Detailed Mechanism and Engineering Applicability of Electrolytic Polymerization Aided by a Magnetic Field in Natural Rubber by Mechanical Approach for Sensing (Part 1): The Effect of Experimental Conditions on Electrolytic Polymerization

Ordinary electrolytic polymerization has involved plastic-type polymer solutions. Rubber, especially natural rubber, is one such polymer solution. Rubber has not been focused on until recently due to the fact that electrolytic polymerization has only a very small effect on rubber. However, when we focus on the C=C bonds of natural rubber, the same electrolytic polymerization is applicable to be enlarged on the natural rubber if a magnetic field and a filler are added. With the application of a magnetic field and a magnetic responsive fluid such as magnetic compound fluid (MCF), the effect of electrolytic polymerization on NR-latex such as plastic-type polymer solutions is enhanced, and the thickness of the vulcanized MCF rubber grows in a short time. The present new method of vulcanization of MCF rubber is effective enough that it is widely used in haptic sensors in various engineering applications. In the present report, as mechanical approach for the sensing, by measuring the temperature under electrolytic polymerization, by investigating the electric and dynamic characteristics, and by observing the magnified appearance of the MCF rubber, we clarified the extrinsic effects of many experimental conditions, including magnetic field strength, applied voltage, the electrodes gap, mass concentration, and the ingredients of the MCF. This report is Part 1, to be followed by another sequential report, Part 2, in which other intrinsic effects on the characteristics are dealt with. The experimental conditions used and the results obtained in the present report provide valuable data that will be useful in the making of MCF rubber.

Detailed Mechanism and Engineering Applicability of Electrolytic Polymerization Aided by a Magnetic Field in Natural Rubber by Mechanical Approach for Sensing (Part 2): Other and Intrinsic Effects on MCF Rubber Property

The same ordinary electrolytic polymerization of plastic-type polymer solution is applicable to natural rubber, with its C=C bonds, if a magnetic field and a filler are added. With the application of a magnetic field and the magnetic responsive fluid known as magnetic compound fluid (MCF), we have clarified the enhancement of the electrolytic polymerization of NR-latex and the growth of the thickness of vulcanized MCF rubber that results from the addition of a magnetic field. The present new method of MCF rubber vulcanization is effective for use in haptic sensors, which are used widely in various engineering applications. In the previous report, part 1 of this study, we investigated many experimental conditions under mechanical approach for sensing: magnetic field strength;applied voltage;electrodes gap;mass concentration, and the ingredients of the MCF. In the present sequential report, part 2, we investigate many other effects on electrolytic polymerization by the same mechanical approach for sensing as in part 1: the Mullins effect;the Piezo effect;vibration;kind of electrode;atmospheric gas. In particular, we clarify that the voltage generates spontaneously in the MCF rubber and that the MCF rubber becomes a Piezo element. These effects on the electrolytic polymerization as well as the effects of the experimental conditions will be useful in engineering applications. By taking the above-mentioned parameters and effects into account, MCF rubber that is electrolytically polymerized with the aid of a magnetic field, the use of MCF as a filler, and doping, can be useful in haptic sensor applications. In particular, the effectiveness of the Piezo element can be shown.

Charting the course to solid-state dual-ion batteries

An electrolyte destined for use in a dual-ion battery(DIB)must be stable at the inherently high potential required for anion intercalation in the graphite electrode,while also protecting the Al current collector from anodic dissolution.A higher salt concentration is needed in the electrolyte,in comparison to typical battery electrolytes,to maximize energy density,while ensuring acceptable ionic conductivity and operational safety.In recent years,studies have demonstrated that highly concentrated organic electrolytes,ionic liquids,gel polymer electrolytes(GPEs),ionogels,and water-in-salt electrolytes can potentially be used in DIBs.GPEs can help reduce the use of solvents and thus lead to a substantial change in the Coulombic efficiency,energy density,and long-term cycle life of DIBs.Furthermore,GPEs are suited to manufacture compact DIB designs without separators by virtue of their mechanical strength and electrical performance.In this review,we highlight the latest advances in the application of different electrolytes in DIBs,with particular emphasis on GPEs.

Mechanism of high Li-ion conductivity in poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network based electrolyte revealed by solid-state NMR

Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.

Bacterial Cellulose/Zwitterionic Dual-network Porous Gel Polymer Electrolytes with High Ionic Conductivity

Bacterial cellulose(BC)was innovatively combined with zwitterionic copolymer acrylamide and sulfobetaine methacrylic acid ester[P(AM-co-SBMA)]to build a dual-network porous structure gel polymer electrolytes(GPEs)with high ionic conductivity.The dual network structure BC/P(AM-co-SBMA)gels were formed by a simple one-step polymerization method.The results show that ionic conductivity of BC/P(AM-co-SBMA)GPEs at the room temperature are 3.2×10^(-2) S/cm@1 M H_(2)SO_(4),4.5×10^(-2) S/cm@4 M KOH,and 3.6×10^(-2) S/cm@1 M NaCl,respectively.Using active carbon(AC)as the electrodes,BC/P(AM-co-SBMA)GPEs as both separator and electrolyte matrix,and 4 M KOH as the electrolyte,a symmetric solid supercapacitors(SSC)(AC-GPE-KOH)was assembled and testified.The specific capacitance of AC electrode is 173 F/g and remains 95.0%of the initial value after 5000 cycles and 86.2%after 10,000 cycles.

A new review of single-ion conducting polymer electrolytes in the light of ion transport mechanisms

With the depletion of fossil fuels and the demand for high-performance energy storage devices,solidstate lithium metal batteries have received widespread attention due to their high energy density and safety advantages.Among them,the earliest developed organic solid-state polymer electrolyte has a promising future due to its advantages such as good mechanical flexibility,but its poor ion transport performance dramatically limits its performance improvement.Therefore,single-ion conducting polymer electrolytes(SICPEs)with high lithium-ion transport number,capable of improving the concentration polarization and inhibiting the growth of lithium dendrites,have been proposed,which provide a new direction for the further development of high-performance organic polymer electrolytes.In view of this,lithium ions transport mechanisms and design principles in SICPEs are summarized and discussed in this paper.The modification principles currently used can be categorized into the following three types:enhancement of lithium salt anion-polymer interactions,weakening of lithium salt anion-cation interactions,and modulation of lithium ion-polymer interactions.In addition,the advances in single-ion conductors of conventional and novel polymer electrolytes are summarized,and several typical highperformance single-ion conductors are enumerated and analyzed in what way they improve ionic conductivity,lithium ions mobility,and the ability to inhibit lithium dendrites.Finally,the advantages and design methodology of SICPEs are summarized again and the future directions are outlined.

In-situ polymerized PEO-based solid electrolytes contribute better Li metal batteries:Challenges,strategies,and perspectives

Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)with good electrochemical stability and excellent Li salt solubility are considered as one of the most promising SPEs for solid-state lithium metal batteries(SSLMBs).However,PEO-based SPEs suffer from low ionic conductivity at room temperature and high interfacial resistance with the electrodes due to poor interfacial contact,seriously hindering their practical applications.As an emerging technology,in-situ polymerization process has been widely used in PEO-based SPEs because it can effectively increase Li-ion transport at the interface and improve the interfacial contact between the electrolyte and electrodes.Herein,we review recent advances in design and fabrication of in-situ polymerized PEO-based SPEs to realize enhanced performance in LMBs.The merits and current challenges of various SPEs,as well as their stabilizing strategies are presented.Furthermore,various in-situ polymerization methods(such as free radical polymerization,cationic polymerization,anionic polymerization)for the preparation of PEO-based SPEs are summarized.In addition,the application of in-situ polymerization technology in PEO-based SPEs for adjustment of the functional units and addition of different functional filler materials was systematically discussed to explore the design concepts,methods and working mechanisms.Finally,the challenges and future prospects of in-situ polymerized PEO-based SPEs for SSLMBs are also proposed.

Bifunctional TiO_(2-x)nanofibers enhanced gel polymer electrolyte for high performance lithium metal batteries

Exploration of advanced gel polymer electrolytes(GPEs)represents a viable strategy for mitigating dendritic lithium(Li)growth,which is crucial in ensuring the safe operation of high energy density Li metal batteries(LMBs).Despite this,the application of GPEs is still hindered by inadequate ionic conductivity,low Li^(+)transference number,and subpar physicochemical properties.Herein,Ti O_(2-x)nanofibers(NF)with oxygen vacancy defects were synthesized by a one-step process as inorganic fillers to enhance the thermal/mechanical/ionic-transportation performances of composite GPEs.Various characterizations and theoretical calculations reveal that the oxygen vacancies on the surface of Ti O_(2-x)NF accelerate the dissociation of Li PF_6,promote the rapid transfer of free Li^(+),and influence the formation of Li F-enriched solid electrolyte interphase.Consequently,the composite GPEs demonstrate enhanced ionic conductivity(1.90m S cm^(-1)at room temperature),higher lithium-ion transference number(0.70),wider electrochemical stability window(5.50 V),superior mechanical strength,excellent thermal stability(210℃),and improved compatibility with lithium,resulting in superior cycling stability and rate performance in both Li||Li,Li||Li Fe PO_(4),and Li||Li Ni_(0.8)Co_(0.1)Mn_(0.1)O_(2)cells.Overall,the synergistic influence of nanofiber morphology and enriched oxygen vacancy structure of fillers on electrochemical properties of composite GPEs is comprehensively investigated,thus,it is anticipated to shed new light on designing high-performance GPEs LMBs.

Incombustible solid polymer electrolytes:A critical review and perspective

Since the advent of the solid-state batteries,employing solid polymer electrolytes(SPEs)to replace routine flammable liquid electrolytes is regarded to be one of the most promising solutions in pursing highenergy-density battery systems.SPEs with superior thermal stability,good processability,and high mechanical modulus obtain increasing attentions.However,SPE-based batteries are not impenetrable due to their decomposition and combustibility under extreme conditions.Researchers believe incorporating appropriate flame-retardant additives/solvents/fragments into SPEs can intrinsically reduce their flammability to solve the battery safety issues.In this review,the recent research progress of incombustible SPEs,with special emphasis on flame-retardant structural design,is summarized.Specifically,a brief introduction of flame-retardant mechanism,evaluation index for safety of SPEs,and a detailed overview of the latest advances on diverse-types SPEs in various battery systems are highlighted.The deep insight into thermal ru naway process,the free-standing incombustible GPEs,and the ratio nal design of pouch cell structures may be the main directions to motivate revolutionary next-generation for safety batteries.

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.

High-performance and robust high-temperature polymer electrolyte membranes with moderate microphase separation by implementation of terphenyl-based polymers

Acid loss and plasticization of phosphoric acid(PA)-doped high-temperature polymer electrolyte membranes(HT-PEMs)are critical limitations to their practical application in fuel cells.To overcome these barriers,poly(terphenyl piperidinium)s constructed from the m-and p-isomers of terphenyl were synthesized to regulate the microstructure of the membrane.Highly rigid p-terphenyl units prompt the formation of moderate PA aggregates,where the ion-pair interaction between piperidinium and biphosphate is reinforced,leading to a reduction in the plasticizing effect.As a result,there are trade-offs between the proton conductivity,mechanical strength,and PA retention of the membranes with varied m/p-isomer ratios.The designed PA-doped PTP-20m membrane exhibits superior ionic conductivity,good mechanical strength,and excellent PA retention over a wide range of temperature(80–160°C)as well as satisfactory resistance to harsh accelerated aging tests.As a result,the membrane presents a desirable combination of performance(1.462 W cm^(-2) under the H_(2)/O_(2)condition,which is 1.5 times higher than that of PBI-based membrane)and durability(300 h at 160°C and 0.2 A cm^(-2))in the fuel cell.The results of this study provide new insights that will guide molecular design from the perspective of microstructure to improve the performance and robustness of HT-PEMs.

Novel sandwich structured glass fiber Cloth/Poly(ethylene oxide)-MXene composite electrolyte

Recently,poly(ethylene oxide)(PEO)-based solid polymer electrolytes have been attracting great attention,and efforts are currently underway to develop PEO-based composite electrolytes for next generation high performance all-solid-state lithium metal batteries.In this article,a novel sandwich structured solid-state PEO composite electrolyte is developed for high performance all-solid-state lithium metal batteries.The PEO-based composite electrolyte is fabricated by hot-pressing PEO,LiTFSI and Ti_(3)C_(2)T_(x) MXene nanosheets into glass fiber cloth(GFC).The as-prepared GFC@PEO-MXene electrolyte shows high mechanical properties,good electrochemical stability,and high lithium-ion migration number,which indicates an obvious synergistic effect from the microscale GFC and the nanoscale MXene.Such as,the GFC@PEO-1 wt%MXene electrolyte shows a high tensile strength of 43.43 MPa and an impressive Young's modulus of 496 MPa,which are increased by 1205%and 6048%over those of PEO.Meanwhile,the ionic conductivity of GFC@PEO-1 wt%MXene at 60℃ reaches 5.01×10^(-2) S m^(-1),which is increased by around 200%compared with that of GFC@PEO electrolyte.In addition,the Li/Li symmetric battery based on GFC@PEO-1 wt%MXene electrolyte shows an excellent cycling stability over 800 h(0.3 mA cm^(-2),0.3 mAh cm^(-2)),which is obviously longer than that based on PEO and GFC@PEO electrolytes due to the better compatibility of GFC@PEO-1 wt%MXene electrolyte with Li anode.Furthermore,the solid-state Li/LiFePO_(4) battery with GFC@PEO-1 wt%MXene as electrolyte demonstrates a high capacity of 110.2–166.1 mAh g^(-1) in a wide temperature range of 25–60C,and an excellent capacity retention rate.The developed sandwich structured GFC@PEO-1 wt%MXene electrolyte with the excellent overall performance is promising for next generation high performance all-solid-state lithium metal batteries.

The Critical Role of Fillers in Composite Polymer Electrolytes for Lithium Battery

With excellent energy densities and highly safe performance,solidstate lithium batteries(SSLBs)have been hailed as promising energy storage devices.Solid-state electrolyte is the core component of SSLBs and plays an essential role in the safety and electrochemical performance of the cells.Composite polymer electrolytes(CPEs)are considered as one of the most promising candidates among all solid-state electrolytes due to their excellent comprehensive performance.In this review,we briefly introduce the components of CPEs,such as the polymer matrix and the species of fillers,as well as the integration of fillers in the polymers.In particular,we focus on the two major obstacles that affect the development of CPEs:the low ionic conductivity of the electrolyte and high interfacial impedance.We provide insight into the factors influencing ionic conductivity,in terms of macroscopic and microscopic aspects,including the aggregated structure of the polymer,ion migration rate and carrier concentration.In addition,we also discuss the electrode-electrolyte interface and summarize methods for improving this interface.It is expected that this review will provide feasible solutions for modifying CPEs through further understanding of the ion conduction mechanism in CPEs and for improving the compatibility of the electrode-electrolyte interface.

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.

Bifunctional flame retardant solid-state electrolyte toward safe Li metal batteries

Solid polymer electrolytes(SPEs)are one of the most promising alternatives to flammable liquid electrolytes for building safe Li metal batteries.Nevertheless,the poor ionic conductivity at room temperature(RT)and low resistance to Li dendrites seriously hinder the commercialization of SPEs.Herein,we design a bifunctional flame retardant SPE by combining hydroxyapatite(HAP)nanomaterials with Nmethyl pyrrolidone(NMP)in the PVDF-HFP matrix.The addition of HAP generates a hydrogen bond network with the PVDF-HFP matrix and cooperates with NMP to facilitate the dissociation of Li TFSI in the PVDF-HFP matrix.Consequently,the prepared SPE demonstrates superior ionic conductivity at RT,excellent fireproof properties,and strong resistance to Li dendrites.The assembled Li symmetric cell with prepared SPE exhibits a stable cycling performance of over 1200 h at 0.2 m A cm^(-2),and the solid-state LiFePO_4||Li cell shows excellent capacity retention of 85.3%over 600 cycles at 0.5 C.

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.

Ultrathin poly(cyclocarbonate-ether)-based composite electrolyte reinforced with high-strength functional skeleton

Composite polymer electrolytes(CPEs)are considered to be the most promising to break through the performance and safety limitations of traditional lithium-ion batteries because of their excellent electrochemical and mechanical properties.Aiming at the performance limitations of the most common polyether matrix such as poly(ethylene oxide)(PEO),a novel poly(cyclocarbonate-ether)polymer matrix was prepared by in-situ thermal curing,the weaker interaction between its C=O bond and Li^(+)can promote the rapid transport of Li^(+).Adding ionic liquid and active filler LLZTO to the matrix can synergistically reduce the crystallinity of matrix and promote the dissociation of lithium salts.In addition,a 3D functional skeleton made of polyacrylonitrile(PAN)and lithium fluoride(LiF)can greatly improve the mechanical strength of polymer matrix after cold pressing,and Li F is also conducive to interface stability.The thickness of the optimal sample(VP6L/CPL)was only 25μm,and its ionic conductivity,lithium ion transference number,and electrochemical stability window were as high as 7.17×10^(-4)S cm^(-1)(25℃),0.54 and 5.4 V,respectively,while the mechanical strength reaches 6.1 MPa,which can fully inhibit the growth of lithium dendrites.The excellent electrochemical performance and mechanical strength enable the assembled Li|VP6L/CPL|Li battery to be continuously charged for over 200 h and cycled stably for more than 2300 h,and Li|VP6L/CPL|LFP battery can be stably cycled for more than 400 and 550 cycles at 1 C(40℃)and 0.5 C(25℃),respectively.

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.

Optimized CeO_(2) Nanowires with Rich Surface Oxygen Vacancies Enable Fast Li-Ion Conduction in Composite Polymer Electrolytes

Low-cost and flexible solid polymer electrolytes are promising in all-solid-state Li-metal batteries with high energy density and safety.However,both the low room-temperature ionic conductivities and the small Li^(+)transference number of these electrolytes significantly increase the internal resistance and overpotential of the battery.Here,we introduce Gd-doped CeO_(2) nanowires with large surface area and rich surface oxygen vacancies to the polymer electrolyte to increase the interaction between Gd-doped CeO_(2) nanowires and polymer electrolytes,which promotes the Li-salt dissociation and increases the concentration of mobile Li ions in the composite polymer electrolytes.The optimized composite polymer electrolyte has a high Li-ion conductivity of 5×10^(-4)4 S cm^(-1) at 30℃ and a large Li+transference number of 0.47.Moreover,the composite polymer electrolytes have excellent compatibility with the metallic lithium anode and high-voltage LiNi_(0.8)Mn _(0.1)Co_(0.1)O_(2)(NMC)cathode,providing the stable cycling of all-solid-state batteries at high current densities.

High-Performance Quasi-Solid-State Pouch Cells Enabled by in situ Solidification of a Novel Polymer Electrolyte

Conventional lithium-ion batteries(LIBs)with liquid electrolytes are challenged by their big safety concerns,particularly used in electric vehicles.All-solid-state batteries using solid-state electrolytes have been proposed to significantly improve safety yet are impeded by poor interfacial solid–solid contact and fast interface degradation.As a compromising strategy,in situ solidification has been proposed in recent years to fabricate quasi-solid-state batteries,which have great advantages in constructing intimate interfaces and cost-effective mass manufacturing.In this work,quasi-solid-state pouch cells with high loading electrodes(≥3 m Ah cm^(-2))were fabricated via in situ solidification of poly(ethylene glycol)diacrylate-based polymer electrolytes(PEGDA-PEs).Both single-layer and multilayer quasi-solid-state pouch cells(2.0 Ah)have demonstrated stable electrochemical performance over500 cycles.The superb electrochemical stability is closely related to the formation of robust and compatible interphase,which successfully inhibits interfacial side reactions and prevents interfacial structural degradation.This work demonstrates that in situ solidification is a facile and cost-effective approach to fabricate quasi-solid-state pouch cells with both excellent electrochemical performance and safety.