Solid electrolyte slurry, preparation method therefor, and all-solid-state battery manufactured using same

Abstract

A solid electrolyte slurry according to a concept of the present invention comprises a compound represented by formula 1. <Formula 1> In formula 1, R1 is hydrogen or an alkyl group, X1 and X2 are each independently O, N, or S, and L1 is a linear or branched alkylene.

Description

Solid electrolyte slurry, method for producing the same, and all-solid-state battery produced thereby

[0001] The present invention relates to a solid electrolyte slurry, a method for producing the same, a solid electrolyte layer produced thereby, and an all-solid-state battery.

[0002] Recent industrial demands have led to the active development of batteries with high energy density and safety. For example, lithium-ion batteries are being used not only in information and communication devices, but also in the automotive sector. Safety is particularly important in the automotive sector, as it is directly related to life.

[0003] All-solid-state batteries are being proposed, replacing the electrolyte with a solid electrolyte. By eliminating the use of flammable organic dispersion media, all-solid-state batteries can significantly reduce the risk of fire or explosion in the event of a short circuit.

[0004] The problem to be solved by the present invention is to provide a solid electrolyte slurry with improved dispersion characteristics.

[0005] Another problem that the present invention seeks to solve is to provide an all-solid-state battery with improved reliability.

[0006] Another problem to be solved by the present invention is to provide a method for producing a solid electrolyte slurry capable of improving the dispersion characteristics of the solid electrolyte slurry.

[0007] According to the concept of the present invention, a solid electrolyte slurry comprises a compound represented by the following chemical formula 1.

[0008] <Chemical Formula 1>

[0009]

[0010] In the above chemical formula 1,

[0011] The above R1 is hydrogen or an alkyl group,

[0012] The above X1 and X2 are each independently O, N or S,

[0013] The above L1 is a straight or branched chain alkylene.

[0014] According to another concept of the present invention, an all-solid-state battery comprises a positive electrode, a negative electrode, and a solid electrolyte layer between the positive electrode and the negative electrode, wherein the solid electrolyte layer comprises a sulfide-based solid electrolyte and a compound represented by the following chemical formula 1.

[0015] <Chemical Formula 1>

[0016]

[0017] In the above chemical formula 1,

[0018] The above R1 is hydrogen or an alkyl group,

[0019] The above X1 and X2 are each independently O, N or S,

[0020] The above L1 is a straight or branched chain alkylene.

[0021] According to another concept of the present invention, a method for producing a solid electrolyte slurry comprises: mixing a solid electrolyte, a binder, and a solvent to produce a slurry mixture; and performing a mixing process on the slurry mixture to produce a solid electrolyte slurry, wherein the solvent comprises a compound represented by the following chemical formula 1.

[0022] <Chemical Formula 1>

[0023]

[0024] In the above chemical formula 1,

[0025] The above R1 is hydrogen or an alkyl group,

[0026] The above X1 and X2 are each independently O, N or S,

[0027] The above L1 is a straight or branched chain alkylene.

[0028] According to the present invention, by preparing a solid electrolyte slurry using a solvent containing a compound of the Propylene glycol methyl ether acetate (PGMEA) series, the solid electrolyte can be more easily dispersed during solid electrolyte slurry mixing.

[0029] In addition, since the solid electrolyte layer includes a sulfide-based solid electrolyte and a PGMEA series compound, the dispersion characteristics of the solid electrolyte are improved, and thus an all-solid-state battery with improved reliability can be provided.

[0030] FIG. 1 is a plan view of an all-solid-state battery according to embodiments of the present invention.

[0031] Figure 2 is a cross-sectional view taken along line A-A' of Figure 1.

[0032] FIG. 3 is a cross-sectional view taken along line A-A' of FIG. 1 to explain an all-solid-state battery according to another embodiment of the present invention.

[0033] FIG. 4 is a cross-sectional view taken along line A-A' of FIG. 1 to explain an all-solid-state battery according to another embodiment of the present invention.

[0034] Figure 5 is a flowchart showing a method for manufacturing a solid electrolyte slurry according to embodiments of the present invention.

[0035] Figure 6 is a schematic diagram illustrating a method for manufacturing a solid electrolyte slurry according to embodiments of the present invention.

[0036] Figure 7 shows the results of comparing the dispersion of the slurries of Example 1 and Comparative Examples 1 and 2 before and after mixing.

[0037] Figure 8 is a graph measuring temperature changes over time in Example 2 and Comparative Examples 3 and 4.

[0038] To fully understand the structure and effects of the present invention, preferred embodiments of the present invention will be described with reference to the accompanying drawings. However, the present invention is not limited to the embodiments disclosed below, but can be implemented in various forms and subject to various modifications. However, the description of these embodiments is provided solely to ensure a complete disclosure of the present invention and to fully inform those skilled in the art of the invention of the scope of the invention.

[0039] In this specification, when a component is referred to as being on another component, it means that it can be formed directly on the other component, or a third component may be interposed between them. Furthermore, in the drawings, the thicknesses of the components are exaggerated for the sake of clarity. Parts designated by the same reference numerals throughout the specification represent the same components.

[0040] Embodiments described herein will be described with reference to cross-sectional and / or plan views, which are ideal illustrations of the present invention. In the drawings, the thicknesses of films and regions are exaggerated for the purpose of effectively explaining the technical contents. Accordingly, the regions illustrated in the drawings have a schematic nature, and the shapes of the regions illustrated in the drawings are intended to illustrate specific shapes of regions of the device and are not intended to limit the scope of the invention. Although terms such as first, second, and third are used to describe various components in various embodiments of the present specification, these components should not be limited by such terms. These terms are used only to distinguish one component from another. The embodiments described and illustrated herein also include complementary embodiments thereof.

[0041] The terminology used herein is for the purpose of describing embodiments and is not intended to limit the present invention. In this specification, the singular also includes the plural unless specifically stated otherwise. As used herein, the words "comprises" and / or "comprising" do not exclude the presence or addition of one or more other components.

[0042] Unless otherwise defined herein, the particle size may be the average particle size. In addition, the particle size refers to the average particle size (D50), which means the diameter of particles with a cumulative volume of 50% by volume in a particle size distribution. The average particle size (D50) can be measured by a method well known to those skilled in the art, for example, by measuring with a particle size analyzer, or by measuring with a transmission electron microscope (TEM) photograph or a scanning electron microscope (SEM) photograph. Alternatively, the average particle size (D50) value can be obtained by measuring with a measuring device that utilizes dynamic light-scattering, performing data analysis to count the number of particles for each particle size range, and calculating from the counted number. Alternatively, the average particle size (D50) value can be obtained by measuring with a laser diffraction method. When measuring by laser diffraction, more specifically, after the particles to be measured are dispersed in a dispersion medium, they are introduced into a commercially available laser diffraction particle size measuring device (e.g., Microtrac MT 3000) and irradiated with ultrasonic waves of approximately 28 kHz at an output of 60 W, and the average particle size (D50) based on 50% of the particle size distribution in the measuring device can be calculated.

[0043] While embodiments of the present invention have been described with reference to the attached drawings, the present invention may be implemented in other specific forms without altering the technical spirit or essential features thereof. Therefore, the embodiments described above should be understood as illustrative in all respects and not restrictive.

[0044]

[0045] All-solid-state battery

[0046] Fig. 1 is a plan view of an all-solid-state battery according to embodiments of the present invention. Fig. 2 is a cross-sectional view taken along line A-A' of Fig. 1.

[0047] Referring to FIGS. 1 and 2, a unit cell (CEL) of an all-solid-state battery according to the present invention may include a positive electrode layer (100), a negative electrode layer (200) facing the positive electrode layer (100), and a solid electrolyte layer (300) disposed between the positive electrode layer (100) and the negative electrode layer (200). However, the present invention is not limited thereto, and the unit cell (CEL) may further include an additional functional layer, such as an adhesion enhancing layer, disposed between the positive electrode layer (100) and the solid electrolyte layer (300) or between the negative electrode layer (200) and the solid electrolyte layer (300).

[0048] A positive electrode layer (100) according to one embodiment of the present invention may include a positive electrode current collector (110) and a positive electrode active material layer (120) disposed on the positive electrode current collector (110). The positive electrode active material layer (120) may include a positive electrode active material, a solid electrolyte, a conductive material, and a binder.

[0049] The positive electrode current collector (110) can provide a reference surface on which the positive electrode active material layer (120) is arranged. The positive electrode current collector (110) can include a plate or foil including, for example, indium (In), copper (Cu), magnesium (Mg), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), nickel (Ni), zinc (Zn), aluminum (Al), germanium (Ge), lithium (Li), or an alloy thereof.

[0050] Meanwhile, unlike that illustrated in FIG. 1, in one embodiment of the present invention, the positive electrode current collector (110) may be omitted. Although not illustrated, a carbon layer having a thickness of 0.1 μm to 4 μm may be additionally disposed between the positive electrode current collector (110) and the positive electrode active material layer (120) to increase the bonding strength between the positive electrode current collector (110) and the positive electrode active material layer (120).

[0051] The positive electrode active material of the positive electrode active material layer (120) may include a material that can reversibly absorb and desorb lithium ions. The positive electrode active material may include a plurality of particles. The positive electrode active material may include, for example, lithium transition metal oxides such as lithium cobalt oxide (LCO), lithium nickel oxide, lithium nickel cobalt oxide, lithium nickel cobalt aluminum oxide (NCA), lithium nickel cobalt manganese oxide (NCM), lithium manganate, lithium iron phosphate, nickel sulfide, copper sulfide, lithium sulfide, iron oxide, or vanadium oxide, but is not necessarily limited thereto. The positive electrode active materials may be each alone or may be a mixture of two or more types.

[0052] Lithium transition metal oxides include, for example, Li a A 1-b B b D2(0.90≤a≤1, 0≤b≤0.5), Li a E 1-b B b O 2-c D c (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05), LiE 2-b B b O 4-c D c (0≤b≤0.5, 0≤c≤0.05), Li a Ni 1-b-c Co b B cD α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Nor 1-b-c Co b B c O 2-α F α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Nor 1-b-c Mn b B c D α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α≤2), Li a Nor 1-b-c Mn b B c O 2-α F α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Nor b E c G d O2(0.90≤a≤1, 0≤b≤0.9, 0≤c≤0.5, 0.001≤d≤0.1), Li a Nor b Co c Mn d GeO2(0.90≤a≤1, 0≤b≤0.9, 0≤c≤0.5, 0≤d≤0.5, 0.001≤e≤0.1), Li a NiG b O2(0.9≤a≤1, 0.001≤b≤0.1), Li a CoG b O2(0.90≤a≤1, 0.001≤b≤0.1), Li a MnG b O2(0.90≤a≤1, 0.001≤b≤0.1), Li a Mn2GbO4(0.90≤a≤1, 0.001≤b≤0.1), QO2, QS2, LiQS2, V2O5, LiV2O5, LiIO2, LiNiVO4, Li 3-f J2(PO4)3(0≤f≤2), Li 3-fA compound represented by any one of Fe2(PO4)3(0≤f≤2), LiFePO4. In these compounds, the capital letter “A” is Ni, Co, Mn, or a combination thereof, the capital letter “B” is Al, Ni, Co, Mn, Cr, Fe, Mg, Sr, V, a rare earth element, or a combination thereof, the capital letter “D” is O, F, S, P, or a combination thereof, the capital letter “E” is Co, Mn, or a combination thereof, the capital letter “F” is F, S, P, or a combination thereof, the capital letter “G” is Al, Cr, Mn, Fe, Mg, La, Ce, Sr, V, or a combination thereof, the capital letter “Q” is Ti, Mo, Mn, or a combination thereof, the capital letter “I” is Cr, V, Fe, Sc, Y, or a combination thereof, and the capital letter “J” is V, Cr, Mn, Co, Ni, Cu, or a combination thereof.

[0053] The cathode active material may include, for example, a lithium salt of a transition metal oxide having a layered rock salt type structure among the lithium transition metal oxides described above. The "layered rock salt type structure" is, for example, a cubic rock salt type structure. <111> It is a structure in which oxygen atomic layers and metal atomic layers are alternately and regularly arranged in a direction, and thereby each atomic layer forms a two-dimensional plane. The "cubic rock salt structure" refers to the sodium chloride type (NaCl type) structure, which is a type of crystal structure, and specifically refers to a structure in which the face-centered cubic lattice (fcc) formed by each cation and anion is arranged with a displacement of half of the ridge of the unit lattice. Lithium transition metal oxides having this layered rock salt structure include, for example, LiNi x Co y Al z O2(NCA) or LiNi x Co y Mn zO2(NCM) (0 <x<1,0<y<1, 0<z<1, x+y+z=1) 등의 삼원계 리튬전이금속산화물일 수 있다. 양극 활물질이 층상암염형 구조를 갖는 삼원계 리튬전이금속산화물을 포함하는 경우, 단위 셀(CEL)의 에너지 밀도가 커지고 열안정성이 향상될 수 있다.

[0054] The above-described compound included in the positive electrode active material may be covered by a coating layer (not shown). The positive electrode active material may also be a mixture of the above-described compound and a compound to which a coating layer is added. Meanwhile, the coating layer added to the surface of the positive electrode active material may include, for example, an oxide, a hydroxide, an oxyhydroxide, an oxycarbonate, or a hydroxycarbonate of the coating elements below. The compound forming the coating layer is amorphous or crystalline. The coating elements included in the coating layer may include Mg, Al, Co, K, Na, Ca, Si, Ti, V, Sn, Ge, Ga, B, As, Zr, or mixtures thereof. The coating layer may include, for example, Li2O-ZrO2 (LZO). The method for forming the coating layer is selected within a range that does not adversely affect the physical properties of the positive electrode active material. The method for forming the coating layer includes, for example, spray coating, dipping, etc.

[0055] When the cathode active material is a ternary lithium transition metal oxide such as NCA or NCM and contains nickel (Ni), it is possible to increase the capacity density of the unit cell (CEL) and reduce metal dissolution of the cathode active material in a charged state. As a result, the cycle characteristics of the unit cell (CEL) in a charged state are improved. Meanwhile, the "cycle characteristics" are characteristics indicating the degree to which the unit cell (CEL) is deteriorated due to charge / discharge of the unit cell (CEL). A unit cell (CEL) with high cycle characteristics may have a small degree of deterioration of the unit cell (CEL) due to charge / discharge, and a unit cell (CEL) with low cycle characteristics may have a large degree of deterioration of the unit cell (CEL) due to charge / discharge.

[0056] The positive electrode active material may have a particle shape such as a sphere or an ellipsoid, for example. The particle size and content of the positive electrode active material are not particularly limited.

[0057] The solid electrolyte of the positive electrode active material layer (120) may have a particle shape. The solid electrolyte may be dispersed between the positive electrode active materials. The solid electrolyte may include a sulfide-based solid electrolyte having excellent lithium ion conductivity characteristics. Examples of the sulfide-based solid electrolyte include Li2S-P2S5, Li2S-P2S5-LiX (X is a halogen element), Li2S-P2S5-Li2O, Li2S-P2S5-Li2O-LiI, Li2S-SiS2, Li2S-SiS2-LiI, Li2S-SiS2-LiBr, Li2S-SiS2-LiCl, Li2S-SiS2-B2S3-LiI, Li2S-SiS2-P2S5-LiI, Li2S-B2S3, Li2S-P2S5-Z m S n (m, n are positive numbers, capital letter “Z” represents Ge, Zn or Ga), Li2S-GeS2, Li2S-SiS2-Li3PO4, Li2S-SiS2-Li p MO q (p, q are positive numbers, capital letter “M” is one of P, Si, Ge, B, Al, Ga In), Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x It may include at least one selected from (0≤x≤2).

[0058] Sulfide-based solid electrolytes include, for example, Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS6-x I x It may be an argyrodite-type compound including at least one selected from (0≤x≤2). In particular, the sulfide-based solid electrolyte may be an argyrodite-type compound including at least one selected from Li6PS5Cl, Li6PS5Br, and Li6PS5I.

[0059] Alternatively, the sulfide-based solid electrolyte is Li 7-a M a PS 6-c X c It may be an argyrodite-type compound containing (0≤a≤2, (0≤c≤2)), where X may be F, Br, Cl, or a combination thereof. M is candium (Sc), yttrium (Y), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), technetium (Tc), rhenium (Re), iron (Fe), ruthenium (Ru), osmium (Os), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), platinum (Pt), copper (Cu), silver (Ag), gold (Au), zinc (Zn), cadmium (Cd), mercury (Hg), aluminum (Al), gallium (Ga), indium (In), thallium (Tl), silicon (Si), germanium (Ge), tin (Sn), lead (Pb), arsenic (As), antimony (Sb), bismuth (Bi), or a combination thereof. Can be.

[0060] The density of the argyrodite-type solid electrolyte may be 1.5 g / cc to 2.0 g / cc. Since the argyrodite-type solid electrolyte has a density of 1.5 g / cc or more, the internal resistance of the all-solid-state battery is reduced, and the defect of the solid electrolyte membrane being penetrated and short-circuited due to the formation of lithium dendrites can be prevented. The elastic modulus of the solid electrolyte may be, for example, 15 GPa to 35 GPa.

[0061] The solid electrolyte in the positive electrode active material layer (120) may have a smaller average particle diameter than the first and second solid electrolytes in the solid electrolyte layer (300) described later. For example, the average particle diameter of the solid electrolyte in the positive electrode active material layer (120) may be 90% or less, 80% or less, 70% or less, 60% or less, 50% or less, 40% or less, 30% or less, or 20% or less of the average particle diameter of the solid electrolyte in the solid electrolyte layer (300). Meanwhile, the average particle diameter may be a median diameter measured using a laser particle size distribution meter.

[0062] The positive electrode active material layer (120) may include a conductive material. The conductive material may be conductive without causing chemical changes in the unit cell (CEL), thereby increasing the conductivity of the positive electrode active material and the solid electrolyte. The conductive material may include a carbon-based material. For example, the conductive material may include one or more selected from graphite, carbon black, acetylene black, carbon nanofibers, and carbon nanotubes.

[0063] The positive electrode active material layer (120) may further include a binder. The binder may bind the positive electrode active material, the solid electrolyte, and the conductive material within the positive electrode active material layer (120) to each other. The binder may include a material for improving the bonding strength between the positive electrode active material layer (120) and the positive electrode current collector (110). The binder may include, for example, polyvinylidene fluoride, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, vinylidene fluoride / hexafluoropropylene copolymer, polyacrylonitrile, and polymethyl methacrylate.

[0064] Based on 100 parts by weight of the total of the positive electrode active material, the solid electrolyte, the conductive material, and the binder, the positive electrode active material layer (120) may include 85 parts by weight or more and 92 parts by weight or less of the positive electrode active material. Based on 100 parts by weight of the total of the positive electrode active material, the solid electrolyte, the conductive material, and the binder, the positive electrode active material layer (120) may include 0.5 parts by weight or more and 1.5 parts by weight or less of the binder.

[0065] Based on 100 parts by weight of the solid electrolyte, the positive electrode active material layer (120) may include 1 part by weight or more and 50 parts by weight or less of a conductive material. If the conductive material is included in the positive electrode active material layer (120) in an amount of less than 1 part by weight based on 100 parts by weight of the solid electrolyte, the proportion of the conductive material may decrease, thereby lowering the electrical conductivity of the positive electrode active material layer (120). If the conductive material is included in the positive electrode active material layer (120) in an amount of more than 50 parts by weight based on 100 parts by weight of the solid electrolyte, the proportion of the conductive material may be excessively high, so that a covering layer covering the surface of the solid electrolyte may not be properly formed.

[0066] The positive electrode active material layer (120) may further include additives such as fillers, coating agents, dispersants, and ion conductive aids in addition to the above-described positive electrode active material, solid electrolyte, conductive agent, and binder.

[0067] The negative electrode layer (200) may include a negative electrode current collector (210) and a negative electrode coating layer (220) on the negative electrode current collector (210). The negative electrode current collector (210) may provide a reference surface on which the negative electrode coating layer (220) is disposed. The negative electrode current collector (210) may include, for example, a material that does not react with lithium, i.e., does not form an alloy or a compound with lithium. For example, the negative electrode current collector (210) may include at least one metal selected from the group consisting of copper (Cu), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), and nickel (Ni). The thickness of the negative electrode current collector (210) may be 1 μm to 20 μm, more specifically 5 μm to 15 μm, and more specifically 7 μm to 10 μm.

[0068] The negative electrode current collector (210) may be composed of one of the above-described metals, or may include an alloy or coating material of two or more metals. The negative electrode current collector (210) may have, for example, a plate shape or a foil shape. Meanwhile, in one embodiment, the negative electrode current collector (210) may be omitted.

[0069] The cathode coating layer (220) can allow lithium metal to grow between the cathode current collector (210) and the unit cell (CEL) when charging. The cathode coating layer (220) can act as a protective layer for the lithium metal and suppress the precipitation and growth of lithium dendrites.

[0070] The cathode coating layer (220) may include a metal and carbon. For example, the cathode coating layer (220) may include at least one metal selected from the group consisting of gold (Au), platinum (Pt), palladium (Pd), silicon (Si), silver (Ag), aluminum (Al), bismuth (Bi), tin (Sn), and zinc (Zn). The cathode coating layer (220) may include at least one carbon selected from the group consisting of carbon black, acetylene black, furnace black, ketjen black, and graphene. In one embodiment, the cathode coating layer (220) may include a mixture of carbon black and silver (Ag).

[0071] The cathode coating layer (220) may further include additives other than metal and carbon. The cathode coating layer (220) may further include, for example, at least one additive selected from the group consisting of a binder, a filler, a coating agent, a dispersant, and an ion conductive additive.

[0072] The negative electrode coating layer (220) may have a smaller thickness than the positive electrode active material layer (120). The thickness of the negative electrode coating layer (220) may be, for example, 50% or less, 40% or less, 30% or less, 20% or less, 10% or less, or 5% or less of the thickness of the positive electrode active material layer (120). The thickness of the negative electrode coating layer (220) may be, for example, 1 um to 20 um, 2 um to 10 um, or 3 um to 7 um. If the thickness of the negative electrode coating layer (220) is too thin, lithium dendrites formed between the negative electrode coating layer (220) and the negative electrode current collector (210) may collapse the negative electrode coating layer (220), thereby deteriorating the cycle characteristics of the unit cell (CEL). If the thickness of the cathode coating layer (220) increases excessively, the energy density of the unit cell (CEL) may decrease and the internal resistance of the unit cell (CEL) due to the cathode coating layer (220) may increase, thereby deteriorating the cycle characteristics of the cell.

[0073] Meanwhile, although not shown, a carbon layer may be further included to improve adhesion between the cathode coating layer (220) and the solid electrolyte layer (300).

[0074] A solid electrolyte layer (300) may be provided between the positive electrode layer (100) and the negative electrode layer (200). The solid electrolyte layer (300) may include a sulfide-based solid electrolyte having excellent lithium ion conductivity characteristics. The solid electrolyte in the solid electrolyte layer (300) may be the same as or different from any one of the materials included in the solid electrolyte in the positive electrode active material layer (120) described above.

[0075] The solid electrolyte layer (300) may include a compound represented by the following chemical formula 1.

[0076] <Chemical Formula 1>

[0077]

[0078] In the above chemical formula 1, R1 is hydrogen or a C1 to C3 alkyl group, X1 and X2 are each independently O, N or S, and L1 may be a straight or branched C1 to C5 alkylene. The compound represented by the above chemical formula 1 may be Propylene glycol methyl ether acetate (PGMEA).

[0079] The solid electrolyte layer (300) may include a first solid electrolyte layer (310) and a second solid electrolyte layer (320). The first solid electrolyte layer (310) may be adjacent to the positive electrode layer (100), and the second solid electrolyte layer (320) may be adjacent to the negative electrode layer (200).

[0080] Referring to FIG. 2, the first solid electrolyte layer (310) may include a first solid electrolyte. The first solid electrolyte may have a particle shape such as a sphere or an ellipsoid. The first solid electrolyte may include a sulfide-based solid electrolyte. The first solid electrolyte may be amorphous, crystalline, or a mixture thereof. In addition, the solid electrolyte may include, for example, at least sulfur (S), phosphorus (P), and lithium (Li) as constituent elements among the above-described sulfide-based solid electrolyte materials. For example, the solid electrolyte may be a material including Li2S-P2S5. When using a sulfide-based solid electrolyte material including Li2S-P2S5 to form the solid electrolyte, the mixing molar ratio of Li2S and P2S5 is, for example, in the range of Li2S:P2S5=50:50 to 90:10.

[0081] In one embodiment, the first solid electrolyte is Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x The first solid electrolyte may include an argyrodite-type compound including at least one selected from (0≤x≤2). The first solid electrolyte may include an argyrodite-type compound including at least one selected from Li6PS5Cl, Li6PS5Br, and Li6PS5I.

[0082] In another embodiment, the first solid electrolyte is Li 7-a M a PS 6-c X cArgyrodite-type compounds may include, wherein X may be Cl, Br, or a combination thereof. M may be Na, K, Fe, Mg, Ca, Ag, Cu, Zr, Zn, or a combination thereof. Each of a and c may be a real number between 0 and 2.

[0083] The density of the argyrodite-type solid electrolyte may be 1.5 g / cc to 2.0 g / cc. When the argyrodite-type solid electrolyte has a density of 1.5 g / cc or more, the internal resistance of the all-solid-state battery is reduced, and the defect of the solid electrolyte membrane being penetrated and short-circuited due to the formation of lithium dendrites can be prevented. The elastic modulus of the first solid electrolyte is, for example, 15 GPa to 35 GPa.

[0084] The first solid electrolyte layer (310) may further include a binder. The binder included in the solid electrolyte layer (300) may be, for example, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, etc., but is not limited thereto. The binder of the first solid electrolyte layer (310) may be the same as or different from the binder included in the positive electrode active material layer (120) or the binder included in the negative electrode coating layer (220).

[0085] The second solid electrolyte layer (320) may include a second solid electrolyte. The second solid electrolyte may have a particle shape such as a sphere or ellipsoid.

[0086] The second solid electrolyte may include a sulfide-based solid electrolyte. The description of the second solid electrolyte may be the same as or similar to that described above for the first solid electrolyte. In one embodiment, the second solid electrolyte may have substantially the same composition as the first solid electrolyte. In another embodiment, the second solid electrolyte may have a similar composition to the first solid electrolyte.

[0087] The second solid electrolyte can be in direct contact with the negative electrode coating layer (220). As a result, the second solid electrolyte can suppress lithium dendrites formed between the negative electrode coating layer (220) and the negative electrode current collector (210). The second solid electrolyte can effectively suppress negative electrode side reactions. As a result, the cell performance of the all-solid-state battery according to the present invention can be improved.

[0088] The first solid electrolyte layer (310) may have a first thickness (TK1), and the second solid electrolyte layer (320) may have a second thickness (TK2). The first thickness (TK1) and the second thickness (TK2) may be the same or different. In one embodiment, the first thickness (TK1) may be greater than the second thickness (TK2). For example, the first thickness (TK1) may be 1.1 to 5 times the second thickness (TK2).

[0089] Referring back to FIGS. 1 and 2, the positive electrode layer (100) and the first solid electrolyte layer (310) may form a positive electrode composite layer (CSH). The negative electrode layer (200) and the second solid electrolyte layer (320) may form a negative electrode composite layer (ASH). The positive electrode composite layer (CSH) may be laminated on the negative electrode composite layer (ASH).

[0090] The area of ​​the cathode composite layer (ASH) and the area of ​​the cathode composite layer (CSH) may be different. Specifically, the area of ​​the cathode composite layer (ASH) may be larger than that of the cathode composite layer (CSH). The cathode composite layer (CSH) may be completely overlapped within the cathode composite layer (ASH).

[0091] In one embodiment of the present invention, the first solid electrolyte layer (310) may have substantially the same area as the positive electrode layer (100). The second solid electrolyte layer (320) may have substantially the same area as the negative electrode layer (200).

[0092] Specifically, the positive electrode composite layer (CSH) may have a first width (WI1) in a first direction (D1). The negative electrode composite layer (ASH) may have a second width (WI2) in the first direction (D1). The first width (WI1) may be smaller than the second width (WI2). The positive electrode composite layer (CSH) may have a third width (WI3) in the second direction (D2). The negative electrode composite layer (ASH) may have a fourth width (WI4) in the second direction (D2). The third width (WI3) may be smaller than the fourth width (WI4).

[0093] A unit cell (CEL) according to the present embodiment can be manufactured by forming a cathode composite layer (ASH) on a first carrier film, forming a cathode composite layer (CSH) on a second carrier film, and then laminating the cathode composite layer (ASH) and the cathode composite layer (CSH).

[0094] In the embodiments described below, detailed descriptions of technical features that overlap with those described previously with reference to FIGS. 1 and 2 will be omitted, and differences will be described in detail.

[0095] FIG. 3 is a cross-sectional view taken along line A-A' of FIG. 1 to explain an all-solid-state battery according to another embodiment of the present invention. Referring to FIG. 3, a unit cell (CEL) according to the present invention may further include a gasket (GSK). The gasket (GSK) may be provided to surround a cathode composite layer (CSH). The gasket (GSK) may fill a step in the side surface of the unit cell (CEL) caused by a difference in area between the cathode composite layer (ASH) and the cathode composite layer (CSH). The gasket (GSK) may surround four side surfaces of the cathode composite layer (CSH). For example, the thickness of the gasket (GSK) may be substantially the same as the thickness of the cathode composite layer (CSH).

[0096] The upper surface of the second solid electrolyte layer (320) may include a first region in contact with the first solid electrolyte layer (310) and a second region in contact with the gasket (GSK). The second region may be a peripheral region of the upper surface of the second solid electrolyte layer (320). The second region may surround the first region.

[0097] FIG. 4 is a cross-sectional view taken along line A-A' of FIG. 1 to explain an all-solid-state battery according to another embodiment of the present invention. Referring to FIG. 4, the negative electrode layer (200) of the unit cell (CEL) may further include a lithium metal layer (400) between the negative electrode current collector (210) and the negative electrode coating layer (220). The thickness of the lithium metal layer (400) may further increase when the unit cell (CEL) is charged. The negative electrode coating layer (220) serves as a protective layer for the lithium metal layer (400), and at the same time, may suppress the growth of lithium dendrites from the lithium metal layer (400).

[0098] The lithium metal layer (400) may be a metal thin film containing lithium or a lithium alloy. The lithium alloy may include, but is not limited to, a Li-Al alloy, a Li-Sn alloy, a Li-In alloy, a Li-Ag alloy, a Li-Au alloy, a Li-Zn alloy, a Li-Ge alloy, a Li-Si alloy, etc., and any lithium alloy may be used. The lithium metal layer (400) may contain one of these alloys or lithium. Alternatively, the lithium metal layer (400) may contain various types of alloys.

[0099] The lithium metal layer (400) may have a fifth width (WI5) in the first direction (D1). The fifth width (WI5) may be equal to or greater than the first width (WI1). The fifth width (WI5) may be equal to or less than the second width (WI2). For example, the fifth width (WI5) may be greater than the first width (WI1) and less than the second width (WI2).

[0100]

[0101] solid electrolyte slurry

[0102] The solid electrolyte slurry according to embodiments of the present invention may include a compound represented by the following chemical formula 1.

[0103] <Chemical Formula 1>

[0104]

[0105] In the above chemical formula 1, R1 is hydrogen or a C1 to C3 alkyl group, X1 and X2 are each independently O, N or S, and L1 may be a straight or branched C1 to C5 alkylene. The compound represented by the above chemical formula 1 may be Propylene glycol methyl ether acetate (PGMEA). The concentration of the compound represented by the above chemical formula 1 may be 10 wt% to 50 wt% relative to the total weight of the solid electrolyte slurry.

[0106]

[0107] Method for preparing solid electrolyte slurry

[0108] Referring to FIGS. 5 and 6, a method for manufacturing a solid electrolyte slurry according to embodiments of the present invention may include mixing a solid electrolyte, a binder, and a solvent to manufacture a slurry mixture (20) (S10), performing a mixing process on the slurry mixture (20) with a mixing device (10) to manufacture a solid electrolyte slurry (SL) (S20), and performing a defoaming process on the solid electrolyte slurry (SL) for which the mixing process has been completed (S30).

[0109] A slurry mixture (20) can be prepared by introducing a solid electrolyte, a binder, and a solvent into a container and mixing them (S10). The solid electrolyte may be a powder-type solid electrolyte. According to one embodiment, the solid electrolyte may include a sulfide-based solid electrolyte with excellent lithium ion conductivity characteristics.

[0110] A sulfide-based solid electrolyte can be manufactured by treating starting materials such as Li2S and P2S5 by a melting rapid cooling method or a mechanical milling method, for example. In addition, a heat treatment can be performed after the treatment. The solid electrolyte can be amorphous, crystalline, or a mixture thereof. In addition, the solid electrolyte can be, for example, a material containing sulfur (S), phosphorus (P), and lithium (Li) as constituent elements among the above-described sulfide-based solid electrolyte materials. For example, the solid electrolyte can be a material containing Li2S-P2S5. When using a material containing Li2S-P2S5 as a sulfide-based solid electrolyte material forming a solid electrolyte, the mixing molar ratio of Li2S and P2S5 is, for example, in the range of Li2S:P2S5=50:50 to 90:10.

[0111] Sulfide-based solid electrolytes include, for example, Li2S-P2S5, Li2S-P2S5-LiX (X is a halogen element), Li2S-P2S5-Li2O, Li2S-P2S5-Li2O-LiI, Li2S-SiS2, Li2S-SiS2-LiI, Li2S-SiS2-LiBr, Li2S-SiS2-LiCl, Li2S-SiS2-B2S3-LiI, Li2S-SiS2-P2S5-LiI, Li2S-B2S3, Li2S-P2S5-Z m S n (m, n are positive numbers, capital letter “Z” represents Ge, Zn or Ga), Li2S-GeS2, Li2S-SiS2-Li3PO4, Li2S-SiS2-Li p MO q (p, q are positive numbers, capital letter “M” is one of P, Si, Ge, B, Al, Ga In), Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x Ix It may include at least one selected from (0≤x≤2).

[0112] Sulfide-based solid electrolytes include, for example, Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x It may be an argyrodite-type compound including at least one selected from (0≤x≤2). In particular, the sulfide-based solid electrolyte may be an argyrodite-type compound including at least one selected from Li6PS5Cl, Li6PS5Br, and Li6PS5I.

[0113] Sulfide-based solid electrolytes include, for example, Li 7-a M a PS 6-c X c It may include an argyrodite-type compound represented by (0≤a≤2, 0≤c≤2). The X may be F, Br, Cl, or a combination thereof. The above M is candium (Sc), yttrium (Y), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), technetium (Tc), rhenium (Re), iron (Fe), ruthenium (Ru), osmium (Os), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), platinum (Pt), copper (Cu), silver (Ag), gold (Au), zinc (Zn), cadmium (Cd), mercury (Hg), aluminum (Al), gallium (Ga), indium (In), thallium (Tl), silicon (Si), germanium (Ge), tin (Sn), lead (Pb), arsenic (As), antimony (Sb), bismuth (Bi) or these. It could be a combination.

[0114] The binder may include, for example, at least one selected from the group consisting of a cellulose polymer, a rubber binder, an acrylate binder, an imide binder, a polyvinylidene fluoride binder, a polyvinylpyrrolidone binder, a nitrile binder, an acetate binder, and a cyano binder.

[0115] The cellulose-based polymer may include at least one selected from the group consisting of, for example, carboxymethyl cellulose (CMC), methyl cellulose (MC), hydroxypropyl cellulose (HPC), methyl hydroxypropyl cellulose (MHPC), ethyl hydroxyethyl cellulose (EHEC), methyl ethyl hydroxyethyl cellulose (MEHEC), and cellulose gum.

[0116] The above acrylate compound may be, for example, polyacrylic acid (PAA), polymethylmethacrylate, polyisobutylmethacrylate, polyethylacrylate, polybutyl acrylate, or polyethylhexyl acrylate (poly(2-ethylhexyl acrylate)).

[0117] The above imide compound may be, for example, polyimide or polyamide imide.

[0118] The polyvinylidene fluoride compound may be, for example, polyvinylidene fluoride-co-hexafluoropropylene, polyvinylidene fluoride-co-trichloroethylene, polyvinylidene fluoride-co-tetrafluoroethylene, polyvinylidene fluoride-co-trifluoroethylene, polyvinylidene fluoride-co-trifluorochloroethylene, polyvinylidene fluoride-co-hexafluoropropylene (PVdF) or polyvinylidene fluoride-co-trichloroethylene.

[0119] The above polyvinylpyrrolidone compound may be, for example, polyvinylpyrrolidone.

[0120] The nitrile compound may be, for example, polyacrylonitrile or an acrylonitrile-styrene-butadiene copolymer.

[0121] The acetate compound may be, for example, polyvinylacetate, polyethylene-co-vinyl acetate, cellulose acetate, cellulose acetate butyrate, or cellulose acetate propionate.

[0122] The above cyano compound may be, for example, cyanoethyl sucrose.

[0123] In one embodiment of the present invention, the binder may include at least one of carboxymethyl cellulose (CMC), styrene butadiene rubber (SBR), and nitrile butadiene rubber (NBR).

[0124] The binder may be added, for example, so that the binder content in the slurry mixture (20) is 1 wt% to 10 wt%. If the binder content is less than the above range, the binder dispersion effect may be reduced in the kneading process described below. If the binder content exceeds the above range, the slurry phase stability may be reduced due to binder agglomeration.

[0125] For example, the solvent may include at least one selected from the group consisting of water, methanol, ethanol, ethylene glycol, diethylene glycol, glycerol, isobutyryl isobutyrate, xylene, toluene, benzene, and hexane. The solvent may include an aqueous solvent. The type of the aqueous solvent may not be limited. In one embodiment, the solvent may be water.

[0126] According to an embodiment of the present invention, the solvent may include a compound represented by the following chemical formula 1.

[0127] <Chemical Formula 1>

[0128]

[0129] In the above chemical formula 1, R1 is hydrogen or a C1 to C3 alkyl group, X1 and X2 are each independently O, N or S, and L1 may be a straight or branched C1 to C5 alkylene. The compound represented by the above chemical formula 1 may be Propylene glycol methyl ether acetate (PGMEA).

[0130] The solids content of the slurry mixture (20) can be controlled through the above solvent. The solids content of the slurry mixture according to the present embodiment can be controlled to, for example, 40 wt% to 60 wt%.

[0131] A mixing process can be performed on a slurry mixture (20) using a mixing facility (10) (S20). The mixing process can be performed using a mixer or a kneader. In one embodiment of the present invention, the mixing process can be performed using a mixing facility (10) including at least one selected from the group consisting of a PD mixer (Planetary Disperser mixer), a planetary mixer, a paddle mixer, a ribbon mixer, a dual shaft mixer mixer, a high-speed impeller mixer, or a propeller mixer.

[0132] The mixing process may further include a kneading process. The kneading process may be performed multiple times (e.g., twice) and sequentially within a single mixer. The solids content of the slurry mixture (20) can be controlled through the kneading process, thereby producing a solid electrolyte slurry (SL) having a desired viscosity.

[0133] A defoaming process can be performed on the solid electrolyte slurry (SL) for which the mixing process has been completed (S30). Through the defoaming process, air bubbles remaining within the solid electrolyte slurry (SL) can be removed. The solid electrolyte slurry (SL) for which the defoaming process has been completed can be recovered from the mixing equipment (10). The recovered solid electrolyte slurry (SL) can be used in a coating process for forming a solid electrolyte layer.

[0134] In the solid electrolyte slurry (SL) according to an embodiment of the present invention, the solvent has very low reactivity with the sulfide-based solid electrolyte and thus does not deteriorate it, can disperse the sulfide-based solid electrolyte well, and can also not increase cell resistance. Therefore, the stability and reliability of the solid electrolyte layer and all-solid-state battery manufactured using such a solvent can be improved.

[0135]

[0136] Hereinafter, embodiments of the present invention will be described in more detail. However, the following embodiments are provided merely to aid understanding of the present invention, and the scope of the present invention is not limited thereby.

[0137]

[0138] Example 1

[0139] A slurry mixture was prepared by placing a sulfide-based solid electrolyte, acrylate rubber, and propylene glycol methyl ether acetate (PGMEA) solvent into a container. The solid content of the mixture was adjusted to 70 wt%. The composition of the slurry mixture was such that the sulfide-based solid electrolyte: acrylate rubber had a weight ratio of 98:2.

[0140] The above slurry mixture was placed in a PD (Planetary Despa) mixer and kneaded. Kneading was performed for 50 minutes with the planetary mixer at 75 rpm.

[0141] The slurry after the kneading process was defoamed for 30 minutes.

[0142] 10 ml of the prepared solid electrolyte slurry was placed in a 20 ml vial.

[0143]

[0144] Comparative Example 1

[0145] A vial was prepared in the same manner as in Example 1 described above, except that Octyl Acetate (OA) was used instead of PGMEA.

[0146]

[0147] Comparative Example 2

[0148] A vial was prepared in the same manner as in Example 1 described above, except that 1,2-Dichloroethane (DCE) was used instead of PGMEA.

[0149]

[0150] Comparative Example 3

[0151] A vial was prepared in the same manner as in Example 1 described above, except that Ethyl Alcohol (EtOH) was used instead of PGMEA.

[0152]

[0153] Experimental Example 1: Comparison of dispersion before and after mixing slurry.

[0154] The dispersion of the slurry in each solvent was confirmed according to Example 1, Comparative Example 1, and Comparative Example 2. Specifically, the vials of Example 1, Comparative Example 1, and Comparative Example 2 were shaken to thoroughly mix the contents. The experiment was conducted at room temperature. Next, the slurry dispersed in the solvent was confirmed. The results are shown in Figure 7.

[0155] Referring to Fig. 7, in Example 1, most of the slurry remaining in the container after mixing was dispersed in the solvent. In contrast, in Comparative Examples 1 and 2, the slurry remained undispersed in the container. In particular, in Comparative Example 2, the slurry was hardly dispersed. It can be confirmed that the solvent (PGMEA) of Example 1 effectively disperses the slurry compared to the solvents of Comparative Examples 1 and 2.

[0156] Meanwhile, even after leaving the vials of Example 1, Comparative Example 1, and Comparative Example 2 for 30 minutes without shaking or mixing the contents, similar results to Experimental Example 1 were observed.

[0157]

[0158] Experimental Example 2: Measurement of hydrogen sulfide gas generation and exothermic temperature

[0159] The amount of hydrogen sulfide (H2S) gas generated and the temperature were measured during solid electrolyte slurry mixing for each solvent according to Example 1, Comparative Example 1, and Comparative Example 3. Specifically, the vials of Example 1, Comparative Example 1, and Comparative Example 3 were left as is without shaking or mixing the contents. The leaving was performed at room temperature. The results are shown in Fig. 8. Gas measurement was performed using a Honeywell minimax X4 4-Gas (measurement range: 0 to 250 ppm). Temperature measurement was performed using a FLIR TG165 Spot thermal camera (measurement range: -25°C to 380°C).

[0160] Referring to Fig. 8, in Example 1, Comparative Example 1, and Comparative Example 3, the solid electrolyte was dispersed in the solvent. When the gas generated was measured, the amount of hydrogen sulfide (H2S) generated was not measured in Example 1. In Comparative Example 1, hydrogen sulfide (H2S) was generated in an amount of more than 10 ppm, causing the alarm of the measuring device to sound. In Comparative Example 3, hydrogen sulfide (H2S) was generated in an amount of more than 10 ppm, causing the alarm of the measuring device to sound. Through this, it can be seen that Example 1 generated less hydrogen sulfide (H2S) gas than Comparative Examples 1 and 3. In other words, it can be seen that the solvent (PGMEA) of Example 1 has less reactivity with the sulfide-based solid electrolyte than the solvents of Comparative Examples 1 and 3, and thus the mixing process can be performed in a more stable state.

[0161] After the solid electrolyte was dispersed in the solvent, the temperature of Example 1 was measured to be 20°C, the same as room temperature. This confirms that almost no heat generation occurs while the solid electrolyte is dispersed in the solvent.

[0162] The temperature of Comparative Example 3 was measured to be 32°C. This shows that the solvent of Example 1 generates little heat during the dispersion of the solid electrolyte compared to the solvent of Comparative Example 3. In other words, the solvent of Example 1 (PGMEA) has a lower exothermic temperature than the solvent of Comparative Example 3 due to its lower reactivity with the sulfide-based solid electrolyte, allowing the mixing process to be performed in a more stable state.

[0163]

[0164] While embodiments of the present invention have been described with reference to the attached drawings, the present invention may be implemented in other specific forms without altering the technical spirit or essential features thereof. Therefore, the embodiments described above should be understood as illustrative in all respects and not restrictive.

Claims

1. A solid electrolyte slurry comprising a compound represented by the following chemical formula 1: <Chemical Formula 1> In the above chemical formula 1, The above R1 is hydrogen or an alkyl group, The above X1 and X2 are each independently O, N or S, The above L1 is a straight or branched chain alkylene.

2. In paragraph 1, A solid electrolyte slurry wherein R1 is hydrogen or an alkyl group of C1 to C3.

3. In paragraph 1, A solid electrolyte slurry wherein the above L1 is a straight or branched C1 to C5 alkylene.

4. In paragraph 1, A solid electrolyte slurry further comprising a sulfide-based solid electrolyte.

5. In paragraph 4, The above sulfide-based solid electrolyte is Li2S-P2S5, Li2S-P2S5-LiX (X is a halogen element), Li2S-P2S5-Li2O, Li2S-P2S5-Li2O-LiI, Li2S-SiS2, Li2S-SiS2-LiI, Li2S-SiS2-LiBr, Li2S-SiS2-LiCl, Li2S-SiS2-B2S3-LiI, Li2S-SiS2-P2S5-LiI, Li2S-B2S3, Li2S-P2S5-Z m S n (m, n are positive numbers, capital letter “Z” is Ge, Zn or Ga), Li2S-GeS2, Li2S-SiS2-Li3PO4, Li2S-SiS2-Li p MO q (p, q are positive numbers, capital letter “M” is one of P, Si, Ge, B, Al, Ga or In), Li7-xPS 6-x Cl x (0≤x≤2), Li7-xPS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x A solid electrolyte slurry comprising at least one selected from (0≤x≤2).

6. In paragraph 4, The above sulfide-based solid electrolyte is Li 7-a M a PS 6-c X c Contains an argyrodite-type compound represented by (0≤a≤2, 0≤c≤2), wherein X is F, Br, Cl or a combination thereof, The above M is candium (Sc), yttrium (Y), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), technetium (Tc), rhenium (Re), iron (Fe), ruthenium (Ru), osmium (Os), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), platinum (Pt), copper (Cu), silver (Ag), gold (Au), zinc (Zn), cadmium (Cd), mercury (Hg), aluminum (Al), gallium (Ga), indium (In), thallium (Tl), silicon (Si), germanium (Ge), tin (Sn), lead (Pb), arsenic (As), antimony (Sb), bismuth (Bi) or these. A combination of solid electrolyte slurry.

7. In paragraph 1, The compound represented by the above chemical formula 1 is a solid electrolyte slurry of Propylene glycol methyl ether acetate (PGMEA).

8. In paragraph 4, The compound represented by the above chemical formula 1 is a solid electrolyte slurry that functions as a solvent for dispersing the above sulfide-based solid electrolyte.

9. In paragraph 1, A solid electrolyte slurry in which the concentration of the compound represented by the above chemical formula 1 is 10 wt% to 50 wt% based on the total weight of the solid electrolyte slurry.

10. In paragraph 1, Including more binders, A solid electrolyte slurry, wherein the binder comprises at least one selected from the group consisting of a cellulose polymer, a rubber binder, an acrylate binder, an imide binder, a polyvinylidene fluoride binder, a polyvinylpyrrolidone binder, a nitrile binder, an acetate binder, and a cyano binder.

11. Including a positive electrode, a negative electrode, and a solid electrolyte layer between the positive electrode and the negative electrode, The solid electrolyte layer is an all-solid-state battery comprising a sulfide-based solid electrolyte and a compound represented by the following chemical formula 1: <Chemical Formula 1> In the above chemical formula 1, The above R1 is hydrogen or an alkyl group, The above X1 and X2 are each independently O, N or S, The above L1 is a straight or branched chain alkylene.

12. In paragraph 11, The above R1 is hydrogen or an alkyl group of C1 to C3, An all-solid-state battery, wherein the above L1 is a straight-chain or branched-chain C1 to C5 alkylene.

13. In paragraph 11, The above negative electrode layer includes a negative electrode current collector and a negative electrode coating layer on the negative electrode current collector, An all-solid-state battery wherein the cathode coating layer comprises a carbon-based material and a metal.

14. In paragraph 11, An all-solid-state battery, wherein the negative electrode layer further comprises a lithium metal layer between the negative electrode current collector and the negative electrode coating layer.

15. Preparing a slurry mixture by mixing a solid electrolyte, a binder, and a solvent; and A method for producing a solid electrolyte slurry, comprising: performing a mixing process on the above slurry mixture; A method for producing a solid electrolyte slurry, wherein the solvent comprises a compound represented by the following chemical formula 1: <Chemical Formula 1> In the above chemical formula 1, The above R1 is hydrogen or an alkyl group, The above X1 and X2 are each independently O, N or S, The above L1 is a straight or branched chain alkylene.

16. In paragraph 15, The above R1 is hydrogen or an alkyl group of C1 to C3, A method for producing a solid electrolyte slurry, wherein the above L1 is a straight or branched C1 to C5 alkylene.

17. In paragraph 15, A method for producing a solid electrolyte slurry, wherein the solid electrolyte comprises a sulfide-based solid electrolyte.

18. In paragraph 17, The above sulfide-based solid electrolyte is Li 7-a M a PS 6-c X c Contains an argyrodite-type compound represented by (0≤a≤2, 0≤c≤2), wherein X is F, Br, Cl or a combination thereof, The above M is candium (Sc), yttrium (Y), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), technetium (Tc), rhenium (Re), iron (Fe), ruthenium (Ru), osmium (Os), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), platinum (Pt), copper (Cu), silver (Ag), gold (Au), zinc (Zn), cadmium (Cd), mercury (Hg), aluminum (Al), gallium (Ga), indium (In), thallium (Tl), silicon (Si), germanium (Ge), tin (Sn), lead (Pb), arsenic (As), antimony (Sb), bismuth (Bi) or these. A method for producing a combination solid electrolyte slurry.

19. In paragraph 15, A method for producing a solid electrolyte slurry, wherein the above mixing process further includes performing a kneading process on the slurry mixture.

20. In paragraph 15, A method for producing a solid electrolyte slurry, further comprising performing a defoaming process on the solid electrolyte slurry after completing the mixing process.

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