Integrated interface between composite electrolyte and cathode with low resistance enables ultra-long cycle-lifetime in solid-state lithium-metal batteries

We report a three-dimensional(3D)nanofiber-reinforced solid composite electrolyte with a 3D Li⁺-conducting ceramic network of Li_6.25Ga_0.25La₃Zr₂O₁₂(LLZO)nanofibers.Benefiting from the 3D structure,the composite shows a high ionic conductivity of 3.2×10^-4S cm^-1and Li-ion transference number of 0.32 at room temperature.The interfacial resistance between the composite solid electrolyte and cathode is mitigated by creating an integrated interfacial structure,in which the polyethylene oxide(PEO)-lithiumbis(trifluoromethylsulphonyl)imide(LiTFSI)binder and ionic liquids(ILs)form a viscoelastic interface.Therefore,intimate contact,low interfacial impedance,and fast ion-transport between the cathode and the solid electrolyte are simultaneously achieved.Solid-state lithium metal batteries with the Li Fe PO₄ cathode deliver a superior capacity(158.0 m A h g^-1)and significant capacity retention(90.4%retention after 800 cycles)at 60℃.Moreover,the smooth and uniform Li surface after long-term cycling confirms the successful suppression of the dendrite formation.The integrated interfacial structure provides a solution to the interfacial problem and improves the cycling performance in solid-state Li-metal batteries.     

Lithiated Nafion-garnet ceramic composite electrolyte membrane for solid-state lithium metal battery

Single-ion conducting solid polymer electrolytes are expected to play a vital role in the realization of solid-state Li metal batteries.In this work,a lithiated Nafion(Li-Nafion)-garnet ceramic Li6.25La3 Zr2 Al0.25O12(LLZAO)composite solid electrolyte(CSE)membrane with 30μm thickness was prepared for the first time.By employing X-ray photoelectron spectroscopy and transmission electron microscope,the interaction between LLZAO and Li-Nafion was investigated.It is found that the LLZAO interacts with the Li-Nafion to form a space charge layer at the interface between LLZAO and Li-Nafion.The space charge layer reduces the migration barrier of Li-ions and improves the ionic conductivity of the CSE membrane.The CSE membrane containing 10 wt%LLZAO exhibits the highest ionic conductivity of2.26×10-4 S cm-1 at 30℃among the pristine Li-Nafion membrane,the membrane containing 5 wt%,20 wt%,and 30 wt%LLZAO,respectively.It also exhibits a high Li-ion transference number of 0.92,and a broader electrochemical window of 0-+4.8 V vs.Li+/Li than that of 0-+4.0 V vs.Li+/Li for the pristine Li-Nafion membrane.It is observed that the CSE membrane not only inhibits the growth of Li dendrites but also keeps excellent electrochemical stability with the Li electrode.Benefitting from the above merits,the solid-state LiFePO4/Li cell fabricated with the CSE membrane was practically charged and discharged at 30℃.The cell exhibits an initial reversible discharge specific capacity of 160 mAh g-1 with 97%capacity retention after 100 cycles at 0.2 C,and maintains discharge specific capacity of 126 mAh g-1 after500 cycles at 1 C.The CSE membrane prepared with Li-Nafion and LLZAO is proved to be a promising solid electrolyte for advanced solid-state Li metal batteries.     

Enhancing interfacial stability in solid-state lithium batteries with polymer/garnet solid electrolyte and composite cathode framework

The solid-state lithium battery is considered as an ideal next-generation energy storage device owing to its high safety,high energy density and low cost.However,the poor ionic conductivity of solid electrolyte and low interfacial stability has hindered the application of solid-state lithium battery.Here,a flexible polymer/garnet solid electrolyte is prepared with poly(ethylene oxide),poly(vinylidene fluoride),Li6.75La3 Zr1.75Ta0.25O12,lithium bis(trifluoromethanesulfonyl)imide and oxalate,which exhibits an ionic conductivity of 2.0 ×10^-4 S cm^-1 at 55℃,improved mechanical property,wide electrochemical window(4.8 V vs.Li/Li+),enhanced thermal stabilities.Tiny acidic OX was introduced to inhibit the alkalinity reactions between Li6.75La3 Zr1.75Ta0.25O12 and poly(vinylidene fluoride).In order to improve the interfacial stability between cathode and electrolyte,an Al2 O3@LiNi0.5Co0.2Mn0.3O2 based composite cathode framework is also fabricated with poly(ethylene oxide) polymer and lithium salt as additives.The solid-state lithium battery assembled with polymer/garnet solid electrolyte and composite cathode framework demonstrates a high initial discharge capacity of 150.6 mAh g^-1 and good capacity retention of 86.7% after 80 cycles at 0.2 C and 55℃,which provides a promising choice for achieving the stable electrode/electrolyte interfacial contact in solid-state lithium batteries.     

Stabilizing the Electrochemistry of Lithium-Selenium Battery via In situ Gelated Polymer Electrolyte: A Look from Anode

Li metal possesses a high theoretical specific capacity,high electronic conductivity,and a low electrochemical potential,making it a promising anode material for building next-generation rechargeable metal batteries.In case conventional liquid electrolytes were used,and the anode using Li metal has been hindered by unstable(electro)chemistry at Li/electrolyte interface and the accompanied dendrite issue.Specifically,for the Li-Se batteries,the dissolution and shuttle of polyselenide intermediates lead to the deposition of poorly-conductive species on the anode,which further aggravates the chemical environment at the anode.In this work,we proposed to stabilize the Li-Se electrochemistry by constructing a gel polymer electrolyte via in situ gelations of conventional ether-based electrolytes at room temperature.The results demonstrate that the in situ gelated electrolyte helps to build electrochemically stable electrode/electrolyte interfaces and promote the efficient transfer of charge carriers across the interface.Compared with the liquid electrolytes,the gelated electrolyte shows improved chemical compatibility with the Li metal anode,which effectively alleviates the unfavorable side reactions and dendrite formation at the anode/electrolyte interface,and the polyselenide shuttle from the cathode to the anode.As a result,the Li-Se battery shows a higher Coulombic efficiency and improved cycling performance.     

Enhancing the ionic conductivity in a composite polymer electrolyte with ceramic nanoparticles anchored to charged polymer brushes

Polymer electrolytes a re essential for next-gene ration lithium batteries because of their excellent safety record.However,low ionic conductivity is the main obstacle restricting their commercial application.Composites with nanoparticles are a promising route to overcome this obstacle.In this work,lithium polystyrene sulfonate brushes(LiPSS)is anchored to silicon dioxide nanoparticles with chemical bonding using atom transfer radial polymerization(SI-ATRP).The composite polymer electrolytes are made by mixing vinylene carbonate and nanoparticles via a facile in situ polymerization process.The ionic conductivity of composite polymer electrolytes is improved to 7.2×10^-4 S/cm at room temperature,which is attributed to the low degree of crystallinity of polymer electrolyte and the fast ion transport on the surfaces of polymer brush layers that act as a conductive network.The composite polymer electrolytes show a wide electrochemical window of approximately 4.5 V vs.Li^+/Li and excellent cycling performance retention of approximately 95%after 100 cycles at ambient temperature.The results also prove that surface groups of ceramic na noparticles are an important way to increase the electrochemical properties of composite polymer electrolytes.     

Synthesis of 3D Porous and Interconnected Hollow Carbon Nanospheres Array and Its Applications in Lithium-sulfur Batteries

Lithium-sulfur(Li–S) batteries are receiving much attention due to their high theoretical lithium storage capacity and energy density. However, the commercialization of Li–S batteries is mainly impeded by the inherent poor electrical conductivity of sulfur, the side shuttle behavior of polysulfides, and the volumetric change of sulfur during cycles. To solve these problems, here we report a unique 3D porous and interconnected hollow carbon nanospheres array(3D-HCNA) as sulfur host for lithium-sulfur batteries. This 3D-HCNA was synthesized through a nanocasting approach with sucrose as carbon precursors and mesoporous silica nanospheres as hard-templates. The silica nanospheres with special nanostructure were obtained by a biphase stratification approach. Owing to its unique architecture, as-prepared 3D-HCNA/S cathode with a high sulfur loading of 76 wt% exhibited excellent electrochemical performance. It showed highinitial capacity of 1318 m Ah/g at 0.05 C and good rate capability of 760 m Ah/g at 1 C. Moreover, excellent cycling performance was also observed with a capacity of 757 m Ah/g maintained after 200 cycles at 0.5 C.     

Application of diatomite as an effective polysulfides adsorbent for lithium-sulfur batteries

The lithium–sulfur batteries show the great potential to be the most promising candidate for high energy applications. However, the shuttling of soluble polysulfides deteriorates the battery performance tremendously. To suppress the diffusion of soluble polysulfides, diatomite that has abundant natural three-dimensional ordered pores is incorporated into the cathode to trap polysulfides. The composite cathode material(S-DM-AB for short), including sulfur(S), diatomite(DM), and acetylene black(AB) is prepared by an impregnation method. For comparison, another composite cathode material(S-AB for short) including sulfur and acetylene black is also prepared by the same method. The battery with S-DMAB composite cathode material delivers a discharge capacity of 531.4 m Ah/g after 300 cycles at 2 C with a capacity retention of 51.6% at room temperature. By contrast, the battery with S-AB composite cathode material delivered a capacity of only 196.9 m Ah/g with a much lower capacity retention of 18.6% under the same condition. The addition of diatomite in the cathode is proved to be a cheap and effective way to improve the life time of the lithium sulfur batteries.     

2D spinel ZnCo2O4 microsheet-coated functional separator for promoted redox kinetics and inhibited polysulfide dissolution

Lithium-sulfur(Li-S)batteries are receiving increasing attention as one of the potential next-generation batteries,owing to their high energy densities and low cost.However,practical Li-S batteries with high energy densities are extremely hindered by the sulfur loss,low Coulombic efficiency,and short cycling life originating from the polysulfide(LiPS)shuttle.In this study,two-dimensional(2D)ZnCo₂O₄ microsheets fabricated by a facile hydrothermal process are employed to modify the separator,for improving the electrochemical performances of Li-S cells.The resulting 2D Zn Co₂O₄-coated separator features a coating thickness of approximately 10 lm,high ionic conductivity of 1.8 m S/cm,and low mass loading of 0.2 mg/cm².This 2D ZnCo₂O₄-coated separator effectively inhibits Li PS shuttle by a strong chemical interaction with Li PS as well as promotes the redox kinetics by Zn CO2O4-coated layers,as determined by X-ray photoelectron spectroscopy analysis,self-discharge,time-dependent permeation test,Li symmetric cell test,and Li2S nucleation analyses.Consequently,the Li-S batteries based on the 2D Zn Co₂O₄-coated separator exhibit a high initial discharge capacity of 1292.2 m Ah/g at 0.1 C.Moreover,they exhibit excellent long cycle stability at 1 and 2 C with capacity retention of 84%and 86%even after800 cycles,corresponding to a capacity fading rate of 0.020%and 0.016%per cycle,respectively.Effectively,these Li-S cells with a high sulfur loading at 5.3 mg/cm² and low electrolyte concentration of 9 l L/mg deliver a high discharge capacity of 4.99 m Ah/cm² after 200 cycles at 0.1 C.     

Asymmetric double-layer composite electrolyte with enhanced ionic conductivity and interface stability for all-solid-state lithium metal batteries

All-solid-state Li metal battery has been regarded as a promising battery technology due to its high energy density based on the high capacity of lithium metal anode and high safety based on the all solid state electrolyte without inflammable solvent.However,challenges still exist mainly in the poor contact and unstable interface between electrolyte and electrodes.Herein,we demonstrate an asymmetric design of the composite polymer electrolyte with two different layers to overcome the interface issues at both the cathode and the anode side simultaneously.At the cathode side,the polypropylene carbonate layer has enough viscosity and flexibility to reduce the inter-facial resistance,while at the Li anode side,the polyethylene oxide layer modified with hexagonal boron nitride has high mechanical strength to suppress the Li dendrite growth.Owing to the synergetic effect between different components,the asprepared double layer composite polymer electrolyte demonstrates a large electrochemical window of5.17 V,a high ionic conductivity of 6.1×10~(-4) S/cm,and a transfe rence number of 0.56,featuring excellent ion transport kinetics and good chemical stability.All-solid-state Li metal battery assembled with LiFePO_4 cathode and Li anode delivers a high capacity of 150.9 mAh/g at 25℃ and 0.1 C-rate,showing great potential for practical applications.     

Preparation and Properties of Poly（ether ether ketone）/Carbon Nanotube Modified Polypropylene Janus Composite Separator北大核心CSCD

Lithium-ion batteries （LIBs）have attracted wide attention because of their broad prospects in electric vehicles. However,the safety problems and low multiplier performance of the commercial polyolefin separator limit their further development,due to the poor dimensional thermal stability and low electrolyte absorption rate. Poly（ether ether ketone）（PEEK）and carbon nanotube（CNT）are compounded to coat on polypropylene （PP） to prepare Janus composite separator （PP@C） through the phase inversion method. PP@C composite separator does not deform at 180 ℃ for 0. 5 h（only slight deformation）,illustrating excellent thermal stability. The electrolyte absorption rate of PP@C2 is 193. 8%. The electrolyte uptake rate of the PP@C2 composite membrane was 193. 8%,which was 64. 5% higher than the PP membrane,showing a superduper electrolyte permeability. As a result,the specific discharge capacity of LIBs assembled with PP@C2 composite separator is 157. 6 mA·h/g at 0. 2 C and 129. 8 mA·h/g at 2 C,showing good rate performance with the capacity recovery rate of more than 99%. This might be attributed to the ultra-high thermal stability of PEEK,the good affinity of the electrolyte,the high conductivity of CNT,as well as the uniform dispersion of Li+ ,so that the separator can have excellent electrochemical performance while improving safety. © 2022, Science Press (China). All rights reserved.     

Freestanding reduced graphene oxide/sodium vanadate composite films for flexible aqueous zinc-ion batteries

With the booming development of portable and wearable electronic devices, flexible energy storage devices have attracted great attention. Among various energy storage devices, aqueous zinc ion batteries(ZIBs) are one of the promising candidates due to their low cost, good safety, high energy and power densities. However, the conventional cathodes of aqueous ZIBs were often prepared by mixing active materials with binders and conductive additives and then coating them onto current collectors. The resultant cathodes often suffer from unsatisfied flexibility. Herein, we fabricated freestanding reduced graphene oxide/NaV_3O_8·1.5H_2O(RGO/NVO) composite films with interlinked multilayered architecture by a vacuum filtrating process. Such composite films exhibit excellent mechanical property and high electronic conductivity. Owing to unique architecture, they display a high capacity of 410 mA h g~(-1) and excellent cycling performance up to 2000 cycles with a high capacity retention of 94%. Moreover, RGO/NVO composite films can directly serve as the cathodes of flexible aqueous ZIBs. As a proof of concept,flexible ZIBs were assembled based on the composite films. Impressively, they exhibit stable performance at different bending states, demonstrating great potential application in flexible energy storage devices.     

Poly(vinylidene fluoride) separators with dual-asymmetric structure for high-performance lithium ion batteries

Dual-asymmetric poly(vinylidene fluoride)(PVDF) separators have been fabricated by thermally induced phase separation with dimethyl sulfone(DMSO2) and glycerol as mixed diluents. The separators have a porous bulk with large interconnected pores(~1.0 μm) and two surfaces with small pores(~30 nm). This dual-asymmetric porous structure endows the separators with higher electrolyte uptake amount and rapider uptake rate, as well as better electrolyte retention ability than the commercialized Celgard 2400. The separators even maintain their dimensional stability up to 160 °C, at which temperature the surface pores close up, leading to a dramatic decrease of air permeability. The electrolyte filled separators also show high ion conductivity(1.72 m S?cm―1) at room temperature. Lithium iron phosphate(Li Fe PO4)/lithium(Li) cells using these separators display superior discharge capacity and better rate performance as compared with those from the commercialized ones. The results provide new insight into the design and development of separators for high-performance lithium ion batteries with enhanced safety.     

CNTs@S composite as cathode for all-solid-state lithium-sulfur batteries with ultralong cycle life

The main challenges in development of traditional liquid lithium-sulfur batteries are the shuttle effect at the cathode caused by the polysulfide and the safety concern at the Li metal anode arose from the dendrite formation. All-solid-state lithium-sulfur batteries have been proposed to solve the shuttle effect and prevent short circuits. However, solid-solid contacts between the electrodes and the electrolyte increase the interface resistance and stress/strain, which could result in the limited electrochemical performances.In this work, the cathode of all-solid-state lithium-sulfur batteries is prepared by depositing sulfur on the surface of the carbon nanotubes(CNTs@S) and further mixing with Li_(10) Ge P_2 S_(12) electrolyte and acetylene black agents. At 60 °C, CNTs@S electrode exhibits superior electrochemical performance, delivering the reversible discharge capacities of 1193.3, 959.5, 813.1, 569.6 and 395.5 m Ah g~(-1) at the rate of 0.1, 0.5,1, 2 and 5 C, respectively. Moreover, the CNTs@S is able to demonstrate superior high-rate capability of660.3 m Ah g~(-1) and cycling stability of 400 cycles at a high rate of 1.0 C. Such uniform distribution of the CNTs, S and Li_(10) Ge P_2 S_(12) electrolyte increase the electronic and ionic conductivity between the cathode and the electrolyte hence improves the rate performance and capacity retention.     

MoS2 nanorods with inner caves through synchronous encapsulation of sulfur for high performance Li–S cathodes

Lithium–sulfur(Li–S)batteries have become one of the most promising candidates for next-generation batteries owing to their high specific capacity,low cost,and environment-friendliness.Many efforts have been made to mitigate the"shuttle effect"through physical adsorption and chemical bonding.MoS2 has been proposed as a cathode material to provide effective anchoring sites for lithium polysulfides(Li PSs),but is still limited by its layer structure.Herein,we designed novel MoS2 nanorods with inner caves based on our previous work,and performed synchronous encapsulation of sulfur during the synthesis process.The outer MoS2 tubular shells physically inhibit the outward diffusion of polysulfide species while the inner particles chemically anchor the polysulfides to prevent shuttling.As the cathode matrix in Li–S batteries,the electrochemical results deliver a high initial discharge capacity of 1213 mAhg^-1 for sulfur at 0.1 C.After cycling at 1 C for 300 cycles,the cells exhibit a capacity decay of only 0.076%per cycle and high average coulombic efficiency over 95%.The tubular MoS2 structure is an innovative and appealing design,which could be regarded as a prospective substrate for the improved performance of Li–S batteries.     

Fabrication and characterization of Ba Ce0.8Y0.2O2.9-Ce0.85Sm0.15O1.925 composite electrolytes for IT-SOFCs

The Ba Ce0.8Y0.2O2.9-Ce0.85Sm0.15O1.925 composite electrolytes were prepared with Ba Ce0.8Y0.2O2.9(BCY) and Ce0.85Sm0.15O1.925(SDC). The SDC and BCY powders were mixed in the weight ratio of 95:5, 85:15, and 75:25, respectively(named as BS95, BS85, and BS75). Because of the composite effect between the SDC and BCY phases, the BS95 and BS85 exhibit improved conductivity compared with the pure SDC and BCY. The conductivity of BS95 is higher than that of BS85, indicating that the composite effect of BS95 is greater than that of BS85. Nevertheless, the composite effect in BS75 does not exist. Hence, we conclude that the composite effect in the BCY-SDC composites will decrease with the increase of the amount of BCY and even disappear when the amount of BCY exceeds a certain value. In our case, the optimum composition of the composite electrolyte is 95 wt% SDC and 5 wt% BCY. The BS95 has the highest conductivity(σ1t=0.07808 S cm-1, at 800 °C) and the fuel cell based on the BS95 shows the best performance(the maximum power density reaches as high as 526 mw cm-2 at 750 °C). The encouraging results suggest that the BCY-SDC composites are the very promising electrolyte materials for IT-SOFCs.     

Mechanistic insights into the processes of the initial stage of electrolyte degradation in lithium metal batteries

The lithium(Li) metal batteries(LMBs) are considered one of the most promising next-generation batteries due to its extremely high theoretical specific capacity. However, there are a couple of issues, e.g., the serious side reactions that occurred at the solid-liquid interface between the electrolyte and Li metal anode, hindering the broad commercialization of LMBs. Thus, a comprehensive understanding of the mechanisms underlying the decomposition of electrolytes is crucial to the design of LMBs...     

Block copolymer electrolyte with adjustable functional units for solid polymer lithium metal battery

Solid polymer electrolytes have been considered as the promising candidates to improve the safety and stability of high-energy lithium metal batteries.However,the practical applications of solid polymer electrolytes are still limited by the low ionic conductivity,poor interfacial contact with electrodes,narrow electrochemical window and weak mechanical strength.Here,a series of novel block copolymer electrolytes with three-dimensional networks are designed by cross-linked copolymerization of the polyethylene glycol soft segments and hexamethylene diisocyanate trimer hard segments.Their ionic migration performances and interface compatibilities with Li metal anode have been optimized delicately by tailoring the ratio of these functional units.The optimized block copolymer electrolyte has shown an amorphous crystalline structure,a high ionic conductivity of ~5.7×10^-4S cm^-1,high lithium ion transference number(~0.49),wide electrochemical window up to ~4.65 V(vs.Li+/Li) and favorable mechanical strength at 55℃.Furthermore,the enhanced interface compatibility can well support the normal operations of lithium metal batteries using both LiFePO4 and LiNi0.8Co0.15Al0.05O2 cathodes.This study not only paves a new way to develop solid polymer electrolyte with optimizing functional units,but also provides a polymer electrolyte design strategy for the application demand of lithium metal battery.     

Quasi-solid-state polymer plastic crystal electrolyte for subzero lithium-ion batteries

Succinonitrile(SN)-based polymer plastic crystal electrolytes(PPCEs)have attracted considerable attention as solid-state electrolytes owing to their high ionic conductivities similar to those of liquid electrolytes,excellent contacts with the electrodes,and good mechanic properties.As a crucial property of a solid-state electrolyte,the ionic conductivity of the PPCE directly depends on the interactions between the constituent parts including the polymer,lithium salt,and SN.A few studies have focused on the effects of polymer–lithium–salt and polymer–SN interactions on the PPCE ionic conductivity.Nevertheless,the impact of the lithium–salt–SN combination on the PPCE ionic conductivity has not been analyzed.In particular,tuning of the lithium-salt–SN interaction to fabricate a subzero PPCE with a high low-temperature ionic conductivity has not been reported.In this study,we design and fabricate five PPCE membranes with different weight ratios of Li N(SO2 CF3)2(Li TFSI)and SN to investigate the effect of the Li TFSI–SN interaction on the PPCE ionic conductivity.The ionic conductivities of the five PPCEs are investigated in the temperature range of–20 to 60°C by electro-chemical impedance spectroscopy.The interaction is analyzed by Fourier-transform infrared spectroscopy,Raman spectroscopy,and differential scanning calorimetry.The Li TFSI–SN interaction significantly influences the melting point of the PPCE,dissociation of the Li TFSI salt,and thus the PPCE ionic conductivity.By tuning the Li TFSI–SN interaction,a subzero workable PPCE membrane having an excellent low-temperature ionic conductivity(6×10-4 S cm–1 at 0°C)is obtained.The electro-chemical performance of the optimal PPCE is evaluated by using a Li Co O2/PPCE/Li4 Ti5 O12 cell,which confirms the application feasibility of the proposed quasisolid-state electrolyte in subzero workable lithium-ion batteries.     

Simple synthesis of sandwich-like SnSe2/rGO as high initial coulombic efficiency and high stability anode for sodium-ion batteries

Metal selenides owing to their high theoretical capacity and good conductivity are considered as one of the potential candidates for the anode materials of sodium-ion batteries(SIBs).However,their practical applications are greatly restricted by the poor cycling performances and complicated synthesis methods.In this work,a sandwich-like Sn Se2/reduced graphene oxide(r GO)composite with a small amount of r GO(7.3%)is synthesized by a simple one-pot solvothermal technique.The as-synthesized Sn Se2/r GO shows improved initial coulombic efficiency(ICE)of 73.7%,high capacity of 402.0 m Ah g-1 after 150 cycles at 0.1 A g-1 with a retention of 86.2%and outstanding rate performances.The abundant Sn-O-C bonds of synthesized material not only accelerate the charge transfer at the interface but also enhance the mechanical strength to accommodate volume variation and prevent active material loss during cycling.Moreover,the compact structure leads to thin solid electrolyte interface(SEI)so that high initial coulombic efficiency was obtained.Furthermore,full cells are assembled to test its potential application.This work offers a simple method to synthesize Sn Se2/r GO as a candidate anode for SIBs.     

In-situ construction of a Mg-modified interface to guide uniform lithium deposition for stable all-solid-state batteries

Uniform lithium(Li)deposition in all-solid-state Li metal batteries is greatly influenced by the anode/electrolyte interface.Herein,a Mg-modified interface was constructed via the simple in-situ electrochemical reduction of Mg²⁺from Mg(TFSI)₂ in polyethylene oxide(PEO)and a Li bis(trifluoromethane)sulfoni mide(Li TFSI)formulae.As confirmed by cryogenic transmission electron microscopy,the anode/electrolyte interface exhibited hybrids consisting of crystalline Mg,Li₂O,and Li dots embedded in an amorphous polymer electrolyte.The crystalline Mg dots guided the uniform Li nucleation and growth,inducing a smoother anode/electrolyte interface compared with the pristine electrolyte.With 1 wt%Mg(TFSI)₂ in the PEO-Li TFSI electrolyte,the Mg-modified electrolyte enabled the Li/Li symmetric cells with cycling performance of over 1700 and 1400 h at current densities of 0.1 and 0.2 m A cm^-2,respectively.Moreover,the full LFP/Li cells using the novel Mg-modified electrolyte delivered a cycling lifespan of over 450 cycles with negligible capacity loss.