Li Metal Anode Research Articles

Improving the interfacial stability of Li1.2Mn0.54Ni0.13Co0.13O2 cathode and Li metal anode via dual electrolyte additives synergistic effect

Improving the interfacial stability of Li1.2Mn0.54Ni0.13Co0.13O2 cathode and Li metal anode via dual electrolyte additives synergistic effect

Synergistic dual-additive regulated carbonate electrolyte stabilizes bidirectional interface for aggressive Ni-rich Li-metal full batteries

The escalating energy demands underscore the importance of Ni-rich Li-metal batteries (LMBs); however, their aggressive bidirectional electrode-electrolyte interfacial issues hinder the practical implementation. Overcoming the limited solubility (∼800 ppm) of lithium nitrate (LiNO3) in commercially available carbonate electrolytes holds promise. Nevertheless, unintended effects caused by solubilizers raise emerging concerns. Herein, an additive solubilized additive strategy is introduced to synergistically stabilize the Ni-rich cathode and Li-metal anode (LMA) in carbonate electrolytes, where tris (2, 2, 2-trifluoroethyl) borate (TTFEB) as a solubilizer utilizes its electron-deficient B atom to snatch electron-rich NO3- anion of insoluble LiNO3 and thus forms a unique TTFEB-LiNO3 solvation structure in carbonate electrolytes. Valuably, the dual-additive electrolyte facilitates the formation of a robust LiF/Li3N-rich solid electrolyte interphase on LMA and a thin, uniform F, B, N-rich cathode electrolyte interphase on Ni-rich cathode, effectively suppressing the breeding of Li dendrites and mitigating the structure degradation of Ni-rich cathode. Consequently, the full cell, featuring a thin Li anode (50 µm) and a high-loading NCM811 cathode (4.04 mAh cm−2) in the dual-additive electrolyte, demonstrates a notable capacity retention of 81.5 % after 140 cycles. This work reveals the intricated LiNO3-carbonate solvation chemistry, inspiring further advancements in electrolyte engineering for practical LMBs.

Passivation Layers in Mg-Metal Batteries: Robust Interphases for Li-Metal Batteries.

In advanced batteries, interphases serve as the key component in stabilizing the electrolyte with reactive electrode materials far beyond thermodynamic equilibria. While an active interphase facilitates the transport of working ions, an inactive interphase obstructs ion flow, constituting the primary barrier to the realization of battery chemistries. Here, a successful transformation of a traditionally inactive passivating layer on Mg-metal anode, characteristic of Mg-metal batteries with typical carbonate electrolytes, into an active and robust interphase in the Li-metal scenario is presented. By further strategically designing magnesiated Li+ electrolytes, the in situ development of this resilient interphase on Li-metal anodes, imparting enduring stability to Li-metal batteries with nickel-rich cathodes is induced. It is identified that the strong affinity between Mg2+ and anions in magnesiated Li+ electrolytes assembles ionic clusters with a bias for reducibility, thereby catalyzing the creation of anion-derived interphases rich in inorganic constituents. The prevalence of ionic clusters induced by magnesiation of electrolytes has brought properties only available in high-concentration electrolytes, suggesting a fresh paradigm of tailing electrolytes for highly reversible LMBs.

Laser‐Constructing 3D Copper Current Collector with Crystalline Orientation Selectivity for Stable Lithium Metal Batteries

The practical application of lithium (Li) metal anodes in high‐capacity batteries is impeded by the formation of hazardous Li dendrites. To address this challenge, this research presents a novel methodology that combines laser ablation and heat treatment to precisely induce controlled grain growth within laser‐structured grooves on copper (Cu) current collectors. Specifically, this approach enhances the prevalence of Cu (100) facets within the grooves, effectively lowering the overpotential for Li nucleation and promoting preferential Li deposition. Unlike approaches that modify the entire surface of collectors, our work focuses on selectively enhancing lithiophilicity within the grooves to mitigate the formation of Li dendrites and exhibit exceptional performance metrics. The half‐cell with these collectors maintains a remarkable Coulombic efficiency of 97.42% over 350 cycles at 1 mA cm−2. The symmetric cell can cycle stably for 1600 h at 0.5 mA cm−2. Furthermore, when integrated with LiFePO4 cathodes, the full‐cell configuration demonstrates outstanding capacity retention of 92.39% after 400 cycles at a 1C discharge rate. This study introduces a novel technique for fabricating selective lithiophilic three‐dimensional (3D) Cu current collectors, thereby enhancing the performance of Li metal batteries. The insights gained from this approach hold promise for enhancing the performance of all laser‐processed 3D Cu current collectors by enabling precise lithiophilic modifications within complex structures.

Metal single-atom catalysts for stable Li metal anode: Principles, progress and perspectives

Metal single-atom catalysts for stable Li metal anode: Principles, progress and perspectives

Interfacial modulation of bifunctional electrolyte additive engineering for dendrite-free and robust lithium metal anode

Anode materials for rechargeable electric car batteries are obtained from Li-metal owing to their extremely high specific capacity and low redox potential. Unfortunately, safety concerns related to dendrite formation on the anode surface caused by the uneven distribution of Li-ions during the discharge process interfere with the use of Li-metal in industrial batteries. In this study, methyl vinyl sulfone (MVS), a sulfone-based functional electrolyte additive, is used in an additive engineering strategy to control Li-electrolyte interactions and address the aforementioned problems. Li dendrite growth may be restricted, and transition metal degradation on the surface of the cathode can be reduced by the MVS-derived functional electrolyte additive interfacial layer. The electrochemical performance of an ethylene carbonate/dimethyl carbonate (EC/DMC) + 1 wt% MVS Li-metal anode of a Li||Li symmetric cell exhibits remarkable cycle stability, maintaining a low overvoltage for over 750 h at 1 mA cm−2, and capacity of 1 mA h cm−2. Additionally, LiNi0.8Co0.1Mn0.1O2 (NCM811) full cells with the MVS additive exhibit enhanced electrochemical stability for 250 cycles at a current density of 100 mA g−1. This study provides an innovative approach for stabilizing the metal-electrolyte interfacial layer that may be used for practical applications in metal-based rechargeable batteries.

Cation-polymerized artificial SEI layer modified Li metal applied in soft-matter polymer electrolyte

Li metal batteries with polymer electrolyte are of great interest for next-generation batteries for high safety and high energy density. However, uneven deposition on the lithium metal surface can greatly affect battery life. Therefore, surface modification on the Li metal become necessary to achieve good performance. Herein, an artificial solid electrolyte interface (SEI) modified lithium metal anode is prepared using cation-polymerization process, as triggered by PF5 generated from CsPF6. As a result, the polarization voltage of Li||Li symmetric battery assembled with artificial SEI-modified Li metal anode was stable with a small over-potential of 25 mV after 3000 h at current density of 1.5 mA cm−2. Electrochemical performance of Li||NCM 622 (LiNi0.6Co0.2Mn0.2O2) full cell with soft-matter polymer electrolyte is significantly improved than bare Li-metal, the capacity retention is 75% after 120 cycles with N/P = 3:1 at a cut-off voltage of 4.3 V. Our work has shed lights on the commercialization of Li metal battery with polymer electrolyte.

Coupling of ion-conducting interphase with lithiophilic-solid-oxide-electrolyte interlayer toward fast-charging lithium metal batteries

The uncontrollable dendritic Li growth and limited Coulombic efficiency have long impeded the implementation of fast-charging lithium metal batteries. Contrary to the widely accepted attempt of using a sintering dense ceramic electrolyte to realize dendrite-free deposition, we report a coupling architecture of ion-conducting-Li3PO4-Li3N interphase with lithiophilic-solid-oxide-electrolyte interlayer for Li-metal anode using a reactive lithiophilic solid oxide electrolyte (RLSE) rather than dense ceramics. The synergistic interphase and protection layer can facilitate the Li-ion transport and enhance the lithiophilicity. As a result, an ultrahigh Li plating/stripping current density of 10 mA cm−2 and areal capacity of 10 mAh cm−2 for over 1000 h, and a remarkable Coulombic efficiency of 99.8 % are achieved simultaneously. Moreover, the use of interphase-interlayer synergistic protection enables a stable long-term 3000-cycling of Li||Li4Ti5O12 cell at 2C rate. More importantly, high-current–density (e.g. 1.8 mA cm−2) cycling of Li||LiNi0.8Co0.1Mn0.1O2 batteries with a practical area capacity of 3.6 mAh cm−2 is achieved in both carbonate and quasi-solid electrolytes. This study demonstrates an alternative approach of solid oxide electrolytes to stabilize Li-metal anode and enable fast-charging lithium metal batteries.

Multiple uniform lithium-ion transport channels in Li6.4La3Zr1.4Ta0.6O12/Ce(OH)3 modified polypropylene composite separator for high-performance lithium metal batteries

Lithium (Li) metal anodes (LMAs) are regarded as leading technology for advanced-generation batteries due to their high theoretical capacity and favorable redox potential. However, the practical integration of LMAs into high-energy rechargeable batteries is hindered by the challenge of Li dendrite growth. In this work, nanoparticles of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) loaded with Ce(OH)3 (LLZTCO) were designed and synthesized by a hydrothermal method. A functional composite separator was crafted by coating one side of a polypropylene (PP) separator with a composite electrolyte comprised of polyvinylidene fluoride (PVDF) and LLZTCO. The synergistic interactions between PVDF and LLZTCO provide numerous rapid lithium-ion (Li+) channels, facilitating the efficient redistribution of disparate Li+ flux originating from the insulated PP separator. The composite separator demonstrated an ionic conductivity (σ) of 3.68 × 10–3 S cm−1, substantial Li+ transference number (t+) of 0.73, and a high electrochemical window of 4.8 V at 25℃. Furthermore, the Li/LLZTCO@PP/Li symmetric cells demonstrated stable cycling for over 2000 h without significant dendrite formation. The Li/LiFePO4 (LFP) cells assembled with LLZTCO@PP separators exhibited a capacity retention of 91.6 % after 400 cycles at 1C. This study offers a practical approach to fabricating composite separators with enhanced safety and superior electrochemical performance.

Elucidating the role of polar functional groups in fluorinated polymer artificial interphase for stable lithium anodes

The properties of solid electrolyte interphase (SEI) are pivotal for stable lithium (Li) metal anodes. However, the process of formation and ion transport behavior of lithium fluoride (LiF) through the polar groups of organic fluorinated artificial SEI has not been clearly elucidated. Herein we demonstrate that the key role of polar functional groups in fluorinated polymer artificial SEI (FPASEI) is elucidated by using 2,2,2-trifluoroethylacrylate (TFEA) through radical polymerization. Density functional theory and ab initio molecular dynamics calculations demonstrate that the abundant CO polar groups in TFEA contribute a large number of electrons, thereby facilitating the degradation kinetics of CF bond cleavage in lithium bis(trifluoromethanesulfonyl)imide salt to yield LiF. Moreover, the presence of CF, COC, and CO groups in TFEA facilitate the migration of Li+ towards interchain regions through cation-dipole interaction, leading to dendrite-free Li deposition. The implementation of FPASEI in a Li||Li cell results in 500 h of Li plating/stripping cycling at 1 mA cm−2 and retains a capacity retention rate of 80 % after 265 cycles in Li||LiNi0.8Co0.1Mn0.1O2 cell. This study not only emphasizes the critical role of polar groups in artificial SEI but also presents a promising strategy for achieving stable Li metal batteries.

Design a polymer-based composite electrolyte with high ionic conductivity for high-performance lithium-metal batteries

Constructing a stable and robust solid polymer electrolyte (SPE) is crucial for achieving dendrite-free lithium-metal anodes and high-performance lithium batteries. However, realizing the integrity of solid electrolytes with high ion conductivity during long-life cycling under high current density remains a significant challenge. In this study, we propose a multifunctional SPE with a polyvinylidene fluoride (PVDF)/co-polyphenol coordination polymer (EACo2) hybrid composite to improve the durability of Li metal anode during repeat plating/stripping cycles by using a facile solution-casting method. The PVDF as a substrate with high mechanical strength and improved lithiophilicity exhibits high ionic conduction and excellent dendrite inhibition ability; meanwhile, the EACo2 fillers with a high density of Lewis-acidic sites contribute to the dissociation of lithium salts and decrystallization of the PVDF, resulting in a high Li-ion transference number and ion conductivity (2.66 × 10−3 S cm−1 at 30 ℃). The symmetrical cells with PVDF/EACo2 SPE can stabilize cycling over 1200 hours at a deposition capacity of 0.1 mAh cm−2. Moreover, the assembled full cells Li|LiFePO4 demonstrate long-term stability (1000 cycles at 1 C) with impressive capacity retention of 75 %, offering a promising approach towards high-performance lithium metal batteries.

Enhancing Lithium-Ion Diffusion Kinetics in a 3D Lithium Metal Host through Surface Modification with Hierarchical Multimetal Oxides.

Lithium metal is a promising anode candidate to achieve high-energy-density lithium metal batteries (LMBs) due to its ultrahigh theoretical capacity (3860 mA h g-1) and low electrochemical potential (-3.04 V vs S.H.E). Unfortunately, the commercialization of lithium metal anodes is hindered by the growth of Li dendrites and the infinite Li volume changes during the cycling process. Herein, we introduce a 3D hierarchical multimetal oxide nanowire framework as a current collector for Li metal anodes. The hierarchical metal oxide layers of CoO and CuxO provide abundant Li nucleation sites and thus offer uniform Li plating and regulate Li nucleation during the charge/discharge process. As a result, half cells present a prolonging Coulombic efficiency of 97% at 1 mA cm-2 with a capacity of 1 mA h cm-2 for over 300 cycles. A stable cyclability of symmetric cells is demonstrated under 1 mA cm-2 with a capacity of 1 mA h cm-2 for 1500 h. Full cells paired with an LFP cathode show a stable capacity of 131.5 mA h g-1 with a capacity retention of 92% for 200 cycles. These results will shed insights into the design of 3D Cu current collectors for high-performance composite Li metal anodes.

Realizing Ultrathin LiSn Alloy Anode by Tuning the Wettability of Molten Li for High-Energy-Density Batteries.

Despite being heralded as the "holy grail" of anodes for their high theoretical specific capacity, lithium (Li) metal anodes still face practical challenges due to difficulties in fabricating ultrathin Li with controllable thickness and suppressing Li dendrites growth. Herein, we introduce a simple and cost-effective dip-coating method to fabricate ultrathin lithium-tin (LiSn) anode with adjustable thicknesses ranging from 4.5 to 45 μm. The in situ formation of Li22Sn5 alloy improves the wettability of the molten Li, enabling the casting of ultrathin Li metal layers on different substrates. More importantly, the abundant Li22Sn5 lithiophilic sites significantly lower the nucleation overpotential, inducing uniform Li deposition and accelerating the electrochemical reaction at the interface. As a result, the symmetric cell assembled with LiSn-Cu electrodes can cycle stably for more than 120 h with a charge/discharge depth of 50%, which is 1.5 times longer than the lifespan of the pure Li anode. In the full cells paired with NCM cathode, the discharge specific capacity is improved from 13.84 to 70.31 mA h g-1 with the LiSn-Cu anode at 8 C. The LiSn-Cu||NCM full cell realized a high energy density of 724.9 Wh kg-1 at the active material level with an N/P ratio of 1.4.

Double-Salts Super Concentrated Carbonate Electrolyte Boosting Electrochemical Performance of Ni-Rich LiNi0.90Co0.05Mn0.05O2 Lithium Metal Batteries.

Current lithium-ion batteries cannot meet the requirement of higher energy density with further large-scale application of electrical vehicles. Lithium metal batteries combined with Ni-rich layered oxides cathode are expected as the one of promising solutions, while the poor electrode and electrolyte interface impedes the commercial development of lithium metal batteries. A new double-salts super concentrated (DSSC) carbonate electrolyte is proposed to improve the electrochemical performance of LiNi0.90Co0.05Mn0.05O2 (NCM9055)||Li metal battery which exhibits stable cycling performance with the capacity retention of 93.04% and reversible capacity of 173.8 mAh g-1 after 100 cycles at 1 C, while cells with conventional 1m diluted electrolyte remains only 60.55% and capacity of 114.2 mAh g-1. The double salts synergistic effect in super concentrated electrolyte promotes the formation for more balanced stable cathode electrolyte interface (CEI) inorganic compounds of CFx, LiNOx, SOF2, Li2SO4, and less LiF by X-ray photoelectron spectroscopy (XPS)test, and the uniform 2-3nm rock-salt phase protection layer on the cathode surface by transmission electron microscope (TEM) characterization, improving the cycling performance of the Ni-rich NCM9055 layered oxide cathode. The DSSC electrolyte also can relief the Li dendrite growth on Li metal anode, as well as exhibit better flame retardance, promoting the application of more safety Ni-rich NCM9055||Li metal batteries.

Lithium spreading layer consisting of nickel particles enables stable cycling of aluminum anode in all‐solid‐state battery

AbstractDeveloping promising substitutes of lithium (Li) metal anode that suffers from a serious interfacial instability against the solid electrolyte (SE) is a formidable challenge for the all‐solid‐state battery. Aluminum (Al), a highly potential candidate owing to its high specific capacity and relatively low working potential, however, cannot withstand stable cycling in all‐solid‐state battery due to the fast structural collapse caused by the solid/solid contact at the Al/SE interface. Herein, a Li spreading layer consisting of metallic nickel (Ni) particles at the Al surface is proposed to raise the performance of Al anode in all‐solid‐state battery. Owing to the immiscibility between Ni and Li solid phases, this Li spreading layer can enable a uniform distribution of Li atoms over the electrode surface followed by a stable Li–Al alloying/dealloying processes, suppressing the stress deformation at the Al/SE interface and significantly improving the cycling performance of Al anode in all‐solid‐state battery. The modified Al anode not only outperforms the bare Al significantly, but also exhibits superior cyclability and rate ability compared with the Li anode. This work provides an efficient strategy to promote the application of Al anode in all‐solid‐state battery, and is expected to be generalized for other alloy anodes.

Self-limiting lithium deposition enabled by synergistic surface chemical and structural engineering of Li metal anodes

Li metal is considered an ideal anode for the next-generation rechargeable batteries due to the high specific capacity and ultralow redox potential. However, the growth of Li dendrites severely impedes its application. In this study, a structural Li anode is constructed by decorating the copper phosphide nanowires modified copper mesh (PCM) on Li surface. A self-limiting Li deposition with dendrite-free feature is achieved based on the rational surface chemical and structural engineering of the Li anode. On the one hand, the meshed PCM layer as well as its lithiated species performs excellent lithiophilicity and favorable electron/ion conductivity, effectively reducing the Li nucleation barrier and redistributing the electric field and Li+ flux. This promotes a preferential and uniform Li deposition. On the other hand, the suitable combination between PCM and Li not only ensures excellent electrical contact for fast charge transfer, but also establishes a well-balanced structure with abundant active sites and large space for Li nucleation and deposition. Moreover, the meshed surface structure effectively accommodates the volume change of Li during plating/stripping. And the multiplied compressive stress between the PCM and separator greatly suppresses Li growth in vertical direction and promotes a dense Li morphology. Consequently, a self-limiting and highly reversible Li plating/stripping along the horizontal direction is achieved, even at a high areal capacity of 10 mA h cm–2. The Li deposition preferentially occurs on the PCM skeleton and gradually expands horizontally into the meshed space, without obvious formation of Li dendrites. The symmetrical cells show excellent cycling stability for over 1700 h with a low overpotential (13.1 mV at 1500 h) at 1 mA cm–2. Furthermore, the cells paired with LiNi0.6Co0.2Mn0.2O2 cathode also show excellent cycling stability for over 450 cycles.

Modeling of pulse and relaxation of high-rate Li/CFx-SVO batteries in implantable medical devices

We present a Hybrid Multiphase Porous Electrode Theory (Hybrid-MPET) model that accurately predicts the performance of Medtronic’s implantable medical device battery lithium/carbon monofluoride (CFx) - silver vanadium oxide (SVO) under both low-rate background monitoring and high-rate pulsing currents. The distinct properties of multiple active materials are reflected by parameterizing their thermodynamics, kinetics, and mass transport properties separately. Diffusion limitations of Li+ in SVO are used to explain cell voltage transient behavior during pulse and post-pulse relaxation. We also introduce change in cathode electronic conductivity, Li metal anode surface morphology, and film resistance buildup to capture evolution of cell internal resistance throughout multi-year electrical tests. We share our insights on how the Li+ redistribution process between active materials can restore pulse capability of the hybrid electrode, allow CFx to indirectly contribute to capacity release during pulsing, and affect the operation protocols and design principles of batteries with other hybrid electrodes. We also discuss additional complexities in porous electrode model parameterization and electrochemical characterization techniques due to parallel reactions and solid diffusion pathways across active materials. We hope our models can complement future experimental research and accelerate development of multi-active material electrodes with targeted performance.

Engineering High-Performance Li Metal Batteries through Dual-Gradient Porous Cu-CuZn Host.

Porous copper (Cu) current collectors show promise in stabilizing Li metal anodes (LMAs). However, insufficient lithiophilicity of pure Cu and limited porosity in three-dimensional (3D) porous Cu structures led to an inefficient Li-Cu composite preparation and poor electrochemical performance of Li-Cu composite anodes. Herein, we propose a porous Cu-CuZn (DG-CCZ) host for Li composite anodes to tackle these issues. This architecture features a pore size distribution and lithiophilic-lithiophobic characteristics designed in a gradient distribution from the inside to the outside of the anode structure. This dual-gradient porous Cu-CuZn exhibits exceptional capillary wettability to molten Li and provides a high porosity of up to 66.05%. This design promotes preferential Li deposition in the interior of the porous structure during battery operation, effectively inhibiting Li dendrite formation. Consequently, all cell systems achieve significantly improved cycling stability, including Li half-cells, Li-Li symmetric cells, and Li-LFP full cells. When paired synergistically with the double-coated LiFePO4 cathode, the pouch cell configured with multiple electrodes demonstrates an impressive discharge capacity of 159.3 mAh g-1 at 1C. We believe this study can inspire the design of future 3D Li anodes with enhanced Li utilization efficiency and facilitate the development of future high-energy Li metal batteries.

Synchronous regulation on solvation structure and interface engineering to enable reversible magnesium metal batteries

Magnesium (Mg) metal anodes are highly regarded as one of ideal substitutes for lithium (Li) metal anodes owing to their exceptional volumetric capacity, remarkable safety property, and abundant crustal reserves. However, the development of Mg batteries is severely impeded by the limited availability of electrolyte types, particularly non-nucleophilic ones. Mg(TFSI)2-based electrolyte is a recently discovered type of electrolyte which is non-nucleophilic, easily prepared, and highly stable. Nevertheless, due to its challenging de-solvation process and unexpected passivation interlayers, it is not performing as well electrochemically and requires effective modification. Here, organic amine dihydrochlorides (NCxN·2HCl) are selected as additives to Mg(TFSI)2-based electrolytes to regulate solvation structure and electrode interlayer synchronously. It helps rearrange the solvation sheath of Mg2+ and forms a Mg2+-permeable solid electrolyte interphase (SEI) on the surface of anode, facilitating the kinetic. Amine cations could also guide uniform Mg2+ deposition through electrostatic shielding effects. After experiments and simulations, ethylenediamine dihydrochloride (NCCN·2HCl) stands out, contributing to a significantly reduced overpotential (< 0.2 V), realizing about 100 % coulombic efficiency and stable long-term full cell cycling for an impressive 2400 cycles.

Fast Interfacial Defluorination Kinetics Enables Stable Cycling of Low-Temperature Lithium Metal Batteries.

The development of low-temperature lithium metal batteries (LMBs) encounters significant challenges because of severe dendritic lithium growth during the charging/discharging processes. To date, the precise origin of lithium dendrite formation still remains elusive due to the intricate interplay between the highly reactive lithium metal anode and organic electrolytes. Herein, we unveil the critical role of interfacial defluorination kinetics of localized high-concentration electrolytes (LHCEs) in regulating lithium dendrite formation, thereby determining the performance of low-temperature LMBs. We investigate the impact of solvation structures of LHCEs on low-temperature LMBs by employing tetrahydrofuran (THF) and 2-methyltetrahydrofuran (2-MeTHF) as comparative solvents. The combination of comprehensive characterizations and theoretical simulations reveals that the THF-based LHCE featured with a strong solvation strength exhibits fast interfacial defluorination reaction kinetics, thus leading to the formation of an amorphous and inorganic-rich solid-electrolyte interphase (SEI) that can effectively suppress the growth of lithium dendrites. As a result, the highly reversible Li metal anode achieves an exceptional Coulombic efficiency (CE) of up to ∼99.63% at a low temperature of -30 °C, thereby enabling stable cycling of low-temperature LMB full cells. These findings underscore the crucial role of electrolyte interfacial reaction kinetics in shaping SEI formation and provide valuable insights into the fundamental understanding of electrolyte chemistry in LMBs.