Thin polymer electrolyte with MXene functional layer for uniform Li^(+) deposition in all-solid-state lithium battery

Solid polymer electrolyte(SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility;however, the unfavourable Li+deposition and large thickness hamper its development and application. Herein, a laminar MXene functional layer-thin SPE layer-cathode integration(MXene-PEO-LFP) is designed and fabricated. The MXene functional layer formed by stacking rigid MXene nanosheets imparts higher compressive strength relative to PEO electrolyte layer. And the abundant negatively-charged groups on MXene functional layer effectively repel anions and attract cations to adjust the charge distribution behavior at electrolyte–anode interface. Furthermore,the functional layer with rich lithiophilic groups and outstanding electronic conductivity results in low Li nucleation overpotential and nucleation energy barrier. In consequence, the cell assembled with MXene-PEO-LFP, where the PEO electrolyte layer is only 12 μm, much thinner than most solid electrolytes, exhibits uniform, dendrite-free Li+deposition and excellent cycling stability. High capacity(142.8 mAh g-1), stable operation of 140 cycles(capacity decay per cycle, 0.065%), and low polarization potential(0.5 C) are obtained in this Li|MXene-PEO-LFP cell,which is superior to most PEO-based electrolytes under identical condition. This integrated design may provide a strategy for the large-scale application of thin polymer electrolytes in all-solid-state battery.

Enhanced High-Temperature Cycling Stability of Garnet-Based All Solid-State Lithium Battery Using a Multi-Functional Catholyte Buffer Layer

The pursuit of safer and high-performance lithium-ion batteries(LIBs)has triggered extensive research activities on solid-state batteries,while challenges related to the unstable electrode-electrolyte interface hinder their practical implementation.Polymer has been used extensively to improve the cathode-electrolyte interface in garnet-based all-solid-state LIBs(ASSLBs),while it introduces new concerns about thermal stability.In this study,we propose the incorporation of a multi-functional flame-retardant triphenyl phos-phate additive into poly(ethylene oxide),acting as a thin buffer layer between LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode and garnet electro-lyte.Through electrochemical stability tests,cycling performance evaluations,interfacial thermal stability analysis and flammability tests,improved thermal stability(capacity retention of 98.5%after 100 cycles at 60℃,and 89.6%after 50 cycles at 80℃)and safety characteristics(safe and stable cycling up to 100℃)are demonstrated.Based on various materials characterizations,the mechanism for the improved thermal stability of the interface is proposed.The results highlight the potential of multi-functional flame-retardant additives to address the challenges associated with the electrode-electrolyte interface in ASSLBs at high temperature.Efficient thermal modification in ASSLBs operating at elevated temperatures is also essential for enabling large-scale energy storage with safety being the primary concern.

Laminar Composite Solid Electrolyte with Poly(Ethylene Oxide)-Threaded Metal-Organic Framework Nanosheets for High-Performance All-Solid-State Lithium Battery

Developing laminar composite solid electrolyte with ultrathin thickness and continuous conduction channels in vertical direction holds great promise for all-solid-state lithium batteries.Herein,a thin,laminar solid electrolyte is synthesized by filtrating–NH 2 functionalized metal-organic framework nanosheets and then being threaded with poly(ethylene oxide)chains induced by the hydrogen-bonding interaction from–NH_(2) groups.It is demonstrated that the threaded poly(ethylene oxide)chains lock the adjacent metal-organic framework nanosheets,giving highly enhanced structural stability(Young’s modulus,1.3 GPa)to 7.5-μm-thick laminar composite solid electrolyte.Importantly,these poly(ethylene oxide)chains with stretching structure serve as continuous conduction pathways along the chains in pores.It makes the non-conduction laminar metal-organic framework electrolyte highly conductive:3.97×10^(−5) S cm^(−1) at 25℃,which is even over 25 times higher than that of pure poly(ethylene oxide)electrolyte.The assembled lithium cell,thus,acquires superior cycling stability,initial discharge capacity(148 mAh g^(−1) at 0.5 C and 60℃),and retention(94% after 150 cycles).Besides,the pore size of nanosheet is tailored(24.5–40.9˚A)to evaluate the mechanisms of chain conformation and ion transport in confined space.It shows that the confined pore only with proper size could facilitate the stretching of poly(ethylene oxide)chains,and meanwhile inhibit their disorder degree.Specifically,the pore size of 33.8˚A shows optimized confinement effect with trans-poly(ethylene oxide)and cis-poly(ethylene oxide)conformation,which offers great significance in ion conduction.Our design of poly(ethylene oxide)-threaded architecture provides a platform and paves a way to the rational design of next-generation high-performance porous electrolytes.

LiNbO3-coated LiNi0.8Co0.1Mn0.1O2 cathode with high discharge capacity and rate performance for all-solid-state lithium battery

In order to obtain high power density,energy density and safe energy storage lithium ion batteries(LIB)to meet growing demand for electronic products,oxide cathodes have been widely explored in all-solidstate lithium batteries(ASSLB)using sulfide solid electrolyte.However,the electrochemical performances are still not satisfactory,due to the high interfacial resistance caused by severe interfacial instability between sulfide solid electrolyte and oxide cathode,especially Ni-rich oxide cathodes,in charge-discharge process.Ni-rich LiNi0.8Co0.1Mn0.1O2(NCM811)material at present is one of the most key cathode candidates to achieve the high energy density up to 300 Wh kg^-1 in liquid LIB,but rarely investigated in ASSLB using sulfide electrolyte.To design the stable interface between NCM811 and sulfide electrolyte should be extremely necessary.In this work,in view of our previous work,LiNbO3 coating with about 1 wt% content is adopted to improve the interfacial stability and the electrochemical performances of NCM811 cathode in ASSLB using Li10GeP2S12 solid electrolyte.Consequently,LiNbO3-coated NCM811 cathode displays the higher discharge capacity and rate performance than the reported oxide electrodes in ASSLB using sulfide solid electrolyte to our knowledge.

In-situ interfacial passivation and self-adaptability synergistically stabilizing all-solid-state lithium metal batteries

The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.

A Review on Engineering Design for Enhancing Interfacial Contact in Solid-State Lithium–Sulfur Batteries

The utilization of solid-state electrolytes(SSEs)presents a promising solution to the issues of safety concern and shuttle effect in Li–S batteries,which has garnered significant interest recently.However,the high interfacial impedances existing between the SSEs and the electrodes(both lithium anodes and sulfur cathodes)hinder the charge transfer and intensify the uneven deposition of lithium,which ultimately result in insufficient capacity utilization and poor cycling stability.Hence,the reduction of interfacial resistance between SSEs and electrodes is of paramount importance in the pursuit of efficacious solid-state batteries.In this review,we focus on the experimental strategies employed to enhance the interfacial contact between SSEs and electrodes,and summarize recent progresses of their applications in solidstate Li–S batteries.Moreover,the challenges and perspectives of rational interfacial design in practical solid-state Li–S batteries are outlined as well.We expect that this review will provide new insights into the further technique development and practical applications of solid-state lithium batteries.

Viability of all-solid-state lithium metal battery coupled with oxide solid-state electrolyte and high-capacity cathode

Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g^(-1)and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La_(3)Zr_(2)O_(12)(LLZO),all-state-state lithium metal batteries(ASLMBs)have been widely accepted as the promising alternatives for providing the satisfactory energy density and safety.However,its applications are still challenged by plenty of technical and scientific issues.In this contribution,the co-sintering temperature at 500℃is proved as a compromise method to fabricate the composite cathode with structural integrity and declined capacity fading of LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM).On the other hand,it tends to form weaker grain boundary(GB)inside polycrystalline LLZO at inadequate sintering temperature for LLZO,which can induce the intergranular failure of SE during the growth of Li filament inside the unavoidable defect on the interface of SE.Therefore,increasing the strength of GB,refining the grain to 0.4μm,and precluding the interfacial defect are suggested to postpone the electro-chemo-mechanical failure of SE with weak GB.Moreover,the advanced sintering techniques to lower the co-sintering temperature for both NCM-LLZO composite cathode and LLZO SE can be posted out to realize the viability of state-of-the-art ASLMBs with higher energy density as well as the guaranteed safety.

Integrated interface configuration by in-situ interface chemistry enabling uniform lithium deposition in all-solid-state lithium metal batteries

All-solid-state lithium metal batteries(ASSLMBs)are considered as one of the ultimate goals for the development of energy storage systems due to their high energy density and high safety.However,the mismatching of interface transport kinetics as well as interfacial instability induces the growth of lithium dendrite and thus,leads to severe degradation of battery electrochemical performances.Herein,an integrated interface configuration(IIC)consisting of in-situ generated Li I interphase and Li-Ag alloy anode is proposed through in-situ interface chemistry.The IIC is capable of not only regulating charge transport kinetics but also synchronously stabilizing the lithium/electrolyte interface,thereby achieving uniform lithium platting.Therefore,Li||Li symmetric cells with IIC achieve a critical current density of up to 1.6 mA cm^(-2)and achieve stable cycling over 1600 hours at a high current density of 0.5 mA cm^(-2).Moreover,a high discharge capacity of 140.1 mA h g-1at 0.1 C is also obtained for the Li(Ni_(0.6)Co_(0.2)Mn_(0.2))O_(2)(NCM622)full battery with a capacity retention of 65.6%after 300 cycles.This work provides an effective method to synergistically regulate the interface transport kinetics and inhibit lithium dendrite growth for high-performance ASSLMBs.

Recent advances in solving Li_(2)CO_(3) problems in garnet-based solid-state battery: A systematic review(2020-2023)

Garnet solid electrolytes are one of the most promising electrolytes for solid-state batteries.However,Li_(2)CO_(3) is a critical issue that hinders the practical application of garnet-based solid-state lithium-ion batteries.There are two sources of Li_(2)CO_(3) contamination.The main one is the aging of garnet electrolytes in the atmosphere.Garnet electrolytes can react with H_(2)O and CO_(2) in the air to form Li_(2)CO_(3),which reduces ion conductivity,increases electrode/garnet electrolyte interface resistance,and deteriorates the electrochemical performance of the battery.Various strategies,such as elemental doping,grain boundary manipulation,and interface engineering,have been suggested to address these issues.The other is the passivation layer(Li_(2)CO_(3),Li_3N,LiOH,Li_(2)O) formed on the surface of the lithium foil after long-term storage,which is ignored by most researchers.To better understand the current strategies and future trends to address the Li_(2)CO_(3) problem,this perspective provides a systematic review of journals published in this field from 2020-2023.

A dynamic database of solid-state electrolyte(DDSE)picturing all-solid-state batteries

All-solid-state batteries(ASSBs)are a class of safer and higher-energy-density materials compared to conventional devices,from which solid-state electrolytes(SSEs)are their essential components.To date,investigations to search for high ion-conducting solid-state electrolytes have attracted broad concern.However,obtaining SSEs with high ionic conductivity is challenging due to the complex structural information and the less-explored structure-performance relationship.To provide a solution to these challenges,developing a database containing typical SSEs from available experimental reports would be a new avenue to understand the structureperformance relationships and find out new design guidelines for reasonable SSEs.Herein,a dynamic experimental database containing>600 materials was developed in a wide range of temperatures(132.40–1261.60 K),including mono-and divalent cations(e.g.,Li^(+),Na^(+),K^(+),Ag^(+),Ca^(2+),Mg^(2+),and Zn^(2+))and various types of anions(e.g.,halide,hydride,sulfide,and oxide).Data-mining was conducted to explore the relationships among different variates(e.g.,transport ion,composition,activation energy,and conductivity).Overall,we expect that this database can provide essential guidelines for the design and development of high-performance SSEs in ASSB applications.This database is dynamically updated,which can be accessed via our open-source online system.

The effects of amino groups and open metal sites of MOFs on polymer-based electrolytes for all-solid-state lithium metal batteries

Metal-organic frameworks(MOFs) are becoming more and more popular as the fillers in polymer electrolytes in recent years. In this study, a series of MOFs(NH_(2)-MIL-101(Fe), MIL-101(Fe), activated NH_(2)-MIL-101(Fe) and activated MIL-101(Fe)) were synthesized and added to PEO-based solid composite electrolytes(SCEs). Furthermore, the role of the —NH_(2) groups and open metal sites(OMSs) were both examined. Different ratios of MOFs vs polymers were also studied by the electrochemical characterizations. At last, we successfully designed a novel solid composite electrolyte containing activated NH_(2)-MIL-101(Fe),PEO, Li TFSI and PVDF for the high-performance all-solid-state lithium-metal batteries. This work might provide new insight to understand the interactions between polymers and functional groups or OMSs of MOFs better.

Polymer dispersed ionic liquid electrolytes with high ionic conductivity for ultrastable solid-state lithium batteries

Solid polymer electrolytes(SPEs)have emerged as one of the most promising candidates for building solid-state lithium batteries due to their excellent flexibility,scalability,and interfacial compatibility with electrodes.However,the low ionic conductivity and poor cyclic stability of SPEs do not meet the requirements for practical applications of lithium batteries.Here,a novel polymer dispersed ionic liquid-based solid polymer electrolyte(PDIL-SPE)is fabricated using the in situ polymerization-induced phase separation(PIPS)method.The as-prepared PDIL-SPE possesses both outstanding ionic conductivity(0.74 mS cm^(-1) at 25℃)and a wide electrochemical window(up to 4.86 V),and the formed unique three-dimensional(3D)co-continuous structure of polymer matrix and ionic liquid in PDIL-SPE can promote the transport of lithium ions.Also,the 3D co-continuous structure of PDIL-SPE effectively accommodates the severe volume expansion for prolonged lithium plating and stripping processes over 1000 h at 0.5 mA cm^(-2) under 25℃.Moreover,the LiFePO_(4)//Li coin cell can work stably over 150 cycles at a 1 C rate under room temperature with a capacity retention of 90.6%from 111.1 to 100.7 mAh g^(-1).The PDIL-SPE composite is a promising material system for enabling the ultrastable operation of solid-state lithium-metal batteries.

All-Solid-State Thin-Film Lithium-Sulfur Batteries

Lithium-sulfur(Li-S)system coupled with thin-film solid electrolyte as a novel high-energy micro-battery has enormous potential for complementing embedded energy harvesters to enable the autonomy of the Internet of Things microdevice.However,the volatility in high vacuum and intrinsic sluggish kinetics of S hinder researchers from empirically integrating it into allsolid-state thin-film batteries,leading to inexperience in fabricating all-solid-state thin-film Li-S batteries(TFLSBs).Herein,for the first time,TFLSBs have been successfully constructed by stacking vertical graphene nanosheets-Li2S(VGsLi2S)composite thin-film cathode,lithium-phosphorous-oxynitride(LiPON)thin-film solid electrolyte,and Li metal anode.Fundamentally eliminating Lipolysulfide shuttle effect and maintaining a stable VGs-Li2S/LiPON interface upon prolonged cycles have been well identified by employing the solid-state Li-S system with an“unlimited Li”reservoir,which exhibits excellent longterm cycling stability with a capacity retention of 81%for 3,000 cycles,and an exceptional high temperature tolerance up to 60℃.More impressively,VGs-Li2S-based TFLSBs with evaporated-Li thin-film anode also demonstrate outstanding cycling performance over 500 cycles with a high Coulombic efficiency of 99.71%.Collectively,this study presents a new development strategy for secure and high-performance rechargeable all-solid-state thin-film batteries.

Tailoring Practically Accessible Polymer/Inorganic Composite Electrolytes for All-Solid-State Lithium Metal Batteries:A Review

Solid-state electrolytes(SSEs)are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density.Among them,polymer solid-state electrolytes(PSEs)are competitive candidates for replacing commercial liquid electrolytes due to their flexibility,shape versatility and easy machinability.Despite the rapid development of PSEs,their practical application still faces obstacles including poor ionic conductivity,narrow electrochemical stable window and inferior mechanical strength.Polymer/inorganic composite electrolytes(PIEs)formed by adding ceramic fillers in PSEs merge the benefits of PSEs and inorganic solid-state electrolytes(ISEs),exhibiting appreciable comprehensive properties due to the abundant interfaces with unique characteristics.Some PIEs are highly compatible with high-voltage cathode and lithium metal anode,which offer desirable access to obtaining lithium metal batteries with high energy density.This review elucidates the current issues and recent advances in PIEs.The performance of PIEs was remarkably influenced by the characteristics of the fillers including type,content,morphology,arrangement and surface groups.We focus on the molecular interaction between different components in the composite environment for designing high-performance PIEs.Finally,the obstacles and opportunities for creating high-performance PIEs are outlined.This review aims to provide some theoretical guidance and direction for the development of PIEs.

Solid polymer electrolytes in all-solid-state lithium metal batteries:From microstructures to properties

All-solid-state lithium(Li)metal batteries(ASSLMBs)are considered one of the most promising secondary batteries due to their high theoretical capacity and high safety performance.However,low room-temperature ionic conductivity and poor interfacial stability are two key factors affecting the practical application of ASSLMBs,and our understanding of the mechanisms behind these key problems from microscopic perspective is still limited.In this review,the mechanisms and advanced characterization techniques of ASSLMBs are summarized to correlate the microstructures and properties.Firstly,we summarize the challenges faced by solid polymer electrolytes(SPEs)in ASSLMBs,such as the low roomtemperature ionic conductivity and the poor interfacial stability.Secondly,several typical improvement methods of polymer ASSLMBs are discussed,including composite SPEs,ultra-thin SPEs,SPEs surface modification and Li anode surface modification.Finally,we conclude the characterizations for correlating the microstructures and the properties of SPEs,with emphasis on the use of emerging advanced techniques(e.g.,cryo-transmission electron microscopy)for in-depth analyzing ASSLMBs.The influence of the microstructures on the properties is very important.Until now,it has been difficult for us to understand the microstructures of batteries.However,some recent studies have demonstrated that we have a better understanding of the microstructures of batteries.Then we suggest that in situ characterization,nondestructive characterization and sub-angstrom resolution are the key technologies to help us further understand the batteries'microstructures and promote the development of batteries.And potential investigations to understand the microstructures evolution and the batteries behaviors are also prospected to expect further reasonable theoretical guidance for the design of ASSLMBs with ideal performance.

A gel polymer electrolyte with IL@UiO-66-NH_(2) as fillers for high-performance all-solid-state lithium metal batteries

All solid-state electrolytes have the advantages of good mechanical and thermal properties for safer energy storage,but their energy density has been limited by low ionic conductivity and large interfacial resistance caused by the poor Li~+transport kinetics due to the solid-solid contacts between the electrodes and the solid-state electrolytes.Herein,a novel gel polymer electrolyte(UPP-5)composed of ionic liquid incorporated metal-organic frameworks nanoparticles(IL@MOFs)is designed,it exhibits satisfying electrochemical performances,consisting of an excellent electrochemical stability window(5.5 V)and an improved Li^(+)transference number of 0.52.Moreover,the Li/UPP-5/LiFePO_(4) full cells present an ultra-stable cycling performance at 0.2C for over 100 cycles almost without any decay in capacities.This study might provide new insight to create an effective Li^(+)conductive network for the development of all-solid-state lithium-ion batteries.

Green recycling of short-circuited garnet-type electrolyte for high-performance solid-state lithium batteries

Solid-state lithium batteries(SSLBs)solve safety issues and are potentially energy-dense alternatives to next-generation energy storage systems.Battery green recycling routes are responsible for the widespread use of SSLBs due to minimizing environmental contamination,reducing production costs,and providing a sustainable solution for resources,e.g.,saving rare earth elements(La,Ta,etc.).Herein,a solid-state recycling strategy is proposed to achieve green recycling of the crucial component solidstate electrolytes(SSEs)in spent SSLBs.The short-circuited garnet Li_(6.5)La_(3)Zr_(1.5)Ta_(0.5)O_(12)(LLZTO)is broken into fine particles and mixed with fresh particles to improve sintering activity and achieve high packing density.The continuous Li absorption process promotes sufficient grain fusion and guarantees the transformation from tetragonal phase to pure cubic phase for high-performance recycled LLZTO.The Li-ion conductivity reaches 5.80×10^(-4)S cm-1with a relative density of 95.9%.Symmetric Li cell with asrecycled LLZTO shows long-term cycling stability for 700 h at 0.3 mA cm^(-2)without any voltage hysteresis.Full cell exhibits an excellent cycling performance with a discharge capacity of 141.5 mA h g^(-1)and a capacity retention of 92.1%after 400 cycles(0.2C).This work develops an environmentally friendly and economically controllable strategy to recycle SSE from spent SSLBs,guiding future directions of SSLBs large-scale industrial application and green recycling study.

Latest progresses and the application of various electrolytes in high-performance solid-state lithium-sulfur batteries

With the emergence of some solid electrolytes(SSEs)with high ionic conductivity being comparable to liquid electrolytes,solid-state lithium-sulfur batteries(SSLSBs)have been widely regarded as one of the most promising candidates for the next generation of power generation energy storage batteries,and have been extensively researched.Though many fundamental and technological issues still need to be resolved to develop commercially viable technologies,SSLSBs using SSEs are expected to address the present limitations and achieve high energy and power density while improving safety,which is very attractive to large-scale energy storage systems.SSLSBs have been developed for many years.However,there are few systematic discussions related to the working mechanism of action of various electrolytes in SSLSBs and the defects and the corresponding solutions of various electrolytes.To fill this gap,it is very meaningful to review the recent progress of SSEs in SSLSBs.In this review,we comprehensively investigate and summarize the application of SSEs in LSBs to determine the differences which still exist between current progresses and real-world requirements,and comprehensively describe the mechanism of action of SSLSBs,including lithium-ion transport,interfacial contact,and catalytic conversion mechanisms.More importantly,the selection of solid electrolyte materials and the novel design of structures are reviewed and the properties of various SSEs are elucidated.Finally,the prospects and possible future research directions of SSLSBs including designing high electronic/ionic conductivity for cathodes,optimizing electrolytes and developing novel electrolytes with excellent properties,improving electrode/-electrolyte interface stability and enhancing interfacial dynamics between electrolyte and anode,using more advanced test equipment and characterization techniques to analyze conduction mechanism of Li^(+)in SSEs are presented.It is hoped that this review can arouse people’s attention and enlighten the development of functional materials and novel structures of SSEs in the next step.

High-performance solid-state lithium metal batteries achieved by interface modification

Garnet-structured ceramic electrolyte Li_(6.75)La_(3)Zr_(1.75)Ta_(0.25)O_(12)(LLZTO)attracts significant consideration in solid-state Li metal batteries due to its wide electrochemical window and favorable compatibility with Li metal.However,the deployment of LLZTO is severely hampered by poor contact between LLZTO and Li metal anode.In this paper,an ultra-thin Al-Si interface buffer layer(10 nm)is constructed on LLZTO by a magnetron sputtering method,which allows superior wetting of Li onto the LLZTO surface due to the alloying reaction between the Al-Si layer and Li metal.The resulting Li/Al-Si coated LLZTO(ASL)/Li symmetrical cell delivers an interfacial resistance of 15.0Ωcm^(-2),which is much lower than that of 1140.3Ωcm^(-2)for the bare LLZTO symmetrical cell.Moreover,the Li/ASL/Li symmetrical cells exhibit stable plating/striping performance(800 h)with small voltage hysteresis at 1.0 mA cm^(-2).Besides,the full cell with LiFePO_(4)cathode reveals a high capacity of 124.1 mA h g^(-1)after 600 cycles at 0.5C with a lowcapacity decay of 0.032%per cycle.We believe this work will facilitate the development of solid-state rechargeable batteries.

Performance Evaluation of Composite Electrolyte with GQD for All-Solid-State Lithium Batteries

The use a stabilized lithium structure as cathode material for batteries could be a fundamental alternative in the development of next-generation energy storage devices.However,the lithium structure severely limits battery life causes safety concerns due to the growth of lithium(Li)dendrites during rapid charge/discharge cycles.Solid electrolytes,which are used in highdensity energy storage devices and avoid the instability of liquid electrolytes,can be a promising alternative for next-generation batteries.Nevertheless,poor lithium ion conductivity and structural defects at room temperature have been pointed out as limitations.In this study,through the application of a low-dimensional graphene quantum dot(GQD)layer structure,stable operation characteristics were demonstrated based on Li^(+)ion conductivity and excellent electrochemical performance.Moreover,the device based on the modified graphene quantum dots(GQDs)in solid state exhibited retention properties of 95.3%for 100 cycles at 0.5 C and room temperature(RT).Transmission electronmicroscopy analysis was performed to elucidate the Li^(+)ion action mechanism in the modified GQD/electrolyte heterostructure.The low-dimensional structure of theGQD-based solid electrolyte has provided an important strategy for stably-scalable solid-state lithium battery applications at room temperature.It was demonstrated that lithiated graphene quantum dots(Li-GQDs)inhibit the growth of Li dendrites by regulating the modified Li^(+)ion flux during charge/discharge cycling at current densities of 2.2–5.5 mA cm,acting as a modified Li diffusion heterointerface.A full Li GQDbased device was fabricated to demonstrate the practicality of the modified Li structure using the Li–GQD hetero-interface.This study indicates that the low-dimensional carbon structure in Li–GQDs can be an effective approach for stabilization of solid-state Li matrix architecture.