CN116529925A - Electrode assembly for secondary battery and secondary battery including the same - Google Patents
Electrode assembly for secondary battery and secondary battery including the same Download PDFInfo
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- CN116529925A CN116529925A CN202280007079.3A CN202280007079A CN116529925A CN 116529925 A CN116529925 A CN 116529925A CN 202280007079 A CN202280007079 A CN 202280007079A CN 116529925 A CN116529925 A CN 116529925A
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- electrode assembly
- electrode
- solid electrolyte
- secondary battery
- positive electrode
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- NJLLQSBAHIKGKF-UHFFFAOYSA-N dipotassium dioxido(oxo)titanium Chemical compound [K+].[K+].[O-][Ti]([O-])=O NJLLQSBAHIKGKF-UHFFFAOYSA-N 0.000 description 1
- 239000011883 electrode binding agent Substances 0.000 description 1
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- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 description 1
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- KHDSWONFYIAAPE-UHFFFAOYSA-N silicon sulfide Chemical compound S=[Si]=S KHDSWONFYIAAPE-UHFFFAOYSA-N 0.000 description 1
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Classifications
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The present invention relates to an electrode assembly including a plurality of electrode structures including a positive electrode, a negative electrode, a solid electrolyte layer between the positive electrode and the negative electrode, and polymer layers at both ends of the electrode assembly, and a secondary battery including the electrode assembly.
Description
Technical Field
The present application claims priority from korean patent application No. 10-2021-01268239, filed 28 at 9 in 2021, and korean patent application No. 10-2022-012393, filed 26 at 9 in 2022, the entire contents of which are incorporated herein by reference.
The present invention relates to an electrode assembly for a secondary battery and a secondary battery including the same, and more particularly, to an electrode assembly for a secondary battery and a secondary battery including the same, which are capable of improving the life of the battery.
Background
As mobile device technologies develop and their demands increase, the demand for secondary batteries also increases rapidly, and among them, lithium secondary batteries having high energy density and operating voltage and excellent preservation and life properties are widely used as energy sources for various electronic products and various mobile devices.
Secondary batteries are broadly classified into cylindrical batteries, prismatic batteries, and pouch-type batteries according to external and internal structural features thereof, wherein the prismatic batteries and the pouch-type batteries can be stacked in a highly integrated manner and have a small width compared to their length, and these batteries are of particular interest.
In addition, secondary batteries are attracting attention as energy sources for electric vehicles, hybrid electric vehicles, and the like, which are proposed as solutions to air pollution caused by existing gasoline and diesel vehicles using fossil fuel. Therefore, due to the advantages of the secondary battery, the type of application using the secondary battery becomes very diversified, and in the future, the secondary battery is expected to be applied to more fields and products than now.
Therefore, as the application fields and products of secondary batteries are diversified, the types of batteries are also being diversified in order to provide output and capacity suitable for them. In addition, batteries applied to the related art and products are very required to be small and light.
For example, in the case of small mobile devices such as cell phones, PDAs, digital cameras, notebook computers, etc., one or two, or three or four small and light battery cells are used per device as related products tend to become smaller, lighter, and thinner. On the other hand, in the case of middle-and large-sized devices, such as electric vehicles and hybrid electric vehicles, a battery module (also referred to as "middle-and large-sized battery pack") in which a plurality of battery cells are electrically connected is being used due to the high output and large capacity required. Meanwhile, since the size and weight of the battery module are directly related to the receiving space and output of the related middle-and large-sized devices, etc., manufacturers have attempted to make the battery module as small and light as possible.
In a state in which the electrode assembly is received in a case formed on an exterior member and an inner surface thereof (composed of upper and lower units), a conventional pouch-type battery is formed by combining both sides, which are contact portions, with upper and lower ends. Since the exterior members have a laminated structure composed of a resin layer/a metal foil layer/a resin layer, they can be bonded by applying heat and pressure to both sides and upper and lower ends that are in contact with each other to bond the resin layers to each other, and in some cases, an adhesive can be used. Since both sides are in direct contact with the same resin layers of the upper and lower exterior members, it is possible to seal uniformly by melting. On the other hand, in the case of the upper and lower parts, since the electrode leads protrude, thermal fusion is performed in a state in which the sealing member on the film is interposed between the electrode leads in consideration of the thickness of the electrode leads and the heterogeneity of materials with the external member to improve sealability.
However, as the pouch type secondary battery repeatedly expands and contracts during charge and discharge, the internal pressure of the battery changes. Therefore, there is a problem in that the battery life is adversely affected.
That is, since the change in the internal pressure of the battery adversely affects the life of the battery, it is necessary to develop a technique capable of effectively controlling the change in the internal pressure of the battery.
[ Prior Art literature ]
[ patent literature ]
(patent document 1) korean patent publication 2014-0141825
(patent document 2) korean patent publication 2021-0039213
Disclosure of Invention
[ technical problem ]
In order to solve the above problems, it is an object of the present invention to provide an electrode assembly capable of effectively controlling internal pressure variation due to volume variation of a secondary battery to improve life performance of the secondary battery, and a pouch-type secondary battery including the same.
Technical scheme
In order to achieve the above object, the present invention provides an electrode assembly including an electrode structure including a positive electrode, a negative electrode, and a solid electrolyte layer disposed between the positive electrode and the negative electrode, wherein polymer layers are included on both ends of the electrode assembly.
Further, the present invention provides an electrode assembly, wherein the yield strength of the polymer layer is 5MPa or more and 20MPa or less.
Further, the present invention provides an electrode assembly, wherein the thickness of the polymer layer satisfies the following formula 1:
[ 1]
The thickness (μm) is more than or equal to 2.5 (μm cm) 2 /mAh.times.X (mAh/cm) 2 ) X and Y (personal)
Wherein X represents the capacity per unit area of the positive electrode, and Y represents the number of positive electrodes in the electrode assembly.
Further, the present invention provides an electrode assembly in which the polymer layer is formed of rubber or silicone resin.
Further, the present invention provides an electrode assembly, wherein the solid electrolyte layer includes a sulfide-based solid electrolyte, an oxide-based solid electrolyte, a polymer-based solid electrolyte, or two or more thereof.
Further, the present invention provides an electrode assembly in which the solid electrolyte layer is a sulfide-based solid electrolyte having a sulfur silver germanium ore structure.
Further, the present invention provides an electrode assembly, wherein the solid electrolyte layer comprises a material selected from the group consisting of Li 2 S-P 2 S 5 、Li 6 PS 5 Cl、Li 10 GeP 2 S 12 、Li 3 PS 4 And Li (lithium) 7 P 3 S 11 One or more of the following.
Further, the present invention provides an electrode assembly, wherein the electrode assembly includes a structure obtained by stacking 1 to 100 of the electrode structures.
Further, the present invention provides an electrode assembly, wherein the positive electrode includes a positive electrode active material, a sulfide-based solid electrolyte, a conductive material, and a binder.
Further, the present invention provides a pouch type secondary battery including the electrode assembly.
Advantageous effects
By including polymer layers having a specific yield strength and a specific thickness on both ends of the electrode assembly, the electrode assembly of the present invention can effectively control the change in internal pressure of the battery due to the volume change occurring during the charge and discharge of the secondary battery.
As described above, the present invention can improve the life characteristics of a secondary battery by effectively controlling the internal pressure variation that occurs during the charge and discharge of the secondary battery.
Drawings
Fig. 1 is a sectional view of a conventional pouch-type secondary battery.
Fig. 2 is a sectional view of a pouch-type secondary battery according to the present invention.
Fig. 3 is a graph showing life characteristics (capacity retention rate) of pouch type secondary batteries manufactured in examples 1 to 5 and comparative examples 1 to 4 of the present invention.
Fig. 4 is a graph showing life characteristics (capacity retention rate) of the pouch type secondary batteries manufactured in example 6 and comparative example 5 of the present invention.
Detailed Description
Hereinafter, the present invention will be described in more detail with reference to the accompanying drawings according to embodiments of the present invention, but the scope of the present invention is not limited thereto.
Referring to fig. 1, a conventional pouch type secondary battery is provided with a stacked electrode assembly 100 in which a plurality of electrode structures are stacked in a pouch type battery case 106. The electrode assembly 100 is composed of: a negative electrode in which a negative electrode active material layer 102 is stacked on both sides of a negative electrode current collector 101; a positive electrode in which positive electrode active material layers 104 are stacked on both sides of a positive electrode current collector 103; and a solid electrolyte layer 105 interposed between the positive electrode and the negative electrode.
A problem with such conventional pouch-type secondary batteries is that when the battery itself repeatedly expands and contracts during charge and discharge, the internal pressure of the battery changes due to the volume change of the electrode assembly, thereby shortening the life of the battery.
In order to solve the above-described conventional problems, the present invention provides an electrode assembly including an electrode structure including a positive electrode, a negative electrode, and a solid electrolyte layer disposed between the positive electrode and the negative electrode, wherein polymer layers are included on both ends of the electrode assembly.
In one embodiment of the present invention, the electrode assembly may be the electrode assembly 200 shown in fig. 2.
Specifically, referring to fig. 2, the electrode assembly of the present invention may have a structure including a negative electrode in which a negative electrode active material layer 202 is stacked on both sides of a negative electrode current collector 201, a positive electrode in which a positive electrode active material layer 204 is stacked on both sides of a positive electrode current collector 203, and a solid electrolyte layer 205 disposed between the positive electrode and the negative electrode, and further including a polymer layer 206 disposed on both ends.
In one embodiment of the present invention, the negative electrode current collector 201 and the positive electrode current collector 203 may be extended to form electrode tabs, respectively, and the electrode tabs may be extended to one side of the battery case. The electrode tab may be fused with one side of the battery case to form an electrode lead extending or exposed to the outside of the battery case.
In another embodiment of the present invention, the polymer layer 206 of the electrode assembly may be in the form of covering the entire surfaces of the adjacent positive and negative electrodes.
In another embodiment of the present invention, the polymer layer 206 of the electrode assembly may be equal to or greater than the area of the adjacent positive and negative electrodes.
In one embodiment of the present invention, the polymer layer may be an elastic body having an elastic force capable of responding to the internal pressure appropriately, thereby controlling the change in the internal pressure according to the volume change of the pouch type secondary battery.
In another embodiment of the present invention, the yield strength of the polymer layer may be 5MPa or more and 20MPa or less. More specifically, the yield strength of the polymer layer may be 5MPa or more, 6MPa or more, 7MPa or more, 8MPa or more, 9MPa or more, 10MPa or more, 11MPa or more, 12MPa or more, and may be 20MPa or less, 19MPa or less, 18MPa or less, 17MPa or less, 16MPa or less, 15MPa or less, 14MPa or less, and 13MPa or less, but is not limited thereto.
By satisfying the above yield strength range, the polymer layer can apply a constant pressure to the battery assembly during operation, so that the lithium metal layer forming the negative electrode is in contact with the solid electrolyte layer at a constant pressure, thereby suppressing the formation of lithium dendrites. In addition, the polymer layer may secure structural stability of the battery by contracting an amount corresponding to an expanded volume of the electrode assembly during operation of the battery.
If the yield strength of the polymer layer exceeds the above range, the internal pressure of the pouch-type secondary battery cannot be effectively controlled, and thus it is preferable that the yield strength of the polymer layer satisfies the above range.
In one embodiment of the present invention, the thickness of the polymer layer may satisfy the following formula 1.
[ 1]
The thickness (μm) is more than or equal to 2.5 (μm cm) 2 /mAh.times.X (mAh/cm) 2 ) X and Y (personal)
Where X represents the capacity per unit area of the positive electrode and Y represents the number of positive electrodes in the electrode assembly.
The polymer layer serves to buffer the volume change of the electrode assembly during the operation of the battery, and preferably has a thickness sufficient to buffer the volume change of the electrode assembly.
That is, if the thickness of the polymer layer of the present invention does not satisfy the above-described range, the volume change of the electrode assembly cannot be sufficiently buffered to effectively control the internal pressure of the electrode assembly, and thus it is preferable that the thickness of the polymer layer satisfies the above-described range.
However, if the thickness of the polymer layer is too thick, the thickness of the polymer layer is preferably less than 5000 μm because the volume of the battery may become too large to be preferable. The thickness of the polymer layer may be, for example, 3000 μm or less, 1000 μm or less, 500 μm or less, or 100 μm or less, but is not limited thereto.
In one embodiment of the present invention, the polymer layer may be an elastomer, and the elastomer may have a structure made of rubber or silicone resin, but is not limited thereto.
The polymer layer is not limited in its type and composition as long as it can cover the surfaces of the positive and negative electrodes at both ends of the battery assembly, and has a uniform thickness and uniform yield strength, and does not affect the operation of the battery.
The polymer layer may be a silicone rubber pad (silicone rubber pad) in terms of maintaining a uniform thickness and uniform yield strength without affecting the operation of the cell.
In one embodiment of the present invention, the solid electrolyte layer is not particularly limited to a specific composition, and may contain one or more of a crystalline solid electrolyte, an amorphous solid electrolyte, and an inorganic solid electrolyte (e.g., a glass-ceramic solid electrolyte).
In one embodiment of the present invention, the solid electrolyte layer may contain a sulfide-based solid electrolyte, an oxide-based solid electrolyte, a polymer-based solid electrolyte, or two or more thereof.
In another embodiment of the present invention, the solid electrolyte layer may include a sulfide-based solid electrolyte having a sulfur silver germanium ore structure.
The solid electrolyte layer may preferably contain a sulfide-based solid electrolyte, examples of which include lithium sulfide, silicon sulfide, germanium sulfide, and boron sulfide. Specific examples of such solid electrolytes may include LPS type solid electrolytes, such as Li 2 S-P 2 S 5 And Li 3.833 Sn 0.833 As 0.166 S 4 、Li 4 SnS 4 、Li 3.25 Ge 0.25 P 0.75 S 4 、B 2 S 3 -Li 2 S、xLi 2 S-(100-x)P 2 S 5 (x＝70～80)、Li 2 S-SiS 2 -Li 3 N、Li 2 S-P 2 S 5 -LiI、Li 2 S-SiS 2 -LiI、Li 2 S-B 2 S 3 -LiI、Li 3 N、LISICON、LIPON(Li 3+y PO 4-x N x ) Thio LISICON (Li) 3.25 Ge 0.25 P 0.75 S 4 )、Li 2 O-Al 2 O 3 -TiO 2 -P 2 O 5 (LATP) and the like.
Preferably, the solid electrolyte layer may include a material selected from the group consisting of Li 2 S-P 2 S 5 、Li 6 PS 5 Cl、Li 10 GeP 2 S 12 、Li 3 PS 4 And Li (lithium) 7 P 3 S 11 One or more of the group consisting of.
In one embodiment of the present invention, the electrode assembly may include a plurality of electrode structures, for example, may include 1 to 100 electrode structures, and preferably may include 1 to 50 electrode structures.
In one embodiment of the present invention, the positive electrode may be composed of a positive electrode active material layer and a positive electrode current collector, and the positive electrode active material layer may include a positive electrode active material, a sulfide-based solid electrolyte, a conductive material, and a binder.
In another embodiment of the invention, the binder may be crosslinked. The content ratio of the sulfide-based solid electrolyte in the positive electrode active material layer may be 5 parts by weight to 100 parts by weight with respect to 100 parts by weight of the positive electrode active material. Further, the content ratio of the binder may be 0.1 to 10 parts by weight with respect to 100 parts by weight of the positive electrode active material layer, and the content ratio of the conductive material may be 0.1 to 10 parts by weight with respect to 100 parts by weight of the positive electrode active material layer.
In one embodiment of the present invention, crosslinking of the binder in the positive electrode active material layer may be achieved by introducing a crosslinking agent solution. According to another embodiment of the present invention, after impregnating the entire electrode assembly with the crosslinking agent solution, crosslinking is performed in the entire electrode assembly, so that crosslinking of the binder can also be formed at, for example, an interface between the electrode and the solid electrolyte. Alternatively, in another embodiment of the present invention, crosslinking may be performed only in the positive electrode depending on the object to be impregnated with the crosslinking agent solution.
In one embodiment of the present invention, when the binder is crosslinked, mechanical properties (e.g., elasticity or rigidity) of the positive electrode are improved so that even if the positive electrode active material expands and/or contracts during charge and discharge, the positive electrode active material layer can suppress or mitigate these effects, and since the adhesiveness of the interface between the positive electrode active material layer and the solid electrolyte layer is maintained, an all-solid battery having excellent cycle characteristics can be provided.
In one embodiment of the invention, the adhesive comprises a rubber-based adhesive resin. The rubber-based binder resin may be dissolved in a nonpolar solvent. If the components of the sulfide-based solid electrolyte are contacted with the polar solvent, they may cause deterioration of physical properties such as reduction of ion conductivity, etc. Therefore, in the present invention, in manufacturing an electrode, a nonpolar solvent is used instead of a polar solvent, and a rubber-based binder resin having high solubility in the nonpolar solvent is used as a component of the binder. In one embodiment of the present invention, as the rubber-based binder resin, those which are soluble at about 25 ℃ to 50 wt% or more, 70 wt% or more, 90 wt% or more, or 99 wt% or more with respect to the solvent used may be selected. In addition, the solvent may comprise a nonpolar solvent having a polarity index of 0 to 3 and/or a dielectric constant of less than 5. By using the nonpolar solvent as described above, a decrease in ion conductivity of the sulfide-based solid electrolyte due to the use of the polar solvent can be prevented.
In one embodiment of the present invention, the positive electrode active material may include one or a mixture of two or more of the following: layered compounds, e.g. lithium manganese complex oxides (LiMn 2 O 4 、LiMnO 2 Etc.), lithium cobalt oxide (LiCoO 2 ) Lithium nickel oxide (LiNiO) 2 ) Or go throughOne or more transition metal substituted compounds; lithium manganese oxides, e.g. of formula Li 1+x Mn 2-x O 4 (wherein x is 0-0.33), liMnO 3 、LiMn 2 O 3 And LiMnO 2 The method comprises the steps of carrying out a first treatment on the surface of the Lithium copper oxide (Li) 2 CuO 2 ) The method comprises the steps of carrying out a first treatment on the surface of the Vanadium oxides, e.g. LiV 3 O 8 、LiFe 3 O 4 、V 2 O 5 And Cu 2 V 2 O 7 The method comprises the steps of carrying out a first treatment on the surface of the From LiNi 1-x M x O 2 (wherein m=co, mn, al, cu, fe, mg, B or Ga, x=0.01-0.3); from LiMn 2-x M x O 2 (wherein M=Co, ni, fe, cr, zn or Ta, x=0.01-0.1) or Li 2 Mn 3 MO 8 (wherein m=fe, co, ni, cu or Zn); liMn in which part of Li is replaced by alkaline earth metal ion 2 O 4 The method comprises the steps of carrying out a first treatment on the surface of the A disulfide compound; fe (Fe) 2 (MoO 4 ) 3 。
In one embodiment of the present invention, the adhesive may comprise a rubber-based adhesive resin. Since PVdF-based binder resins or acrylic binder resins used as electrode binders have low solubility in nonpolar solvents, it is difficult to prepare electrode pastes. Therefore, in the present invention, a rubber-based resin having high solubility in a nonpolar solvent is used as the binder. In one embodiment of the present invention, the rubber-based binder resin may include at least one selected from the group consisting of: natural rubber, butyl rubber, bromobutyl rubber, chlorinated butyl rubber, styrene isoprene rubber, styrene-ethylene-butylene-styrene rubber, acrylonitrile-butadiene-styrene rubber, polybutadiene rubber, nitrile-butadiene rubber, styrene-butadiene-styrene rubber (SBS) and Ethylene Propylene Diene Monomer (EPDM) rubber.
In one embodiment of the present invention, the conductive material may be, for example, at least one selected from the group consisting of: graphite, carbon black, carbon fiber or metal fiber, metal powder, conductive whisker, conductive metal oxide, activated carbon and polyphenylene derivative, or a mixture of two or more conductive materials among them. More specifically, the conductive material may be at least one selected from the group consisting of: natural graphite, artificial graphite, super-p, acetylene black, ketjen black, channel black, furnace black, lamp black, thermal black, denka black, aluminum powder, nickel powder, zinc oxide, potassium titanate, and titanium oxide, or a mixture of two or more of these conductive materials.
In one embodiment of the present invention, the anode may include an anode active material stacked on an anode current collector, and the anode active material may include any one selected from the group consisting of: lithium metal oxides, carbon, e.g., non-graphitized carbon, graphite-based carbon; metal complex oxides, e.g. Li x Fe 2 O 3 (0≤x≤1)、Li x WO 2 (0≤x≤1)、Sn x Me 1-x Me' y O z (Me: mn, fe, pb, ge; me': al, B, P, si, elements of groups 1,2 and 3 of the periodic Table, halogen; 0)<x is less than or equal to 1; y is more than or equal to 1 and less than or equal to 3; z is more than or equal to 1 and less than or equal to 8); lithium metal; a lithium alloy; silicon-based alloy; a tin-based alloy; metal oxides, e.g. SnO, snO 2 、PbO、PbO 2 、Pb 2 O 3 、Pb 3 O 4 、Sb 2 O 3 、Sb 2 O 4 、Sb 2 O 5 、GeO、GeO 2 、Bi 2 O 3 、Bi 2 O 4 、Bi 2 O 5 The method comprises the steps of carrying out a first treatment on the surface of the Conductive polymers such as polyacetylene; lithium cobalt nickel material; titanium oxide; or a mixture of two or more thereof.
In one embodiment of the present invention, the positive electrode current collector and the negative electrode current collector are not particularly limited as long as they have high conductivity without causing chemical changes in the battery, and may be, for example, stainless steel, copper, aluminum, nickel, titanium, sintered carbon, or aluminum or stainless steel surface-treated with carbon, nickel, titanium, silver, or the like.
The present invention provides a pouch-type secondary battery in which the above-described electrode assembly is accommodated.
Specifically, the above-described positive electrode, solid electrolyte layer, and negative electrode are sequentially stacked and laminated to manufacture a unit electrode structure, then the solid electrolyte layer is interposed between a plurality of unit electrode structures to prepare a stacked body of the unit electrode structure, then the above-described polymer layers are stacked at both ends of the stacked body of the unit electrode structure, then they are accommodated in a pouch-type battery case, and then sealed to manufacture a pouch-type secondary battery.
Hereinafter, preferred embodiments are given to aid in understanding the present invention, but the following embodiments are provided for easier understanding of the present invention, and the present invention is not limited thereto.
Examples
Manufacturing of pouch-type secondary battery
1. Example 1
A positive electrode active material, a sulfide-based solid electrolyte (Li 6 PS 5 Cl), a conductive material, and a binder are mixed at a mass ratio of 80:15:1:4 to prepare a slurry for a positive electrode active material. The slurry for positive electrode active material was prepared at a rate of 4mAh/cm 2 Is applied to an aluminum current collector, and then dried to manufacture a positive electrode. Lithium metal was pressed on a copper foil to a thickness of 20 μm and used as a negative electrode. As the solid electrolyte layer, sulfide-based solid electrolyte (Li 6 PS 5 Cl)。
The positive electrode, the solid electrolyte layer, and the negative electrode were stacked in this order, and then laminated to manufacture a unit electrode structure. Two of the above-described unit electrode structures were prepared, and a solid electrolyte layer was laminated between the positive electrode of each unit electrode structure and the other unit electrode structure to prepare a stacked body of unit electrode structures.
Thereafter, a silicone rubber pad having a thickness of 20 μm and a yield strength of 5MPa was attached as a polymer layer to both ends of the stack of unit electrode structures to manufacture an electrode assembly.
The electrode assembly was received in a pouch-type battery case, and then sealed to prepare a pouch-type secondary battery.
2. Example 2
A pouch-type secondary battery was manufactured in the same manner as in example 1, except that the yield strength of the silicone rubber pad was 10 MPa.
3. Example 3
A pouch-type secondary battery was manufactured in the same manner as in example 1, except that the yield strength of the silicone rubber pad was 20 MPa.
4. Example 4
A pouch-type secondary battery was fabricated in the same manner as in example 1, except that the thickness of the silicone rubber pad was 50 μm.
5. Example 5
A pouch-type secondary battery was fabricated in the same manner as in example 1, except that the thickness of the silicone rubber pad was 100 μm.
6. Example 6
A pouch-type secondary battery was manufactured in the same manner as in example 1, except that the slurry for the positive electrode active material was prepared at 3mAh/cm 2 Is applied to the aluminum current collector, and the thickness of the silicone rubber pad is 15 μm.
Comparative example
1. Comparative example 1
A pouch-type secondary battery was manufactured in the same manner as in example 1, except that a silicone rubber pad was not included.
2. Comparative example 2
A pouch-type secondary battery was manufactured in the same manner as in example 1, except that the yield strength of the silicone rubber pad was 3 MPa.
3. Comparative example 3
A pouch-type secondary battery was manufactured in the same manner as in example 1, except that the yield strength of the silicone rubber pad was 30 MPa.
4. Comparative example 4
A pouch-type secondary battery was fabricated in the same manner as in example 1, except that the thickness of the silicone rubber pad was 15 μm.
5. Comparative example 5
A pouch-type secondary battery was fabricated in the same manner as in example 6, except that the thickness of the silicone rubber pad was 10 μm.
Experimental example
1. Measuring volume change occurring during charge/discharge of pouch-type secondary battery
For the pouch type secondary batteries of examples 1 to 5 and comparative examples 1 to 4, the volume change occurring during charge/discharge was measured.
Specifically, for the pouch type secondary batteries of examples 1 to 5 and comparative examples 1 to 4, the charging and discharging were initially (once) performed at room temperature using an electrochemical device for charging and discharging, and then the volume of the pouch type secondary batteries was measured. In charging and discharging, charging is performed by applying a current at a current density of 0.1C magnification up to a voltage of 4.2V, and discharging to 3.0V at the same current density. It is defined as the initial volume.
Thereafter, after a total of 100 times of charge and discharge were performed, the volume was measured. Which is defined as the final volume.
The volume change rate (%) was calculated by substituting the measured values of the initial volume and the final volume into the following equation 2, and the results are shown in table 1.
[ equation 2]
Volume change rate (%) = { (final volume-initial volume)/initial volume } ×100 (%)
Table 1:
| rate of change in volume (%) | |
| Example 1 | 2 |
| Example 2 | 2 |
| Example 3 | 2 |
| Example 4 | 2 |
| Example 5 | 2 |
| Comparative example 1 | 6 |
| Comparative example 2 | 6 |
| Comparative example 3 | 2 |
| Comparative example 4 | 5 |
Referring to table 1 above, it was confirmed that in the case of the pouch type secondary batteries of examples 1 to 5 of the present invention, the change in internal pressure was effectively controlled as compared with the pouch type secondary batteries of comparative examples 1 to 2 and 4.
Meanwhile, in the case of the pouch type secondary battery of comparative example 3, since the yield strength of the silicone rubber pad is too large, the internal pressure of the pouch type secondary battery is excessively high, although the volume change of the pouch type secondary battery is small, thereby causing a short circuit and thus rapid deterioration of life performance.
2. Evaluation of life characteristics of pouch-type secondary batteries
The capacity retention was measured in the following manner using the pouch type secondary batteries of examples 1 to 6 and comparative examples 1 to 5. The results are shown in table 2, fig. 3 and fig. 4.
(1) Specifically, for the pouch-type secondary batteries of examples 1 to 5 and comparative examples 1 to 4, charging and discharging were initially (once) performed at room temperature using an electrochemical device for charging and discharging. In charging and discharging, charging is performed by applying a current at a current density of 0.1C magnification up to a voltage of 4.2V, and discharging to 3.0V at the same current density. The above-described charge and discharge were performed 100 times in total.
The capacity of each cell was measured during the above-described charge and discharge processes.
Thus, the capacity retention rate of each battery was calculated according to the following equation 3, and the results are shown in table 2 below.
[ equation 3]
Capacity retention (%) = (capacity at 100 th cycle/initial capacity) ×100
Table 2:
as shown in table 2 above, it was confirmed that the capacity retention rate of the pouch type secondary batteries of examples 1 to 5 of the present invention was significantly improved as compared to the pouch type secondary batteries of comparative examples 1 to 4.
(2) Further, for the pouch type secondary batteries of example 6 and comparative example 5, charging and discharging were initially performed (once) at room temperature using an electrochemical device for charging and discharging. In charging and discharging, charging is performed by applying a current at a current density of 0.1C magnification up to a voltage of 4.2V, and discharging to 3.0V at the same current density. The above charge and discharge were performed 50 times in total.
The capacity of each cell was measured during the above-described charge and discharge processes, and the results are shown in fig. 4.
As shown in fig. 4, it was confirmed that the capacity retention rate of the pouch type secondary battery of example 6 of the present invention was significantly improved as compared with the pouch type secondary battery of comparative example 5.
(3) When this was considered, it was confirmed that in the pouch type secondary battery of the present invention, when an elastic body having a yield strength of 5 to 20MPa and a thickness satisfying the following formula 1 was disposed on both ends of the stack of unit electrode structures, the life characteristics were significantly improved.
[ 1]
The thickness (μm) is more than or equal to 2.5 (μm cm) 2 /mAh.times.X (mAh/cm) 2 ) X and Y (personal)
Where X represents the capacity per unit area of the positive electrode and Y represents the number of positive electrodes in the electrode assembly.
All simple modifications and variations of the invention fall within the scope of the invention, and the particular scope of the invention will become apparent from the appended claims.
[ description of reference numerals ]
10,20 pouch-type secondary battery
100,200 electrode Assembly
101,201 negative electrode current collector
102,202 negative electrode active material layer
103,203 positive electrode current collector
104,204 positive electrode active material layer
105,205 solid electrolyte layer
106,207 Battery case
Claims (10)
1. An electrode assembly comprising an electrode structure comprising a positive electrode, a negative electrode, a solid electrolyte layer between the positive electrode and the negative electrode, and polymer layers at both ends of the electrode assembly.
2. The electrode assembly of claim 1, wherein the polymer layer has a yield strength of 5MPa or more and 20MPa or less.
3. The electrode assembly of claim 1, wherein a thickness of the polymer layer satisfies the following formula 1:
[ 1]]The thickness (μm) is more than or equal to 2.5 (μm cm) 2 /mAh.times.X (mAh/cm) 2 ) X and Y (personal)
Wherein X represents the capacity per unit area of the positive electrode, and Y represents the number of positive electrodes in the electrode assembly.
4. The electrode assembly of claim 1, wherein the polymer layer is formed of rubber or silicone resin.
5. The electrode assembly of claim 1, wherein the solid electrolyte layer comprises a sulfide-based solid electrolyte, an oxide-based solid electrolyte, a polymer-based solid electrolyte, or two or more thereof.
6. The electrode assembly of claim 1, wherein the solid electrolyte layer comprises a sulfide-based solid electrolyte having a sulfur silver germanium ore structure.
7. The electrode assembly of claim 1, wherein the solid electrolyte layer comprises a material selected from the group consisting of Li 2 S-P 2 S 5 、Li 6 PS 5 Cl、Li 10 GeP 2 S 12 、Li 3 PS 4 And Li (lithium) 7 P 3 S 11 One or more of the group consisting of.
8. The electrode assembly according to claim 1, wherein the electrode assembly comprises a structure body in which 1 to 100 of the electrode structure bodies are stacked.
9. The electrode assembly of claim 1, wherein the positive electrode comprises a positive electrode active material, a sulfide-based solid electrolyte, a conductive material, and a binder.
10. A pouch type secondary battery comprising the electrode assembly of claim 1.
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| KR10-2021-0128239 | 2021-09-28 | ||
| KR1020220121373A KR20230045568A (en) | 2021-09-28 | 2022-09-26 | Electrode assembly for a rechargeable battery and a rechargeable battery comprising the same |
| KR10-2022-0121373 | 2022-09-26 | ||
| PCT/KR2022/014507 WO2023055044A1 (en) | 2021-09-28 | 2022-09-28 | Electrode assembly for secondary battery, and secondary battery comprising same |
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| CN116529925A true CN116529925A (en) | 2023-08-01 |
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| CN202280007079.3A Pending CN116529925A (en) | 2021-09-28 | 2022-09-28 | Electrode assembly for secondary battery and secondary battery including the same |
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| CN (1) | CN116529925A (en) |
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