Solid-state electrolyte

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All Solid-State Battery with the solid-state electrolyte. All-Solid-State Battery.png
All Solid-State Battery with the solid-state electrolyte.

A solid-state electrolyte (SSE) is a solid ionic conductor and electron-insulating material and it is the characteristic component of the solid-state battery. It is useful for applications in electrical energy storage in substitution of the liquid electrolytes found in particular in the lithium-ion battery. [1] [2] Their main advantages are their absolute safety, no issues of leakages of toxic organic solvents, low flammability, non-volatility, mechanical and thermal stability, easy processability, low self-discharge, higher achievable power density and cyclability. [3] This makes possible, for example, the use of a lithium metal anode in a practical device, without the intrinsic limitations of a liquid electrolyte thanks to the property of lithium dendrite suppression in the presence of a solid-state electrolyte membrane. The use of a high-capacity and low reduction potential anode, like lithium with a specific capacity of 3860 mAh g−1 and a reduction potential of -3.04 V vs standard hydrogen electrode, in substitution of the traditional low capacity graphite, which exhibits a theoretical capacity of 372 mAh g−1 in its fully lithiated state of LiC6, [4] is the first step in the realization of a lighter, thinner and cheaper rechargeable battery. [5] This allows for gravimetric and volumetric energy densities high enough to achieve 500 miles per single charge in an electric vehicle. [6] Despite these promising advantages, there are still many limitations that are hindering the transition of SSEs from academic research to large-scale production, mainly the poor ionic conductivity compared to that of liquid counterparts. However, many car OEMs (Toyota, BMW, Honda, Hyundai) expect to integrate these systems into viable devices and to commercialize solid-state battery-based electric vehicles by 2025. [7] [8]

Contents

History

The first inorganic solid-state electrolytes were discovered by Michael Faraday in the nineteenth century, these being silver sulfide (Ag2S) and lead(II) fluoride (PbF2). [9] The first polymeric material able to conduct ions at the solid-state was PEO, discovered in the 1970s by V. Wright. The importance of the discovery was recognized in the early 1980s. [10] [11]

However, unresolved fundamental issues remain in order to fully understand the behavior of all-solid batteries, especially in the area of electrochemical interfaces. [12] In recent years the needs of safety and performance improvements with respect to the state-of-the-art Li-ion chemistry are making solid-state batteries very appealing and are now considered an encouraging technology to satisfy the need for long range battery electric vehicles of the near future.

In March 2020, the Samsung Advanced Institute of Technology (SAIT) published research on an all-solid-state battery (ASSB) using an argyrodite-based solid-state electrolyte with a demonstrated energy density of 900 Wh L−1 and a stable cyclability of more than 1000 cycles, reaching for the first time a value close to the 1000 Wh L−1. [13]

Properties

For Solid State Batteries (SSBs) / Solid Electrolytes (SEs) to become a major market challenger it must meet some key performance measurements. [14] [15] [16] The major criteria that an SSB/SE should have are: [12] [17]

It is hard for one material to fulfill all the above criteria, hence a number of other approaches can be used for example a hybrid electrolyte system which combines the advantages of inorganic and polymer electrolytes.

Categories

SSEs have the same role of a traditional liquid electrolyte and they are classified into all-solid-state electrolyte and quasi-solid-state electrolyte (QSSE). All-solid-state electrolytes are furthermore divided into inorganic solid electrolyte (ISE), solid polymer electrolyte (SPE) and composite polymer electrolyte (CPE). On the other hand, a QSSE, also called gel polymer electrolyte (GPE), is a freestanding membrane that contains a certain amount of liquid component immobilized inside the solid matrix. In general the nomenclatures SPE and GPE are used interchangeably but they have a substantially different ionic conduction mechanism: SPEs conducts ions through the interaction with the substitutional groups of the polymer chains, while GPEs conducts ions mainly in the solvent or plasticizer. [23]

All-solid-state electrolyte

All-solid-state electrolytes are divided into inorganic solid electrolyte (ISE), solid polymer electrolyte (SPE) and composite polymer electrolyte (CPE). They are solid at room temperature and the ionic movement occurs at the solid-state. Their main advantage is the complete removal of any liquid component aimed to a greatly enhanced safety of the overall device. The main limitation is the ionic conductivity that tends to be much lower compared to a liquid counterpart. [24]

Inorganic solid electrolyte (ISE)

Inorganic solid electrolyte (ISE) are a particular type of all-solid-state electrolyte that is constituted by an inorganic material in the crystalline or glassy state, that conducts ions by diffusion through the lattice. [25] The main advantages of this class of solid-state electrolyte are the high ionic conductivity (of the order of a few mS cm−2 at room-temperature), high modulus (of the order of GPa) and high transfer number compared to other classes of SSEs. [26] They are generally brittle and with this comes a low compatibility and stability towards the electrode, with a rapidly increasing interfacial resistance and a complicated scale-up from academic to industry. [27] They can be oxides, sulfides or phosphates-based and the crystalline structures include LISICON (lithium superionic conductor) (e.g. LGPS, LiSiPS, LiPS), argyrodite-like (e.g. Li6PS5X, X = Cl, Br, I), [28] garnets (LLZO), [29] NASICON (sodium superionic conductor) (e.g. LTP, LATP, LAGP), [30] lithium nitrides (e.g. Li3N), [31] lithium hydrides (LiBH4), [32] lithium phosphidotrielates [33] and phoshidotetrelates, [34] perovskites (e.g. lithium lanthanum titanate, "LLTO"), [35] lithium halides (LYC, LYB)., [36] RbAg4I5. [37] [38] Some ISEs can be glass ceramics assuming an amorphous state instead of a regular crystalline structure. Popular examples are lithium phosphorus oxynitride (LIPON) [39] and the lithium thiophosphates (Li2S–P2S5). [40]

Solid polymer electrolyte (SPE)

Solid polymer electrolytes (SPE) are defined as a solvent-free salt solution in a polymer host material that conducts ions through the polymer chains. Compared to ISEs, SPEs are much easier to process, generally by solution casting, making them greatly compatible with large-scale manufacturing processes. Moreover, they possess higher elasticity and plasticity giving stability at the interface, flexibility and improved resistance to volume changes during operation. [23] A good dissolution of Li salts, low glass transition temperature (Tg), electrochemical compatibility with most common electrode materials, a low degree of crystallinity, mechanical stability, low temperature sensitivity are all characteristics for the ideal SPE candidate. [41] In general though the ionic conductivity is lower than the ISEs and their rate capability is restricted, limiting fast charging. [42] PEO-based SPE is the first solid-state polymer in which ionic conductivity was demonstrated both through inter and intra molecular through ion hopping, thanks to the segmental motion of the polymeric chains [43] because of the great ion complexation capability of the ether groups, but they suffer from the low room-temperature ionic conductivity (10−5 S cm−1) [44] due to the high degree of crystallinity.

Copolymerization, [45] crosslinking, [46] interpenetration, [47] and blending [48] may also be used as polymer/polymer coordination to tune the properties of the SPEs and achieve better performances, introducing in the polymeric chains polar groups like ethers, carbonyls or nitriles drastically improve the dissolution of the lithium salts. Thus the main alternatives to polyether-based SPEs are polycarbonates, [49] polyesters, [50] polynitriles (e.g. PAN), [51] polyalcohols (e.g. PVA), [52] polyamines (e.g. PEI), [53] polysiloxane (e.g. PDMS) [54] [55] and fluoropolymers (e.g. PVDF, PVDF-HFP). [56] Bio-polymers like lignin, [57] chitosan [58] and cellulose [59] are also gaining a lot of interest as standalone SPEs or blended with other polymers, on one side for their environmentally friendliness and on the other for their high complexation capability on the salts. Furthermore, different strategies are considered to increase the ionic conductivity of SPEs and the amorphous-to-crystalline ratio. [60]

Composite electrolytes

Traditional ISEs, like garnet-based (LLZO) and sulfide-based (LGPS) electrolytes, have poor mechanical compatibility with lithium electrodes. The poor interfacial contact with lithium metal anodes leads to high interfacial resistance and unstable cycling performance, which restricts practical use in all-solid-state batteries. [61] [62] Thin-film interfacial coatings with lithium phosphorus oxynitride (LiPON), lithium niobate (LiNbO3), and aluminum oxide (Al2O3) have been proposed to mitigate the problem. [63] [64] Alternatively, high-pressure sintering can densify the contact between the electrolyte and electrodes, improving ionic transport pathways and reducing interface resistance. [65]

Dual-phase electrolytes, such as LLZO-LGPS composites, leverage the high conductivity of sulfides and the chemical stability of oxides, leading to improved overall electrochemical performance in solid-state batteries. [66]

Another alternative are composite solid electrolytes (CSEs), which integrate small inorganic particles into a polymeric matrix. These materials combine the high ionic conductivity of inorganic phases with the flexibility and improved electrode compatibility of polymers. [67] The particles can be inert to the Li+ conduction (Al2O3, TiO2, SiO2, MgO, zeolite, montmorillonite, ...), [68] [69] [70] with the sole purpose of reducing the crystallinity, or active (LLTO, LLZO, LATP...); [71] [72] [73] the latter case is called either ceramic-in-polymer and polymer-in-ceramic, depending on stoichiometry. [74]

Quasi-solid-state electrolyte

Comparison of different polymer based quasi-solid-state electrolyes Comparison of Polymer Electrolytes.png
Comparison of different polymer based quasi-solid-state electrolyes

Quasi solid-state electrolytes (QSSEs) are a wide class of composite compounds consisting of a liquid electrolyte and a solid matrix. This liquid electrolyte serves as a percolating pathway of ion conduction while the solid matrix adds mechanical stability to the material as a whole. As the name suggests, QSSEs can have a range of mechanical properties from strong solid-like materials to those in a paste form. [75] [76] [77] QSSEs can be subdivided into a number of categories including gel polymer electrolytes (GPEs), Ionogel electrolytes, [78] and gel electrolytes (also known as "soggy sand" electrolytes). The most common QSSE, GPEs have a substantially different ionic conduction mechanism than SPEs, which conduct ions through the interaction with the substitutional groups of the polymer chains. Meanwhile, GPEs conduct ions mainly in the solvent, which acts as plasticizer. [79] The solvent acts to increase the ionic conductivity of the electrolyte as well as soften the electrolyte for improved interfacial contact. The matrix of GPEs consist of a polymer network swollen in a solvent that contains the active ions (e.g., Li+, Na+, Mg2+, etc.). This allows for the composite to contain both the mechanical properties of solids and the high transport properties of liquids. A number of polymer hosts have been used in GPEs, including PEO, PAN, PMMA, PVDF-HFP, etc. The polymers are synthesized with increased porosity to incorporate solvents such as ethylene carbonate (EC), propylene carbonate (PC), diethyl carbonate (DEC), and dimethyl carbonate (DMC). [80] [81] [82] Low molecular weight poly(ethylene glycol) (PEG) or other ethers or aprotic organic solvents with high dielectric constant like dimethylsulfoxide (DMSO) can also be mixed the SPE matrix. [83] [84] UV and thermal cross-linking are useful ways to polymerize in-situ the GPE directly in contact with the electrodes for a perfectly adherent interface. [85] Values of ionic conductivity on the order of 1 mS cm−1 can be easily achieved with GPEs, as demonstrate the numerous research articles published. [86]

Emerging subclasses of QSSEs use matrix materials and solvents. Ionogels, for example use ionic liquids as a solvent that has improved safety including non-flammability and stability at high temperatures. [78] [87] Matrix materials in ionogels can vary from polymer materials [88] to inorganic nano-materials. [76] These matrix materials (as with all QSSEs) provide mechanical stability with a storage moduli up to 1 MPa or higher. Meanwhile, these materials can provide ionic conductivities on the order of 1 mS cm−1 without using flammable solvents. However, gel electrolytes (i.e. "soggy sand" electrolytes) can achieve liquid-like ionic conductivities (~ 10 mS cm−1) while being in the solid state. Matrix materials such as SiO2 nanoparticles are typically paired with low viscosity solvents (e.g., ethylene carbonate (EC)) to create a gel, whose properties can be modified based on the matrix loading. [89] Matrix content ranging from 10 to 40 wt% can shift the mechanical properties of the electrolyte from a soft paste into a hard gel. [75] However, a tradeoff between mechanical strength and ionic conductivity as one goes up with changing matrix content the other suffers. [90] Despite this, matrix content in these materials can have added benefits including enhanced lithium transference number due to functionalized matrix materials. [91] These new classes of QSSEs are an active area of research to develop the optimal combination of matrix and solvent. [75] [89]

See also

References

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