Rational design of F,N-rich artificial interphase via chemical prelithiation initiation strategy enabling high coulombic efficiency and stable micro-sized SiO anodes

Silicon monoxide(SiO)is regarded as a potential candidate for anode materials of lithium-ion batteries(LIBs).Unfortunately,the application of SiO is limited by poor initial Coulombic efficiency(ICE)and unsteady solid electrolyte interface(SEI),which induce low energy,short cycling life,and poor rate properties.To address these drawbacks of SiO,we achieve in-situ construction of robust and fast-ion conducting F,N-rich SEI layer on prelithiated micro-sized SiO(P-μSiO)via the simple and continuous treatment ofμSiO in mild lithium 4,4′-dimethylbiphenyl solution and nonflammable hexafluorocyclotriphosphazene solution.Chemical prelithiation eliminates irreversible capacity through pre-forming inactive lithium silicates.Meanwhile,the symbiotic F,N-rich SEI with good mechanical stability and fast Li^(+)permeability is conductive to relieve volume expansion ofμSiO and boost the Li+diffusion kinetics.Consequently,the P-μSiO realizes an impressive electrochemical performance with an elevated ICE of 99.57%and a capacity retention of 90.67%after 350 cycles.Additionally,the full cell with P-μSiO anode and commercial LiFePO_(4) cathode displays an ICE of 92.03%and a high reversible capacity of 144.97 mA h g^(-1).This work offers a general construction strategy of robust and ionically conductive SEI for advanced LIBs.

Activation mechanism of conventional electrolytes with amine solvents:Species evolution and hydride-containing interphase formation

Rechargeable magnesium(Mg)-metal batteries have brought great expect to overcome the safety and energy density concerns of typical lithium-ion batteries.However,interracial passivation of the Mgmetal anode impairs the reversible Mg plating/stripping chemistries,resulting in low Coulombic efficiency and large overpotential.In this work,a facile isobutylamine(IBA)-assisted activation strategy has been proposed and the fundamental mechanism has been unveiled in a specific way of evolving active species and forming MgH_(2)-based solid-electrolyte interphase.After introducing IBA into a typical electrolyte of magnesium bis(trifluoromethanesulfo nyl) imide(Mg(TFSI)_(2)) in diglyme(G2) solvents,electrolyte species of [Mg^(2+)(IBA)5]^(2+) and protonated amine-based cations of [(IBA)H]^(+) have been detected by nuclear magnetic resonance and mass spectra.This not only indicates direct solvation of IBA toward Mg^(2+)but also suggests its ionization,which is central to mitigating the decomposition of G2 and TFSI anions by forming neutrally charged [(IBAH^(+))(TFSI^(-))]~0 and other complex ions.A series of experiments,including cryogenic-electron microscopy,D_(2)O titration-mass spectra,and time of flight secondary ion mass spectrometry results,reveal a thin,non-passivated,and MgH_(2)-containing interphase on the Mg-metal anode.Besides,uniform and dendrite-free Mg electrodeposits have been revealed in composite electrolytes.Benefiting from the activation effects of IBA,the composite electrolyte displays superior electrochemical performance(overpotential is approximately 0.16 V versus 2.00 V for conventional electrolyte;Coulombic efficiency is above 90% versus <10% for conventional electrolyte).This work offers a fresh direction to advanced electrolyte design for next-generation rechargeable batteries.

Anchoring polysulfide with artificial solid electrolyte interphase for dendrite-free and low N/P ratio Li-S batteries

Lithium sulfur batteries are regarded as a promising candidate for high-energy-density energy storage devices.However,the lithium metal anode in lithium-sulfur batteries encounters the problem of lithium dendrites and lithium metal consumption caused by polysulfide corrosion.Herein we design a dualfunction PMMA/PPC/LiNO3composite as an artificial solid electrolyte interphase(PMCN-SEI)to protect Li metal anode.This SEI offers multiple sites of C=O for polysulfide anchoring to constrain corrosion of Li metal anode.The lithiated polymer group and Li3N in PMCN-SEI can homogenize lithium-ion deposition behavior to achieve a dendrite-free anode.As a result,the PMCN-SEI protected Li metal anode enables the Li||Li symmetric batteries to maintain over 300 cycles(1300 h)at a capacity of 5 m Ah cm^(-2),corresponding to a cumulative capacity of 3.25 Ah cm^(-2).Moreover,Li-S batteries assembled with 20μm of Li metal anode(N/P=1.67)still deliver an initial capacity of 1166 m A h g-1at 0.5C.Hence,introducing polycarbonate polymer/inorganic composite SEI on Li provides a new solution for achieving the high energy density of Li-S batteries.

Electrolyte design for Li-conductive solid-electrolyte interphase enabling benchmark performance for all-solid-state lithium-metal batteries

Sulfide-based solid-state electrolytes (SSEs) with high Li+ conductivity (δLi^(+)) and trifling grain boundaries have great potential for all-solid-state lithium-metal batteries (ASSLMBs). Nonetheless, the in-situ development of mixed ionic-electronic conducting solid-electrolyte interphase (SEI) at sulfide electrolyte/Li-metal anode interface induces uneven Li electrodeposition, which causes Li-dendrites and void formation, significantly severely deteriorating ASSLMBs. Herein, we propose a dual anionic, e.g., F and N, doping strategy to Li7P3S11, tuning its composition in conjunction with the chemistry of SEI. Therefore, novel Li_(6.58)P_(2.76)N_(0.03)S_(10.12)F_(0.05) glass-ceramic electrolyte (Li_(7)P_(3)S_(11-5)LiF-3Li_(3)N-gce) achieved superior ionic (4.33 mS·cm^(−1)) and lowest electronic conductivity of 4.33 × 10^(−10) S·cm^(−1) and thus, offered superior critical current density of 0.90 mA·cm^(−2) (2.5 times 】Li7P3S11) at room temperature (RT). Notably, Li//Li cell with Li6.58P2.76N0.03S10.12F0.05-gce cycled stably over 1000 and 600 h at 0.2 and 0.3 mA·cm^(−2) credited to robust and highly conductive SEI (in-situ) enriched with LiF and Li3N species. Li3N’s wettability renders SEI to be highly Li+ conductive, ensures an intimate interfacial contact, blocks reductive reactions, prevents Li-dendrites and facilitates fast Li+ kinetics. Consequently, LiNi0.8Co0.15Al0.05O_(2) (NCA)/Li_(6.58)P_(2.76)N_(0.03)S_(10.12)F_(0.05)-gce/Li cell exhibited an outstanding first reversible capacity of 200.8/240.1 mAh·g^(−1) with 83.67% Coulombic efficiency, retained 85.11% of its original reversible capacity at 0.3 mA·cm^(−2) over 165 cycles at RT.

The influence of formation temperature on the solid electrolyte interphase of graphite in lithium ion batteries

Lithium-ion battery has greatly changed our lifestyle and the solid electrolyte interphase(SEI)covered on the graphite anode determines the service life of a battery.The formation method and the formation temperature at initial cycle of a battery determine the feature of the SEI.Herein,we investigate the gap of formation behavior in both a half cell(graphite matches with lithium anode)and a full cell(graphite matches with NCM,short for LiNixCoyMn1-x-yO2)at different temperatures.We conclude that high temperature causes severe side reactions and low temperature will result in low ionic conductive SEI layer,the interface formed at room temperature owns the best ionic conductivity and stability.

In-situ formation of hierarchical solid-electrolyte interphase for ultra-long cycling of aqueous zinc-ion batteries

Aqueous rechargeable zinc ion batteries have received widespread attention due to their high energy density and low cost.However,zinc metal anodes face fatal dendrite growth and detrimental side reactions,which affect the cycle stability and practical application of zinc ion batteries.Here,an in-situ formed hierarchical solid-electrolyte interphase composed of InF3,In,and ZnF2 layers with outside-in orientation on the Zn anode(denoted as Zn@InF3)is developed by a sample InF3 coating.The inner ultrathin ZnF2 interface between Zn anode and InF3 layer formed by the spontaneous galvanic replacement reaction between InF3 and Zn,is conductive to achieving uniform Zn deposition and inhibits the growth of Zinc dendrites due to the high electrical resistivity and Zn2+conductivity.Meanwhile,the middle uniformly generated metallic In and outside InF3 layers functioning as corrosion inhibitor suppressing the side reaction due to the waterproof surfaces,good chemical inactivity,and high hydrogen evolution overpotential.Besides,the as-prepared zinc anode enables dendrite-free Zn plating/stripping for more than 6,000 h at nearly 100%coulombic efficiency(CE).Furthermore,coupled with the MnO2 cathode,the full battery exhibits the long cycle of up to 1,000 cycles with a low negative-to-positive electrode capacity(N/P)ratio of 2.8.

A robust interphase via in-situ pre-reconfiguring lithium anode surface for long-term lithium-oxygen batteries

Lithium-oxygen(Li-O) battery is considered as one of the most promising alternatives because of its ultrahigh theoretical energy density. However, their cycling stability is severely restricted by the uncontrollable dendrite growth and serious oxygen corrosion issue on Li surface. Herein, a sulfur-modified Li surface can be successfully constructed via chemical reaction of guanylthiourea(GTU) molecule on Li,which can induce the selectively fast decomposition of lithium bis(trifluoromethanesulfonyl)imide(LiTFSI) to form a smooth and stable inorganics-rich solid-electrolyte interphase(IR-SEI) during the subsequent electrochemical process. Such an IR-SEI cannot only offer a highly reversible and stable Li plating/stripping chemistry with dendrite-free property(10 mA cm^(-2)-10 mAh cm^(-2), > 0.5 years;3 mA cm^(-2)-3 m Ah cm^(-2), > 1 year) but also endows the Li metal an anti-oxygen corrosion function, thereby significantly improving the cycling stability of Li-Obatteries. This work provides a new idea for constructing functional solid-electrolyte interphase(SEI) to achieve highly stable Li metal anode.

Enabling an Inorganic-Rich Interface via Cationic Surfactant for High-Performance Lithium Metal Batteries

An anion-rich electric double layer(EDL)region is favorable for fabricating an inorganic-rich solid-electrolyte interphase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium bromide(CTAB),a cationic surfactant,is adopted to draw more anions into EDL by ionic interactions that shield the repelling force on anions during lithium plating.In situ electrochemical surface-enhanced Raman spectroscopy results combined with molecular dynamics simulations validate the enrichment of NO_(3)^(−)/FSI−anions in the EDL region due to the positively charged CTA^(+).In-depth analysis of SEI structure by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results confirmed the formation of the inorganic-rich SEI,which helps improve the kinetics of Li^(+)transfer,lower the charge transfer activation energy,and homogenize Li deposition.As a result,the Li||Li symmetric cell in the designed electrolyte displays a prolongated cycling time from 500 to 1300 h compared to that in the blank electrolyte at 0.5 mA cm^(-2) with a capacity of 1 mAh cm^(-2).Moreover,Li||LiFePO_(4) and Li||LiCoO_(2) with a high cathode mass loading of>10 mg cm^(-2) can be stably cycled over 180 cycles.

Regulating interfacial stability of SiO_(x) anode with fluoride-abundant solid–electrolyte interphase by fluorine-functionalized additive

Silicon oxide(SiO_(x))has received remarkable attention as a next-generation battery material;however,the sudden decrease in the cycling retention constitutes a significant challenge in facilitating its application.Tris(2,2,2-trifluoroethyl)phosphite(TTFP),which can control parasitic reactions such as the pulverization of SiO_(x)anode materials and electrolyte decomposition,has been proposed to improve the lifespan of the cell.The electrochemical reduction of TTFP results in solid-electrolyte interphase(SEI)layers that are mainly composed of LiF,which occur at a higher potential than the working potential of the SiO_(x)anode and carbonate-based solvents.The electrolyte with TTFP exhibited a substantial improvement in cycling retention after 100 cycles,whereas the standard electrolyte showed acutely decreased retention.The thickness of the SiO_(x)anode with TTFP also changed only slightly without any considerable delamination spots,whereas the SiO_(x)anode without TTFP was prominently deformed by an enormous volume expansion with several internal cracks.The cycled SiO_(x)anode with TTFP exhibited less increase in resistance after cycling than that in the absence of TTFP,in addition to fewer decomposition adducts in corresponding X-ray photoelectron spectroscopy(XPS)analyses between the cycled SiO_(x)anodes.These results demonstrate that TTFP formed SEI layers at the SiO_(x)interface,which substantially reduced the pulverization of the SiO_(x)anode materials;in addition,electrolyte decomposition at the interface decreased,which led to improved cycling retention.

Interfacial chemistry of anode/electrolyte interface for rechargeable magnesium batteries

Rechargeable magnesium batteries(RMBs),as a low-cost,high-safety and high-energy storage technology,have attracted tremendous attention in large-scale energy storage applications.However,the key anode/electrolyte interfacial issues,including surface passivation,uneven Mg plating/stripping,and pulverization after cycling still result in a large overpotential,short cycling life,poor power density,and possible safety hazards of cells,severely impeding the commercial development of RMBs.In this review,a concise overview of recently advanced strategies to address these anode/electroyte interfacial issues is systematically classified and summarized.The design of magnesiophilic substrates,construction of artificial SEI layers,and modification of electrolyte are important and effective strategies to improve the uniformity/kinetics of Mg plating/stripping and achieve the stable anode/electrolyte interface.The key opportunities and challenges in this field are advisedly put forward,and the insights into future directions for stabilizing Mg metal anodes and the anode/electrolyte interface are highlighted.This review provides important references fordeveloping the high-performance and high-safety RMBs.

Interfacial fusion-enhanced 11 μm-thick gel polymer electrolyte for high-performance lithium metal batteries

In the pursuit of ultrathin polymer electrolyte(<20 μm) for lithium metal batteries, achieving a balance between mechanical strength and interfacial stability is crucial for the longevity of the electrolytes.Herein, 11 μm-thick gel polymer electrolyte is designed via an integrated electrode/electrolyte structure supported by lithium metal anode. Benefiting from an exemplary superiority of excellent mechanical property, high ionic conductivity, and robust interfacial adhesion, the in-situ formed polymer electrolyte reinforced by titanosiloxane networks(ISPTS) embodies multifunctional roles of physical barrier, ionic carrier, and artificial protective layer at the interface. The potent interfacial interactions foster a seamless fusion of the electrode/electrolyte interfaces and enable continuous ion transport. Moreover, the built-in ISPTS electrolyte participates in the formation of gradient solid-electrolyte interphase(SEI) layer, which enhances the SEI's structural integrity against the strain induced by volume fluctuations of lithium anode.Consequently, the resultant 11 μm-thick ISPTS electrolyte enables lithium symmetric cells with cycling stability over 600 h and LiFePO_(4) cells with remarkable capacity retention of 96.6% after 800 cycles.This study provides a new avenue for designing ultrathin polymer electrolytes towards stable, safe,and high-energy–density lithium metal batteries.

Synergy effect of regulated Li-plating and functional solid electrolyte interphase on graphite anodes

The growth of Li dendrites poses potential safety hazard to lithium-ion batteries(LIBs),and eliminating Li dendrites thoroughly stills face tough difficulties ahead.Thus,regulating Li-plating is a critical optimization-direction to address the issue.Herein,a“graphite-Li hybrid”anode with high reversibility is realized under the constant-capacity lithiation(CCL).Within CCL,the uniform distribution of Li-plating on the graphite surface is successfully achieved.The evolution in different states of solid electrolyte interphase(SEI)is investigated in detail to study the interaction between the potentials and impedance during the process of Liintercalation and Li-deintercalation.Under the potential below 0 V and the state of charge(SOC)of 110%relative to the theoretical capacity,the F-rich SEI with high stability is constructed to hinder the emergency of Li dendrites and maintain the intact structure of graphite anode under long cycling.The cell presents more than 100%Coulombic efficiency(CE)with the 900 cycles,demonstrating the reversible Li-plating and the utilization of defects.And the CCL half-cell provides a good cycling performance and specific capacity of 900 cycles at 0.5 C,it is attributed to the synergy effect of stable inorganic-rich SEI and regulated active Li-plating.

Long‐life lithium batteries enabled by a pseudo‐oversaturated electrolyte

The specific energy of Li metal batteries(LMBs)can be improved by using high‐voltage cathode materials;however,achieving long‐term stable cycling performance in the corresponding system is particularly challenging for the liquid electrolyte.Herein,a novel pseudo‐oversaturated electrolyte(POSE)is prepared by introducing 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropyl ether(TTE)to adjust the coordination structure between diglyme(G2)and lithium bis(trifluoromethanesulfonyl)imide(LiTFSI).Surprisingly,although TTE shows little solubility to LiTFSI,the molar ratio between LiTFSI and G2 in the POSE can be increased to 1:1,which is much higher than that of the saturation state,1:2.8.Simulation and experimental results prove that TTE promotes closer contact of the G2 molecular with Li^(+)in the POSE.Moreover,it also participates in the formation of electrolyte/electrode interphases.The electrolyte shows outstanding compatibility with both the Li metal anode and typical high‐voltage cathodes.Li||Li symmetric cells show a long life of more than 2000 h at 1 mA cm^(−2),1 mAh cm^(−2).In the meantime,Li||LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cell with the POSE shows a high reversible capacity of 134.8 mAh g^(−1 )after 900 cycles at 4.5 V,1 C rate.The concept of POSE can provide new insight into the Li^(+)solvation structure and in the design of advanced electrolytes for LMBs.

A Review of Solid Electrolyte Interphase(SEI)and Dendrite Formation in Lithium Batteries

Lithium-metal batteries with high energy/power densities have significant applications in electronics,electric vehicles,and stationary power plants.However,the unstable lithium-metal-anode/electrolyte interface has induced insufficient cycle life and safety issues.To improve the cycle life and safety,understanding the formation of the solid electrolyte interphase(SEI)and growth of lithium dendrites near the anode/electrolyte interface,regulating the electrodeposition/electrostripping processes of Li^(+),and developing multiple approaches for protecting the lithium-metal surface and SEI layer are crucial and necessary.This paper comprehensively reviews the research progress in SEI and lithium dendrite growth in terms of their classical electrochemical lithium plating/stripping processes,interface interaction/nucleation processes,anode geometric evolution,fundamental electrolyte reduction mechanisms,and effects on battery performance.Some important aspects,such as charge transfer,the local current distribution,solvation,desolvation,ion diffusion through the interface,inhibition of dendrites by the SEI,additives,models for dendrite formation,heterogeneous nucleation,asymmetric processes during stripping/plating,the host matrix,and in situ nucleation characterization,are also analyzed based on experimental observations and theoretical calculations.Several technical challenges in improving SEI properties and reducing lithium dendrite growth are analyzed.Furthermore,possible future research directions for overcoming the challenges are also proposed to facilitate further research and development toward practical applications.

A promising solution for highly reversible zinc metal anode chemistry:Functional gradient interphase

Rechargeable zinc(Zn)metal batteries have long been plagued by dendrite growth and parasitic reactions due to the absence of a stable Zn-ion conductive solid-electrolyte interphase(SEI).Although the current strategies assist in suppressing dendritic Zn growth,it is still a challenge to obtain the operation-stability of Zn anode with high Coulombic efficiency(CE)required to implement a sustainable and long-cycling life of Zn metal batteries.In this perspective,we summarize the advantages of the functional gradient interphase(FGI)and try to fundamentally understand the transport behaviors of Zn ions,based on recently an article understanding Zn chemistry.The correlation between the function-orientated design of gradient interphase and key challenges of Zn metal anodes in accelerating Zn2+transport kinetics,improving electrode reversibility,and inhibiting Zn dendrite growth and side reactions was particularly emphasized.Finally,the rational design and innovative directions are provided for the development and application of functional gradient interphase in rechargeable Zn metal battery systems.

锂离子电池SEI成膜添加剂的研究

开发高效优质的固体电解质界面(SEI)成膜添加剂是提高锂离子电池性能的一种经济而有效的途径.本文从SEI成膜添加剂成膜机理的角度,分析和评价了已有的还原型添加剂、反应型添加剂及修饰型添加剂的作用效果;综述了理论计算在锂离子电池SEI成膜添加剂研究中的应用,并提出了"理论设计、材料合成、性能评估"三个研究环节无缝连接锂离子电池中SEI成膜添加剂创新研发的新思路.

Interface challenges and optimization strategies for aqueous zinc-ion batteries

Aqueous zinc-ion batteries have advantages over lithium-ion batteries,such as low cost,and good safety.However,their development is currently facing several challenges.One of the main critical challenges is their poor electrode–electrolyte interface.Addressing this requires understanding the physics and chemistry at the electrode–electrolyte interface,including the cathode-electrolyte interface and anodeelectrolyte interface.This review first identifies and analyses the interfacial challenges of aqueous zincion batteries.Then,it discusses the design strategies for addressing the defined interfacial issues from the perspectives of electrolyte optimization,electrode modification,and separator improvement.Finally,it provides corrective recommendations and strategies for the rational design of electrode–electrolyte interface in aqueous zinc-ion batteries towards their high-performance and reliable energy storage.

In-situ constructed polymer/alloy composite with high ionic conductivity as an artificial solid electrolyte interphase to stabilize lithium metal anode

Lithium(Li)metal is regarded as the best anode material for lithium metal batteries(LMBs)due to its high theoretical specific capacity and low redox potential.However,the notorious dendrites growth and extreme instability of the solid electrolyte interphase(SEI)layers have severely retarded the commercialization process of LMBs.Herein,a double-layered polymer/alloy composite artificial SEI composed of a robust poly(1,3-dioxolane)(PDOL)protective layer,Sn and LiCl nanoparticles,denoted as PDOL@Sn-LiCl,is fabricated by the combination of in-situ substitution and polymerization processes on the surface of Li metal anode.The lithiophilic Sn-LiCl multiphase can supply plenty of Li-ion transport channels,contributing to the homogeneous nucleation and dense accumulation of Li metal.The mechanically tough PDOL layer can maintain the stability and compact structure of the inorganic layer in the long-term cycling,and suppress the volume fluctuation and dendrites formation of the Li metal anode.As a result,the symmetrical cell under the double-layered artificial SEI protection shows excellent cycling stability of 300 h at 5.0 mA·cm^(−2)for 1 mAh·cm^(−2).Notably,the Li||LiFePO_(4)full cell also exhibits enhanced capacity retention of 150.1 mAh·g^(−1)after 600 cycles at 1.0 C.Additionally,the protected Li foil can effectively resist the air and water corrosion,signifying the safe operation of Li metal in practical applications.This present finding proposed a different tactic to achieve safe and dendrite-free Li metal anodes with excellent cycling stability.

Dynamically lithium-compensated polymer artificial SEI to assist highly stable lithium-rich manganese-based anode-free lithium metal batteries

Owing to the unique structure,anode-free lithium metal batteries(AFLMBs)have higher energy density and lower production cost than traditional lithium metal batteries(LMBs)or lithium-ion batteries(LIBs),However,AFLMBs suffer from an inherently finite Li reservoir and exhibit poor cycle stability,low Coulombic efficiency(CE)and severe dendrite growth.In this work,polydiallyl lithium disulfide(PDS-Li)was successfully synthesized and coated on Cu current collector by electrochemical polymerization.The PDS-Li acts as an additional lithium resource to compensate for the irreversible loss of lithium during cycling.In addition,the special structure and lithiophilicity of PDS-Li contribute to lower nucleation overpotential and uniform lithium deposition.When coupled with Li-rich manganese-based(LRM)cathode of Li1.2Mn0.54Ni0.13Co0.13O2,the anode-free full cell exhibits significantly improved cycle stability over 100 cycles and capacity retention of 63.3%and 57%after 80 and 100 cycles,respectively.We believe that PDS-Li can be used to ensure stable cycling performance and high-energy-density in AFLMBs.

Electrolyte and interphase engineering through solvation structure regulation for stable lithium metal batteries

Lithium metal batteries(LMBs)are considered to be one of the most promising high-energy-density battery systems.However,their practical application in carbonate electrolytes is hampered by lithium dendrite growth,resulting in short cycle life.Herein,an electrolyte regulation strategy is developed to improve the cyclability of LMBs in carbonate electrolytes by introducing LiNO3 using trimethyl phosphate with a slightly higher donor number compared to NO_(3)^(-)as a solubilizer.This not only allows the formaion of Li^(+)-coordinated NO3 but also achieves the regulation of electrolyte solvation structures,leading to the formation of robust and ion-conductive solid-electrolyte interphase films with inorganic-rich inner and organic-rich outer layers on the Li metal anodes.As a result,high Coulombic efficiency of 99.1%and stable plating/stripping cycling of Li metal anode in LilCu cells were realized.Furthermore,excellent performance was also demonstrated in Li||LiNi_(0.83)Co_(0.11)Mn_(0.06)O_(2)(NCM83)full cells and Cul/NCM83 anodefree cells using high mass-loading cathodes.This work provides a simple interphase engineering strategy through regulating the electrolyte solvation structures for high-energy-density LMBs.