growing Bi2Se3 nanodots on two-dimensional (2D) MXene nanosheets at room temperature through simply adding high-reactive hydroxyethylthioselenide in Bi3+/MXene aqueous solution. Bi2Se3@MXene exhibits a 2D structure due to the template effect of 2D MXene. Bi2Se3@MXene can not only facilitate the conversion of lithium polysulfides (LiPSs) but also inhibit their shuttling in the S cathode due to its catalytic effect and adsorption force with LiPSs. Bi2Se3@MXene can also be used as an interfacial lithiophilic layer to inhibit Li dendrite growth in the Li metal anode. Theoretical calculations reveal that Bi2Se3 nanodots in Bi2Se3@MXene can effectively boost the adsorption ability with LiPSs, and the MXene in Bi2Se3@MXene can accelerate the electron transport. Under the bidirectional regulation of Bi2Se3@MXene in the Li metal anode and S cathode, the Li-S battery shows an enhanced electrochemical performance.

Recent Progress of Advanced Functional Separators in Lithium Metal Batteries.

As a representative in the post-lithium-ion batteries (LIBs) landscape, lithium metal batteries (LMBs) exhibit high-energy densities but suffer from low coulombic efficiencies and short cycling lifetimes due to dendrite formation and complex side reactions. Separator modification holds the most promise in overcoming these challenges because it utilizes the original elements of LMBs. In this review, separators designed to address critical issues in LMBs that are fatal to their destiny according to the target electrodes are focused on. On the lithium anode side, functional separators reduce dendrite propagation with a conductive lithiophilic layer and a uniform Li-ion channel or form a stable solid electrolyte interphase layer through the continuous release of active agents. The classification of functional separators solving the degradation stemming from the cathodes, which has often been overlooked, is summarized. Structural deterioration and the resulting leakage from cathode materials are suppressed by acidic impurity scavenging, transition metal ion capture, and polysulfide shuttle effect inhibition from functional separators. Furthermore, flame-retardant separators for preventing LMB safety issues and multifunctional separators are discussed. Further expansion of functional separators can be effectively utilized in other types of batteries, indicating that intensive and extensive research on functional separators is expected to continue in LIBs.

Homogeneous Li deposition guided by ultra-thin lithiophilic layer for highly stable anode-free batteries

Li-metal batteries (LMBs) are intensively studied to keep up with the growing demand for sustainable and high-capacity energy storage devices. However, the practical implementation of LMBs is still challenging owing to the catastrophic side effects associated with the growth of dendritic Li and inferior Coulombic efficiency. To enhance the long-term electrochemical stability and high-rate performance of LMBs, it is crucial to control the morphology of Li deposition over the current collectors. Herein, we propose surface-modified current collectors to investigate how a lithiatable layer affects the morphology of Li deposition and thus contributes to the stable electrochemical performance of LMBs at high current densities. The lithiatable layer improves the electrolyte wetting ability, which efficiently diminishes the interfacial resistance between electrode and electrolyte. Moreover, the lithiatable layer induces homogeneous Li nucleation, consequently leading to the uniform Li deposition over the surface of current collectors. Due to these synergistic effects, the anode-free cells with surface-modified current collectors have achieved excellent cycle stability in comparison to that with conventional Cu current collector.

Constructing porous nickel-zinc alloy layer on nickel foam for dendritic-free lithium metal anode

The uncontrollable growth of lithium (Li) dendrites and continuous accumulation of “dead Li” directly lead to poor electrochemical performance concominantly with serious safety hazards of Li metal batteries (LMBs). Herein, a porous NiZn alloy lithiophilic layer (P-NiZn) is fabricated on the surface of nickel foam (NF), P-NiZn@NF, by electrodeposition, heating and subsequent selective etching. The NiZn alloy with excellent lithiophilicity contributes to the lower Li nucleation barrier and uniform Li deposition, while its porous structure enables reduced local current density that is beneficial to inhibit the growth of Li dendrites. Accordingly, the symmetrical cells can run stably for 2500 h at 0.5 mA cm−2, and the full-cell with LiFePO4 electrode achieves an excellent capacity retention of 86% over 600 cycles at 2 C with a high Coulombic efficiency (CE) of 99.98%. This work provides a promising idea for the surface modification of 3D current collectors for Li metal anodes which enlightens the construction of high-energy, stable, and safe LMBs.

Mediating Lithium Plating/Stripping by Constructing 3D Au@Cu Pentagonal Pyramid Array

Lithium (Li) metal is perceived as the “holy grail” of anodes for secondary batteries due to its innate merits. Regrettably, the commercial application of Li metal anodes (LMAs) has been hampered by problems derived from the uncontrollable growth of Li dendrites, which could result in formation of short-circuits, thereby leading to fatal safety accidents. Here, a three-dimensional lithiophilic gold (Au)-coated copper (Cu) pentagonal pyramid array (Au@CuPPA) is constructed on planar Cu foil via electrodeposition followed by a chemical reduction method. Owing to the features of the lithiophilic layer and 3D porous structure, the proposed Au@CuPPA can not only facilitate Li-ion migration and charge transfer, but also effectively diminish the nucleation overpotential. Consequently, an even and steady Li plating/stripping process for up to 460 h and with a charge capacity of 3 mAh cm−2 is accomplished by using the Au@CuPPA current collector. The Li@Au@CuPPA|LiFePO4 full cell achieves a high Coulombic efficiency (CE) of 99.4% for 150 cycles at 0.5 C with a capacity retention of 92.4%.

Hierarchical porous and lithiophilic CuMn current collector for advanced lithium metal batteries

Lithium metal faces serious problems such as dendrite growth and volume expansion, which make lithium metal batteries lose the opportunity in commercialization. Herein, we report a simple route to prepare a hierarchical porous CuMn (hp-CuMn) current collector (CC) with an epitaxially grown lithiophilic layer to solve these problems. The hp-CuMn with industrialization potential can achieve uniform current distribution and geometric constraints. Meanwhile, the epitaxially grown MnO by annealing the hp-CuMn with surface absorbed oxygen in reductive atmosphere effectively improves the interfacial bonding force and lithiophilicity. Consequently, the hp-CuMn@MnO with thickness about 85 μm (can store Li of 14.45 mAh cm−2 by molten lithium injection, 5 times of the graphite anode) have a small hysteresis voltage and can be stable for up to 1500 h. Full cells with LiFePO4 display ultrahigh capacity retention ratio (96.8 %) after 600 cycles at 2 C, and has good compatibility with the current industry, which verifies the application value.

One step hot-pressing method for hybrid Li metal anode of solid-state lithium metal batteries

Safety issues induced by infinite anode volume change and uncontrolled lithium (Li) dendrite growth have become the biggest obstacle to the practical application of Li metal batteries. In addition, the traditional rolling method makes it difficult to manufacture thin Li foil with high mechanical strength and low Li content. Herein, a three-dimensional (3D) lithophilic carbon paper/copper (Cu) current collector hybrid anode with ultra-low Li metal content is prepared by a hot-pressing method. The highly reversible and stable lithiophilic layer LiCx formed in situ by heating/pressing treatment provides abundant nucleation sites and reduces the Li nucleation overpotential, thereby effectively suppressing Li dendrite growth. Moreover, the volume change and pulverization problems of Li metal anode during deposition/stripping also can be accommodated by the 3D skeleton. The optimization effect has been directly confirmed by in-situ optical and ex-situ scanning electron microscope observation. Therefore, highly stable performance (158.4 mA h g−1 at 2 C after 200 cycles with a capacity retention of 95.24%) in Li@LCP-Cu||NCM811 coin cell can be achieved. Furthermore, the solid-state battery assembled with the hybrid anode, poly(vinylidene fluoride) (PVDF)-based polymer electrolyte and polyethylene oxide (PEO) interface functional layer also exhibits the best electrochemical and safety performance, which also proves that the Li@LCP-Cu anode has great potential for application in solid-state batteries.

Uniform lithium deposition guided by Au nanoparticles in vertical-graphene/carbon-cloth skeleton for dendrite-free and stable lithium metal anode

Owing to the high electrochemical reactivity and infinite volume expansion of lithium metal anode, the uncontrollable lithium dendrite growth drags the lithium metal anode out of the real application for a long time. Herein, a heterogeneous seed layer of Au nanoparticles (NPs) is uniformly deposited on the 3D porous vertical graphene nanosheets on carbon cloth (Au-VG/CC) to construct a lithiophilic surface, achieving a smooth and dendrite-free morphology. As a result, Au-VG/CC electrode delivers a small voltage hysteresis of 67.2 mV and a long cycling life of more than 500 h at a high current density of 5 mA cm−2 with 5 mAh cm−2. Results of XRD and in-situ transmission electron microscopy indicate that the formed lithiophilic layer is Li3Au which can guide the lithium deposition. Moreover, a full battery assembled with Li@Au-VG/CC as the anode and LiFePO4 as the cathode delivers 77.3 mAh g−1 at 100 mA g−1 after 200 cycles.

In-situ formation of LiF-rich solid-electrolyte interphases on 3D lithiophilic skeleton for stable lithium metal anode

Lithium (Li) metal with high theoretical capacity is considered as one of the important anode materials for the next-generation high-energy density batteries. However, the further commercial application of Li metal anode is hindered by the severe growth of uncontrollable Li dendrites and the destructive regrowth of unstable solid-electrolyte interphases (SEI) layer. Herein, through the combination of thin film deposition coating and in-situ fluoridation, a composite layer with the lithophilic layer and the LiF-rich SEI layer is realized on Cu foam current collector. Specifically, the lithiophilic layer on the surface of current collector helps to regulate the homogeneous Li plating/stripping behavior. More importantly, after in-situ fluoridation, the LiF-rich layer as a robustly artificial SEI can be in-situ generated on the surface of current collector during initial activation process to stabilize cycling performance with dendrite-free. Consequently, the well-designed 3D current collector enables dendrite-free Li deposition behavior, high average coulombic efficiency (97.74% for 500 cycles at 1 mA cm−2 & 1 mAh cm−2), stable Li plating/stripping behavior (over 2400 h with an ultra-low overpotential of 10 mV at 2 mA cm−2 & 2 mAh cm−2) and remarkable cycling stability/rate performance in both coin-type and pouch full cells. These encouraging results provide new insights into the design of high-performance Li metal anodes for the development of Li metal batteries.

Roll-To-Roll Fabrication of Zero-Volume-Expansion Lithium-Composite Anodes to Realize High-Energy-Density Flexible and Stable Lithium-Metal Batteries.

The lithium (Li)-metal anode offers a promising solution for high-energy-density lithium-metal batteries (LMBs). However, the significant volume expansion of the Li metal during charging results in poor cycling stability as a result of the dendritic deposition and broken solid electrolyte interphase. Herein, a facile one-step roll-to-roll fabrication of a zero-volume-expansion Li-metal-composite anode (zeroVE-Li) is proposed to realize high-energy-density LMBs with outstanding electrochemical and mechanical stability. The zeroVE-Li possesses a sandwich-like trilayer structure, which consists of an upper electron-insulating layer and a bottom lithiophilic layer that synergistically guides the Li deposition from the bottom up, and a middle porous layer that eliminates volume expansion. This sandwich structure eliminates dendrite formation, prevents volume change during cycling, and provides outstanding flexibility to the Li-metal anode even at a practical areal capacity over 3.0mAhcm-2 . Pairing zeroVE-Li with a commercial NMC811 or LCO cathode, flexible LMBs that offer a record-breaking figure of merit (FOM, 45.6), large whole-cell energy density (375WhL-1 , based on the volume of the anode, separator, cathode, and package), high-capacity retention (> 99.8% per cycle), and remarkable mechanical robustness under practical conditions are demonstrated.

Electrosynthesis of Vertically Aligned Zinc Oxide Nanoflakes on 3D Porous Cu Foam Enables Dendrite-Free Li-Metal Anode.

Three dimensional (3D) hosts have been recognized as effective current collectors for Li metal anodes because of their physical suppression of the lithium dendrites growth. A lithiophilic surface layer on them could increase the Li metal nucleation sites, further regulating the genuine plating of Li metal. The current strategies to construct this lithiophilic layer on 3D structure is complex and not suitable for the scalable fabrication of Li metal anode. In this work, we developed a facile method to grow vertically aligned ZnO nanoflakes on the surface of 3D Cu foam through an electrochemical synthetic process, which physically suppressed the Li dendrites growth due to the unique structure during the Li plating/stripping process. Moreover, these lithiophilic flakes effectively increase the specific surface area of the anode and Li metal nucleation sites number, which reduces the local current densities, leading to the formation of a robust SEI and further suppressing the Li dendrites growth. Consequently, the performances of the symmetric Li plated Cu foam/Li cell and the Li plated Cu foam/LiFePO4 full cell have been greatly enhanced after the growth of vertically aligned ZnO nanoflakes on the Cu foam surface, including capacity, cycling stability, overpotential, and rate capability.

Ultralow‐Expansion Lithium Metal Composite Anode via Gradient Framework Design

AbstractImproving the stability of lithium (Li) anodes is critical for the safety and reliability of Li metal batteries. Developing a 3D conductive Li host is suggested as one of the most promising strategies in this context, especially for suppressing the pulverization of the electrode. However, the material consistency and volume expansion of the electrodes (<15%) represent significant challenges for their applications in commercial pouch cells. In this work, dual‐gradient architecture, combining rigidity and flexibility through the synergistic effect of silver wires and carbon nanotubes, is fabricated by a facile suction filtration method. This unique network shows a volume expansion of only 5.4%, outperforming all previously reported composite Li anodes. In addition, the online digital holography clearly monitors the preferential deposition of metallic Li at the lithiophilic layer. Consequently, the present gradient host effectively prevents the deposition of metallic Li at the electrode/separator interface, resulting in excellent cycling stability in both symmetric and full cells.

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.

Stable lithium metal anode achieved by shortening diffusion path on solid electrolyte interface derived from Cu2O lithiophilic layer

• We found the lithiation of Cu 2 O film would participate in the SEI generation. • The thickness of Cu 2 O film can affect Li + diffusion path in the derived SEI layer. • The oxidation state/thickness of Cu 2 O film can be tuned by oxygen plasma rapidly. The stable operation of lithium metal batteries is crucial for high energy density requirements, but it is plagued by Li dendrite growth and unstable solid electrolyte interphase (SEI). Lithiophilic transition metal oxides (TMOs) have been studied extensively on Cu current collectors to stabilize lithium metal anodes by decreasing the Li nucleation overpotential, yet less is known about the SEI derived from the lithiation reaction of TMOs. Here we report a novel approach to regulate the SEI interface precisely, especially to construct a nanoscale inorganic-dominated SEI with shortened diffusion path by controlling the oxidization state of Cu 2 O film on Cu current collector. The highly stable cyclic performance is achieved by generating the thin SEI that contains dense inorganic inner layer and organic layer. Consequently, the lithium metal anode based on Cu 2 O/Cu current collector exhibits low and stable polarization voltage for an ultralong life-span (∼22.5 mV at 1 mA cm −2 for 3000 h). This work elucidates the relationship between lithiation reaction of oxides modified layer and derived SEI, guiding for constructing stable lithium metal batteries.

Uniform lithiophilic layers in 3D current collectors enable ultrastable solid electrolyte interphase for high-performance lithium metal batteries

Uniform lithium plating/stripping during charging/discharging in 3D lithiophilic current collectors (3DLCC) is essential to suppress growth of lithium dendrites and to mitigate infinite volume variations of lithium metal for long-lived lithium metal batteries. This study reveals the decisive role played by uniformity of the lithiophilic layer of the 3DLCC in achieving uniform lithium plating/stripping. Herein, a series of metal oxide-based 3DLCCs are successfully fabricated with a simple and an ultrafast solution combustion method, from which formation of a uniform and stable lithium dendrite-free solid electrolyte interphase via a uniform lithiophilic layer is demonstrated. Taking Co3O4 as the lithiophilic material deposited on a nickel foam as the 3DLCC (Co@NF) for a proof of concept, the loading amount of Co3O4, closely correlated with the uniformity of the Co3O4 layer, is modulated to optimize its lithium ion hosting performances. With a uniform Co3O4 layer grown in the 3DLCC, an ultralow nucleation overpotential of 33.4 mV is achieved in half-cell tests at 1 mA cm−2 and 1 mAh cm−2, and a high Coulombic efficiency of 97.1% is maintained after 210 cycles under a severe cycling condition of 2 mA cm−2 and 1 mAh cm−2. A small polarization voltage of 13 mV together with an ultralong cycle life of 2400 h at 0.5 mA cm−2 and 1 mAh cm−2 in symmetric Li cells is achieved. Moreover, the composite Li anode delivers sensational rate capability and cyclability in full-cells. This work not only provides new and valuable insights into the interphasial chemistry of solid electrolyte interphase layers, but also sheds light on the development of ultrastable lithium metal batteries.