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Hybridelectrolytes are organic electrolytes comprising inorganicnano-particles covalently bonded with at least one anion of anorganic sodium or lithium salt. Hybrid electrolytes are comprised ofnano-scale silica or organic hybrid materials (NOHMS) [1]. They arethe most suitable electrolytes for Li-ion and sodium batteries forbeen specifically solvent free. In this type of electrolyte, theparticle cores are uniformly dispersed and the chain of polyethyleneelements are bonded covalently [2]. In addition, they are completelyself-suspended and contribute to give rise to homogeneous fluids. Inhybrid electrolytes, the oligomers of polyethylene glycol (PEG) serveas the suspended media of the small particle cores. The same PEGoligomer works as a supportive element in the transportation oflithium ions in an ion-conducting network [3, 4]. It is thereforeimportant to identify and understand the structural features ofhybrid electrolytes affecting performance.


Thefollowing are the properties and characteristics that determine theoutline and structure of hybrid electrolytes. Aspects such aselectromechanical stability, lithium ion conductivity and lithiumtransference number are addressed. Electromechanical stability ofhybrid electrolytes is above 5V which implies a high conductivitycapacity of lithium ions [5]. Ionicconductivity of hybrid electrolytes is in the scope of 10−2&nbsp–10−4&nbspS&nbspcm−1atroom temperature increasing the electrical conductivity of theelectrolyte. The electrochemical stability window is approximately 4Vversus Li/Li+.The high voltage window ensures that hybrid electrolytes are noteither oxidized or chemically reduced which therefore increases theperformance window of the electrolytes. Most hybrid electrolytesfurthermore have a high temperature steadiness of 400°C and shearmechanical moduli of 105–106 Pascal [6].Consequently, the electrolyte can successfully perform under extremeenvironments such as high temperature and pressure. Lithiumtransference numbers (0.35± 0.04)are expanded within the ions, at a molecule stacking of 48 in volumepercentage [7][8].Thisis due to lithium ions in the electrolyte been the only mobile ionsand implies that conductivity of lithium ions is dependent uponsimply these mobile ions.The short circuit time of lithium metal battery in light of ionicfluid nano-ions half breed electrolytes demonstrates that ionic fluidnano-particles electrolytes can successfully impede the developmentof lithium dendrites [9].Subsequently, the durability of lithium ions batteries is increasedas the electrolyte does not promote high formation of dendrites.Nano-particles can avoid space charge by changing the anion fixation.As a result of the solid mechanical properties, the nucleateddendrites are difficult to short circuit in such a battery [10].These properties make hybrid electrolytes among the safest batteriesdue to the minimization of short circuits, other than consistence ofcomposite features.

Thehybrid materials possess composite properties which consist ofcomponents at the molecular and non-molecular levels. Additionally,the mixing of a component at the microscopic level makes it ahomogeneous material [11].

Naturalmaterials that are used in making hybrid electrolytes usually consistof organic and inorganic building blocks distributed at the level ofnano-scale. In many conditions, the inorganic portion stimulates thedevelopment of mechanical strength and building of an overallarrangement of natural object [12]. The organic portion strengthensthe bonding in between soft tissues and building blocks of inorganiccompounds. Nacres or bones are two typical examples of such a hybridelectrolytic materials. The hybrid properties can be classified intotwo major parts based on the potential interaction of organic andinorganic species [13].

Class-Ihybrid materials are comprised of all those that show very poorinteraction in between two phases such as weak electrostatic force,hydrogen bonding or van der Waals` forces. In class-II however, allthe hybrid materials are included indicating very strong chemicalreaction. The interaction of such materials in between components isattained through covalent bonds [14] [15]. Hybrid electrolytes havestructural differences with the same properties in solid electrolytesincluding lithium ion conductivity, electrochemical stability andtemperature steadiness. Solid electrolytes are discussed below tooffer an insight where one can see these structural differences fromhybrid electrolytes.


Technologyin the manufacture of Li-ion batteries is moving towards dry cellsand consequently, solid electrolytes have become more common [16].Partly, this is due to solid electrolyte’s simplified handlingmethods since liquid electrolyte can be spilled easily from theircasing [17].Solid electrolytes also pose a safer alternative and increaseddurability of the batteries. The utilization of a solid electrolytesimplifies the battery design process because it does not need cellsinside the battery, as compared to liquid electrolytes, decreasingproduction costs as well as time expenditure [18].When selecting the solid electrolyte for Li-ion batteries, the twomost important aspects to take into consideration are ionicconductivity and electrode durability. Durability determines the downtime during which the Li-ion battery will be under maintenance [19].Two main types of solid electrolytes are organic polymers andinorganic ceramics. Mechanically, the organic polymers are lesselastic making them less flexible [20][21].Lithium ion conduction is achieved in polymer solid electrolytesthrough addition of solvating lithium salts such as poly ethyleneoxide (PEO). On the other hand, ionic conductivity in organicceramics is directly dependent on temperature [22].An increase in temperature causes a proportional increase in ionicconductivity through point defect movements. Inorganic ceramics havehigh elastic limit making them optimum for use in a battery designedto operate in rigid and harsh environments. Sulfide, oxide, andphosphate compounds are commonly used as inorganic ceramics in solidelectrolytes.

Gel/ Polymer Electrolyte

Advancingtechnology has enabled incorporation of ionic liquids in organicelectrolyte solution to increase ionic conductivity and stabilizelithium ions [23]. Gel or polymer electrolytes possess variousadvantages over solid state ceramic electrolytes includingflexibility and processing ability [24]. This electrolyte also hasvarious advantages as compared to liquid electrolyte including highersafety, dimensional stability and the capability to prevent dendriteformation on the lithium material [25][26][27]. In some particulargel or polymer electrolytes, polymer chains and lithium salts aresolvated while in other electrolyte variations, solvents areincorporated for the formation of polymer gel [28][29]. Generally,the former mechanical strength prevents the formation offree-standing film [30]. On the other hand, the gel or polymerelectrolytes require strong mechanical support as compared to othercomponents of the battery despite the higher ionic conductivity[31][32][33]. In this type of electrolyte, no shape restrictionexists. The power density value is additionally much higher and therate of charging and discharging cycles is faster [34]. Polymerelectrolytes oligomers are considered the major host matrix andefficiently used in Li-ion batteries. The conduction process oflithium ions in gel or polymer electrolytes is done through thecomplexities in between an oxygen atom and a lithium ion [35]. Thisis an important aspect that can enhance a deeper understanding of theproperties of gel polymer electrolytes.


Themost relevant characteristics of gel/polymer electrolytes includeconductivity of lithium ions, mobility and carrier concentration,electromechanical stability, and flexibility of the electrolytes.Conductivity of gel polymer electrolytes ions can reach5.5&nbsp×&nbsp10−3&nbspS&nbspcm−1at a room temperature (typically 25&nbsp°C) [36]. Temperaturedependence of the ionic conductivity is consistent in a temperaturerange of 20–90&nbsp°C. Under the same conditions, goodcharge–discharge properties and stable cycle performance areprevalent. While the polymer fraction in gel increases, the diffusioncoefficient of gel in the electrolyte decreases. The carrierconcentration shows an order 3 magnitude variation and 80% to 20% offraction change in the polymer volume therefore, demonstrating thatwhen the polymer interacts with the electrolyte, the mobility of gelelectrolytes and carrier concentration are affected [37]. The overallinteractive effect is detected throughout the measurement of relationtime of spin lattice [38]. The deviation of temperature of symmetriccurve with respect to the relation time of spin lattice is dividedinto two major components. The first component is dependent on thevalue of polymer fraction in gel and the second is constant withcomponent solution.

Ionicliquids at room temperature have been extensively used as supportiveelectrolytes and organic solvents in scientific research. This ismostly due to the significant properties such as non-flammability,high ion conductivity and non-volatility that they possess.Considerable improvement on non-volatility is due to theelectrochemical and thermal properties of polymer and conductivity ofionic liquids. The combination of different gel electrolytes hasdemonstrated that ionic liquids work as the charge carriers as wellas the plasticizers in gel electrolytes. During such process,superior properties and simplified preparation is expected. Thecopolymers and ionic liquids are incorporated for the formation ofgel or polymer electrolytes. To acquire the needed target lithiumions, inorganic salts are added such as LiCF3SO3,LiClO4 and LiBF4.The gel or polymer electrolytes that contain ionic liquid areprominently dependent on the nature and content of ionic liquid andlithium salts [39].

Electrochemicalstability window of the gel polymer electrolytes is usually 5V at25&nbsp°C [40]. The frequency of impedance at the anode and cathodecan directly affect dynamic mechanical properties of polymers thereason is the equivalence of time and temperature in the polymermaterials. As the value of frequency increases, the modulus (measureof elastic property of gel polymers when subjected to deformingforces such as tension) values also increase moderately. There arefour major materials for gel or polymer electrolytes poly-vinylidenefluoride (PVdF), poly-methyl methacrylate (PMMA), poly-acrylonitrile(PAN) and polyethylene oxide (PEO) [41].

Whenproperly processed, the ionic liquid gel electrolytes arefreestanding and flexible films [42]. The freestanding propertyenables the electrolyte to have a self-supportive mechanismcharacterized by the physical appearance of gel. Consequently, thephysical stability of polymer electrolyte is improved and theirhandling process becomes simpler than liquid electrolyte’s. Whilestill stable, the nature of gel polymer electrolyte is one with highion conductivity rate. This is attributed to the flexible nature ofgel which enables efficient conduction of lithium ions within theelectrolyte. Since gel polymer electrolytes are nonvolatile andthermally stable, the electrolytes can operate at elevatedtemperatures without performance degradation. This therefore helps inrepresenting a critical characteristic due to the interference causedby the exposure to harsh environments affecting the performance ofthe battery. In such a case, a Li-ion battery having gel polymerelectrolyte has higher probability of remaining in operation even asthe temperature increases [43]. From the ionic conductivity property,if the temperature of operation reaches 90 degrees centigrade, thebattery would still have its functional performance. These featureshave potential differences with the close solid electrolytes commonlyknown as solid state ceramic electrolytes.

Solid-stateCeramic Electrolyte

Solidstate ceramic electrolytes are those that exist in solid orcrystalline form. Ceramic electrolyte has several added advantagesfrom liquid electrolytes, as is with gel polymer electrolytes. Acouple of these include better handling system, increased safety andincreased durability. Developing solid electrolyte batteries usingceramic membrane separators involves a sodium metal anode with asodium conductive ceramic membrane. Lithium anode with lithiumconductive ceramic membrane is another viable alternative [44].Utilization of these lightweight energetic anodes combined with aceramic separator allows for Li-ion battery systems to acquire veryhigh specific energy and energy densities. Some designs alsoeliminate binders and separators. Solid-state ceramic designs arefocused on preventing overheating and catching fire since the solidelectrolyte prevents dendrites from creating short circuits withinthe battery [45].Acceptance of solid state electrolytes has been limited to poorconductance of such materials. Thevalue of ionic conductivity is high in ceramics due to their openstructure. Single cation conduction in a ceramic material belongs tothe decoupled system.Ina decoupled system, the relaxation mode of ion conduction isdecoupled with the mode of structural relaxation [47]. The crystalpossesses super-ionic conduction capacity as the metastable phase isusually formed from the inorganic and ceramic electrolytes [47]. Theprocess of ionic conduction in ceramic materials arises from to themovement of ionic points. Conductivity of such electrolytes increaseswith gradual increase in temperature. There are various examples ofinorganic ceramics that conduct lithium-ions and which have beenfurther investigated for the purpose of Li-ion battery improvement.


Themost relevant properties to consider for an efficient ceramicelectrolyte include conductivity of lithium ions, electromechanicalcharacteristics, transference number and defects present in solidceramic electrolytes. Glass ceramics or solid ceramic electrolyteshave a conductivity of 2×10−4&nbspScm−1&nbspatroom temperature and activation energy of 27 kJ mol−1[46].Solidceramic compounds are present in crystalline, partially crystallineand amorphous forms and have been extensively used in the conductionof lithium ions. The conductivities of Li2S–P2S5&nbspforexample are presented in Figure 1.

Afterthe crystallization process, conductivity of glass ceramics is muchhigher as compared to other glasses at lower temperatures [48].This indicates that the crystalline phase has low activation energyof ions (approximately 0.1eV) and high conductivity than theamorphous phase [49].Although there are a couple of exceptional cases, some ceramicglasses exhibit a decrease in conductivity due to crystallization[50]. Solid ceramic electrolytes are majorly used in the batteries oflithium-indium anodes and combined with various cathodes such assulfide and copper-molybdenum, copper and nickel. These cathodesoperate with lithium ions at the potential level of 2-3V [51]

Solidceramic electrolytes also have a wide electrochemical window of 5Vand are thus electrochemically stable.When a solid ceramic electrolytes are used with aNiP2&nbspcathode&nbsp(usuallyin Li-ion batteries), the electrolyte operates at the lower potential[52].The conductivities of ions in most solid ceramic electrolytes such assulfides arealso quite similar.Conductivity of such electrolytes can be improved with the additionof lithium silicates (Li4SiO4)as well as lithium iodide [53].Similarly, theconductivity of Li2S–P2S5andLi2S–Ga2S3–GeS2resembleeach other and can be enhanced with the addition of iodide.Some of the lithium ions have the ability to conduct sulfide crystalsand are referred to as thio-LISICON [54].

Lithiumtransference number is less than 1.0 for most ceramic electrolytes(the value is approximately 0.95) [55]. Dueto the high conductivity of lithiumions,there is a low polarization and a high value of capacity of&nbspcathodesused in solid ceramic electrolytes in comparison tographite anode. Adding oxygen to solidceramic electrolytes&nbspresultsin an increment in ion conductivity [56].This is attributed to an increase in lithium coordination number, buta greater amount of oxygen results in a decrease of free volume whicheventually leads to a decrease in conductivity.

Inorder for a lithium ion to acquire the ability to move through acrystal it must be transported from an occupied site to a vacant site[57]. Ionic conductivity thus can only occur if defects are present. Thetwo simple types of point defects are Schottky and Frenkel defects[58]. In Schottky defects, sodium and sodium chloride ions existingin crystal form squezze through the crystal lattice thereby leadingto a distortion called Schottky defect. In Frenkel defects, silverchloride ions push along the sides of the crystal lattice diagonallyor transversely causing horizontal or Frenkel defects. Such defectsaffect the direction as well as the conductivity of lithium ionswithin the crystal lattice.

Alarge number of the ions of one species should further improvemobility [59]. This requires a large number of empty sites, eithervacancies or accessible interstitial sites to increase transfer oflithium, sodium or silver ions depending on the element making up thecrystal electrolytes. Ceramic electrolytes exhibit fast lithium ionmotion due to rotational disorder and the existence of vacancies inthe lattice as previously mentioned [60]. The combination of possiblestructural variations of the plastic crystal matrix andconductivities as high as 0.0002 S cm-1 at 60°C make these materialsvery attractive for solid electrolyte Li-ion battery applications.

*Source: (Hayashi,Noi, Sakuda, and Tatsumisago, 2012 , p.856)

Adifferential thermal analysis (DTA) curve is shown above withtemperature dependence of conductivities for the solid glass–ceramicselectrolytes. The DTA curve of the solid ceramic electrolytes showsan endothermic change of glass transition phenomena at 210&nbsp°C(Tg)and several exothermic peaks attributable to crystallization over(Tg).

Inconclusion, sulfide glass-based ceramics solid electrolytes are themost suitable for use as solid-state Li-ion batteries. This is due tothe improved conductivity of lithium ions in the amorphous form ofthe electrolyte. The majority of solid state ceramic electrolyteshave showed significant cycling performance. To obtain a highperformance rate, ions should be smoothly supplied to activematerials by interfacing electrolytes and electrodes. All solid statebatteries in which sulfide glass network is commonly used aselectrolytes and electrodes are successfully fabricated.

Voltagevs. Li/Li+ for Germanium and lithium oxide is 0.2-2.1


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