Separator for lithium secondary battery and manufacturing method thereof

Abstract

The separator according to the present invention has an organic / inorganic composite porous coating layer formed on the surface of a polymer substrate, and the organic / inorganic composite porous coating layer has a first region having a high content of inorganic particles and a second region having a low content of inorganic particles, and the first region improves wettability of the electrolyte, and the second region enables high adhesive strength with the electrode to be maintained.

Description

[Technical field]

[0001] The present invention relates to a separator for a lithium secondary battery and a method for producing the same. This application claims priority to Korean Patent Application No. 2022-0026842 filed on March 2, 2022, the entire contents of which are incorporated herein by reference in their entirety in the specification and drawings. [Background technology]

[0002] In recent years, interest in energy storage technology has been increasing. Applications are expanding to include mobile phones, camcorders, and notebook computers, as well as the energy of electric vehicles, and as a result, research and development efforts on electrochemical elements are becoming more and more concrete. Among the wide range of electrochemical elements, lithium secondary batteries, which can be charged and discharged, have a high operating voltage, and have a much higher energy density, are attracting attention.

[0003] A lithium secondary battery is manufactured by using a material into which lithium ions can be inserted and extracted as an active material for a positive electrode and a negative electrode, respectively, disposing a porous separator between the positive electrode and the negative electrode, and injecting a liquid electrolyte. Electricity is generated or consumed by an oxidation-reduction reaction accompanying the insertion and desorption of lithium ions in the negative electrode and the positive electrode.

[0004] As the porous separator, a microporous membrane made of a polyolefin material is used, or a composite separator in which a coating layer containing inorganic particles is formed on the surface of a microporous membrane in consideration of improving mechanical properties and safety is used.

[0005] On the other hand, as a part of increasing the energy density of batteries, the development of large-area batteries is being considered. However, when the area of ​​a battery is expanded, the electrolyte does not flow smoothly to the center of the inside of the battery, and the movement of lithium ions is restricted due to a lack of electrolyte in the parts that are not wetted by the electrolyte, and lithium is precipitated from the parts where the movement of lithium ions is concentrated. For this reason, there is a current situation where the development of a separator with improved electrolyte flow characteristics to the inside of the battery is required even for large-area batteries. Summary of the Invention [Problem to be solved by the invention]

[0006] An object of the present invention is to provide a separator for an electrochemical element which has excellent wettability with an electrolyte and adhesive strength with electrodes.

[0007] As will be readily apparent to those skilled in the art, the objects and advantages of the present invention can be realized by the means or methods recited in the claims and combinations thereof. [Means for solving the problem]

[0008] In order to solve the above problems, a first aspect of the present invention provides a separator for an electrochemical element according to the following embodiments.

[0009] The separator for electrochemical elements according to a first aspect comprises a porous polymer substrate and a porous organic / inorganic composite coating layer formed on both surfaces or on at least one surface of the polymer substrate, the organic / inorganic composite coating layer being defined into a first region and a second region, the first region and the second region each independently comprising inorganic particles and a binder material, and the separator for electrochemical elements according to a first aspect is characterized in that the content ratio of inorganic particles in the first region based on Formula 1 is higher than the content ratio of inorganic particles in the second region based on Formula 2. [Formula 1] Inorganic particle content ratio (wt%) of the first region = [amount of inorganic particles in the first region / (amount of inorganic particles in the first region + amount of binder material in the first region)] × 100 ... (1) [Formula 2] Content ratio (wt%) of inorganic particles in the second region = [amount of inorganic particles in the second region / (amount of inorganic particles in the second region + amount of binder material in the second region)] × 100 ... (2)

[0010] According to a second aspect, the separator for an electrochemical element may be the separator for an electrochemical element according to the first aspect, wherein the porosity of the first region in the coating layer is higher than the porosity of the second region.

[0011] According to a third aspect, the separator for electrochemical elements may be as described in the first or second aspect, in which the content ratio of inorganic particles in the first region is higher than that in the second region and is 70 wt % or more and 90 wt % or less.

[0012] According to a fourth aspect, the separator for electrochemical elements may be the one described in any one of the first to third aspects, in which the content ratio of inorganic particles in the second region is lower than that in the first region and is 85 wt % or less.

[0013] According to a fifth aspect, the separator for electrochemical elements may be as described in any one of the first to fourth aspects, in which the second region is disposed in a partial section around the first region, at least a part of a side surface of the first region is exposed to the outside, and the second region is disposed so as to be in contact with the boundary of the first region.

[0014] According to a sixth aspect, the separator for an electrochemical element according to any one of the first to fifth aspects may be a single, integral region, or may be divided into two or more units, with any one of the units being disposed apart from the other units.

[0015] According to a seventh aspect, the separator for electrochemical elements may be as described in any one of the first to sixth aspects, in which the first region is arranged in a rectangular shape inside a surface of a polymer-based material, and the second region has units arranged on one side of the first region and on another side opposite thereto, and the second region is not arranged on the remaining two sides.

[0016] According to an eighth aspect, the separator may be a separator for an electrochemical element according to any one of the first to seventh aspects, wherein the separator is a rectangle having an aspect ratio of more than 1, and the second regions are disposed on two shorter sides of the separator, respectively.

[0017] A second aspect of the present invention provides an electrochemical device according to the following embodiment.

[0018] An electrochemical device according to a ninth aspect relates to an electrochemical device including an electrode assembly including a positive electrode, a negative electrode, and a separator sandwiched between the positive electrode and the negative electrode, the separator being as described in any one of the first to eighth aspects.

[0019] According to a tenth aspect, the electrochemical device may be the electrochemical device according to the ninth aspect, which is a lithium ion secondary battery.

[0020] A third aspect of the present invention provides a method for producing a separator according to the following embodiment.

[0021] A method for producing a separator according to an eleventh aspect is a method for producing the separator according to any one of the first to eighth aspects, and the method is carried out by a roll-to-roll process in which a long, rectangular polymer substrate is continuously supplied, and includes a step of forming second regions having a predetermined width on both ends of the polymer substrate in a width direction (TD direction) perpendicular to the running direction (MD direction) and forming a first region between the second regions to obtain a separator strip including a composite coating layer having a first region and a second region.

[0022] According to a twelfth aspect, the method for producing the separator according to the eleventh aspect may be such that the formation of the first region and the second region is carried out by applying slurries for forming the first region and the second region to defined portions, respectively, using a double slot die.

[0023] According to a thirteenth aspect, the method may be a method for producing the separator according to the eleventh or twelfth aspect, in which the separator strip is cut to a predetermined width to obtain a separator, and side surfaces of the first region are exposed at both ends in the MD direction of the polymer-based material. Effect of the Invention

[0024] A separator according to one aspect of the present invention includes an organic / inorganic composite porous coating layer formed on a surface of a polymer substrate, the organic / inorganic composite porous coating layer having a first region having a high content of inorganic particles and a second region having a low content of inorganic particles, and the first region can improve wettability of the electrolyte and the second region can maintain high adhesive strength with the electrode, but the effects of the present invention are not limited thereto. [Brief description of the drawings]

[0025] [Figure 1] 1 is a schematic diagram of a separator according to the present invention. [Diagram 2]1 is a schematic diagram showing a method for producing a separator according to the present invention. [Diagram 3] 1 is a photographic image of the negative electrode surface taken from the battery of Example 1. [Figure 4] 1 is a photographic image of the negative electrode surface taken from the battery of Example 2. [Diagram 5] 1 is a photographic image of the negative electrode surface taken out from the battery of Comparative Example 1. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0026] The present invention will be described in detail below. Prior to this, the terms and words used in the present specification and claims are not to be construed as being limited to their ordinary or dictionary meanings, but are to be construed as being in accordance with the meaning and concept of the technical idea of ​​the present invention, in accordance with the principle that the inventor himself can appropriately define the concept of the term in order to best describe the invention. Therefore, it should be understood that the embodiment described in this specification and the configuration shown in the drawings are merely the most preferred embodiment of the present invention, and do not represent the entire technical idea of ​​the present invention, and therefore there may be various equivalents and modifications that can be substituted therefor at the time of this application.

[0027] Throughout this specification, when a part is described as "comprising" a certain component, this does not mean that other components are excluded, and means that other components may also be included, unless otherwise specified.

[0028] Throughout this specification, the phrase "A and / or B" means "A or B or both."

[0029] One aspect of the present invention relates to a separator for an electrochemical element.

[0030] The electrochemical device is a device that converts chemical energy into electrical energy through an electrochemical reaction, and is a concept that encompasses both primary and secondary batteries. The secondary battery is capable of being charged and discharged, and is a concept that encompasses lithium ion batteries, nickel-cadmium batteries, nickel-metal hydride batteries, etc.

[0031] In this specification, the separator serves as a porosity-conducting barrier that allows ions to pass while blocking electrical contact between the negative and positive electrodes in an electrochemical device. It is preferable that a plurality of pores are formed inside the separator, and the pores are interconnected to allow gas and / or liquid to pass from one side of the separator to the other side.

[0032] A separator 100 according to one aspect of the present invention includes a porous polymer substrate 110 that includes a plurality of pores and includes a polymer material. The separator further includes a porous organic / inorganic composite coating layer (hereinafter referred to as coating layer 120) disposed on both surfaces or on at least one surface of the polymer substrate 110.

[0033] In one embodiment of the present invention, the coating layer may have a layered structure including inorganic particles and a binder material, and the inorganic particles are bound by the binder material. The coating layer has a porous structure due to spaces (interstitial volumes) formed between the inorganic particles. This porous structure has the effect of improving the electrolyte retention of the separator.

[0034] In one embodiment of the present invention, the coating layer may be 3 vol% to 40 vol% based on the total volume of the separator being 100 vol%, and simultaneously or independently, the layer thickness of the coating layer may be 5% to 50% based on the total film thickness of the separator being 100%.

[0035] In one embodiment of the present invention, the polymer substrate is a sheet-like porous membrane including a polymer material and having a plurality of pores. For example, the polymer substrate may have a form including at least one selected from the group consisting of porous polymer films and nonwoven fabrics. The pores include open pores, and the open pores are structured to be interconnected, allowing gas and / or liquid to pass from one side of the polymer substrate to the other side.

[0036] In one embodiment of the present invention, the polymer-based material may have an air permeability of 2000 sec / 100 cc or less and a porosity of 30 vol% to 60 vol% in terms of battery output and cycle characteristics. Meanwhile, in the present invention, the polymer-based material may have a pore diameter in the range of 10 nm to 100 nm.

[0037] In the present invention, the air permeability means the time (seconds) required for 100 ml of air to pass through a polymer substrate or separator having a size of 1 square inch under a constant air pressure of 4.8 inches. The air permeability can be measured, for example, using an EG01-55-1MR device manufactured by Asahi Seiko Co., Ltd.

[0038] In the present invention, the porosity means the ratio of the volume of pores to the total volume, and is expressed in units of vol% and can be used interchangeably with terms such as porosity and net density. In the present invention, the measurement of the porosity is not particularly limited, and can be measured, for example, by the Brunauer-Emmett-Teller (BET) measurement method using nitrogen gas or by a mercury porosimeter according to an embodiment of the present invention. Alternatively, in one embodiment of the present invention, the true density of the object to be measured can be calculated from the density (apparent density) of the object to be measured for porosity, the composition ratio of the components constituting the object, and the density of each component, and the porosity of the object to be measured can be calculated from the difference between the apparent density and the true density (net density).

[0039] In one embodiment of the present invention, the polymer-based material may have a thickness of 5 μm to 20 μm in terms of thinning the electrochemical device and increasing the energy density. If the thickness of the polymer-based material is less than this range, the conductive barrier function is insufficient, whereas if the thickness excessively exceeds this range (i.e., is too thick), the resistance of the separator may increase excessively.

[0040] In one embodiment of the present invention, the polymer material is preferably a thermoplastic resin having a melting point of 200° C. or less from the viewpoint of providing a shutdown function, and may include one or more polyolefin-based resins. The shutdown function refers to a function in which, when the temperature of the battery becomes high, the polymer resin melts and closes the pores of the polymer substrate, thereby blocking the movement of ions between the positive and negative electrodes and preventing thermal runaway of the battery.

[0041] The polyolefin resin may include, for example, any one or more selected from the group consisting of polyethylene, polypropylene, polybutene, and polypentene. In particular, the polyolefin resin may be polyethylene and / or polypropylene. In addition, the polymer material may further include, together with the polyolefin resin, any one or more selected from polymer resins such as polyethylene terephthalate, polybutylene terephthalate, polyacetal, polyamide, polycarbonate, polyimide, polyether ether ketone, polyether sulfone, polyphenylene oxide, polyphenylene sulfide, and polyethylene naphthalene.

[0042] Next, the inorganic particles and binder material contained in the coating layer of the separator will be described.

[0043] In one embodiment of the present invention, the inorganic particles are not particularly limited as long as they have a particle size smaller than the desired thickness of the coating layer, for example, a particle size of 1 / 2 to 1 / 1,000 of the thickness of the coating layer, and are electrochemically stable. For example, the diameter of the inorganic particles may be 10 nm or more. Meanwhile, for example, the diameter of the inorganic particles may be 10 μm or less, 7 μm or less, 5 μm or less, 2 μm or less, or 1 μm or less. That is, the inorganic particles are selected from the group consisting of inorganic particles having a diameter within the operating voltage range (e.g., Li / Li) of the applied electrochemical device. + There are no particular limitations as long as oxidation and / or reduction reactions do not occur at a potential of 0 to 5 V relative to the reference potential. In particular, when inorganic particles having ion-transferability are used, the ion conductivity in the electrochemical element can be increased to improve performance. In addition, when inorganic particles having a high dielectric constant are used as the inorganic particles, they can contribute to an increase in the degree of dissociation of the electrolyte salt in the liquid electrolyte, for example, the lithium salt, thereby improving the ion conductivity of the electrolyte solution.

[0044] For the reasons described above, in a specific embodiment of the present invention, the inorganic particles may include high dielectric constant inorganic particles having a dielectric constant of 5 or more, or 10 or more, inorganic particles having lithium ion transfer ability, or a mixture thereof. Non-limiting examples of inorganic particles having a dielectric constant of 5 or more include BaTiO 3 , Pb(Zr,Ti)O 3 (PZT), Pb 1-x La x Zr 1-y Ti y O 3 (PLZT, where 0 <x<1,0<y<1である。)、Pb(Mg 1 / 3 Nb 2 / 3 )O 3 -PbTiO 3 (PMN-PT), hafnia (HfO 2 ), SrTiO 3 , SnO 2 , CEO 2 , MgO, NiO, CaO, ZnO, ZrO 2 , Y 2 O 3 , Al 2 O 3 , SiC, TiO 2 These can be used alone or in combination of two or more. In particular, the above-mentioned BaTiO 3 , Pb(Zr,Ti)O 3 (PZT), Pb 1-x La x Zr 1-y Ti y O 3 (PLZT, where 0 <x<1,0<y<1である。)、Pb(Mg 1 / 3 Nb 2 / 3 )O 3 -PbTiO 3 (PMN-PT), hafnia (HfO 2Inorganic particles such as ) not only exhibit high dielectric constant characteristics with a dielectric constant of 100 or more, but also have piezoelectricity, which generates an electric charge when stretched or compressed by applying a certain pressure, resulting in a potential difference between both surfaces, thereby preventing the occurrence of internal short circuits in both electrodes due to external impact and improving the safety of electrochemical devices. In addition, when the above-mentioned inorganic particles with high dielectric constant are mixed with inorganic particles having lithium ion transport ability, the synergistic effect of these two can be multiplied.

[0045] In a specific embodiment of the present invention, the inorganic particles having lithium ion transport ability refer to inorganic particles that contain lithium elements but do not store lithium but have the function of transporting lithium ions. The inorganic particles having lithium ion transport ability can transport and transport lithium ions through a type of defect present inside the particle structure, thereby improving the conductivity of lithium ions in a battery and thereby improving the battery performance. Non-limiting examples of the inorganic particles having lithium ion transport ability include lithium phosphate (Li 3 PO 4 ), lithium titanium phosphate (Li x Ti y (PO 4 ) 3 ,0 <x<2,0<y<3)、リチウムアルミニウムチタンホスフェート(Li x Al y Ti z (PO 4 ) 3 ,0 <x<2,0<y<1,0<z<3)、14Li 2 O-9Al 2 O 3 -38TiO 2 -39P 2 O 5 (LiAlTiP) x O y Glass (0 <x<4,0<y<13)、リチウムランタンチタネート(Li x La y TiO 3 ,0 <x<2,0<y<3)、Li3.25 Ge 0.25 P 0.75 S 4 such as lithium germanium thiophosphate (Li x Ge y P z S w , 0 < x < 4, 0 < y < 1, 0 < z < 1, 0 < w < 5), Li 3 nitrides such as Li x N y , 0 < x < 4, 0 < y < 2), Li 3 PO 4 -Li 2 S - SiS 2 such as SiS 2 -based glasses (Li x Si y S z , 0 < x < 3, 0 < y < 2, 0 < z < 4), LiI - Li 2 S - P 2 S 5 such as P 2 S 5 -based glasses (Li x P y S z , 0 < x < 3, 0 < y < 3, 0 < z < 7) or mixtures thereof, etc.

[0046] In one embodiment of the present invention, non-limiting examples of binder materials that can be used in the coating layer include polyvinylidene fluoride-co-hexafluoropropylene, polyvinylidene fluoride-co-trichloroethylene, polymethylmethacrylate, polybutylacrylate, polyacrylonitrile, polyvinylpyrrolidone, polyvinylacetate, ethylene-vinyl acetate, polyethylene oxide, and the like. Examples of the polymer resin include any one selected from the group consisting of polyvinyl alcohol, cyanoethyl cellulose, cyanoethyl sucrose, pullulan, and carboxyl methyl cellulose, or a mixture of two or more of these polymer resins. However, the polymer resin is not limited to these.

[0047] On the other hand, in a separator according to one embodiment of the present invention, the coating layer is defined into a first region and a second region, and the first region and the second region each independently contain inorganic particles and a binder material, and it may be preferable that the content ratio of the inorganic particles in the first region based on Formula 1 is higher than the content ratio of the inorganic particles in the second region based on Formula 2.

[0048] [Formula 1] Inorganic particle content ratio (wt%) of the first region = [amount of inorganic particles in the first region / (amount of inorganic particles in the first region + amount of binder material in the first region)] × 100 ... (1) [Formula 2] Inorganic particle content ratio (wt%) of the second region = [amount of inorganic particles in the second region / (amount of inorganic particles in the second region + amount of binder material in the second region)] × 100 ... (2)

[0049] 1 shows the shape of a separator 100 according to an embodiment of the present invention. Referring to the figure, a first region 121 having a high content ratio of inorganic particles is disposed, a part of a side surface of the first region is exposed to the outside, and second regions 122 having a low content ratio of inorganic particles are disposed on two opposing sides of the first region.

[0050] In this way, since the coating layer 120 has a first region and a second region, when the separator according to the present invention is used to manufacture an electrode, the first region promotes the flow of electrolyte into the interior of the battery, and at the same time, since the second region has a higher content of binder material than the first region, the second region can be used to achieve high adhesion between the separator and the electrode.

[0051] In one embodiment of the present invention, the content ratio of inorganic particles in the first region is higher than the content ratio of inorganic particles in the second region, and may be 70 wt% or more, 75 wt% or more, or 80 wt% or more. Meanwhile, the content of inorganic particles may be 90 wt% or less within the above range. Meanwhile, in a preferred embodiment of the present invention, the first region preferably has a binder resin content of more than 10 wt%. If the binder resin content is less than the above range, it is difficult to ensure adhesive strength between the separator and the electrode required to maintain the dimensional stability and durability of the electrode assembly. In one embodiment of the present invention, the content ratio of inorganic particles in the second region is lower than the content ratio of inorganic particles in the first region, and may be less than 90 wt%, 89 wt% or less, 85 wt% or less, 80 wt% or less, or 75 wt% or less. In one embodiment of the present invention, the content of the inorganic particles may be greater than 75 wt% in the first region and less than 75 wt% in the second region, or greater than 80 wt% in the first region and less than 80 wt% in the second region.

[0052] Meanwhile, in one embodiment of the present invention, the porosity may be higher as the content range of the inorganic particles increases, and thus the porosity of the first region may be higher than the porosity of the second region, while the air permeability (sec / 100cc) of the first region may be lower than that of the second region.

[0053] Next, various embodiments of the coating layer will be described by way of example, however, the embodiments provided are merely for the purpose of enhancing understanding of the present invention, and the scope of the present invention is not limited thereto.

[0054] In one embodiment of the present invention, the second region is preferably disposed in a portion of the periphery of the first region, and at least a portion of the side of the first region is exposed to the outside. The second region is disposed so as to be in contact with the boundary of the first region. In the separator according to the present invention, the first region is disposed in the coating layer to promote the flow of the electrolyte into the inside. The first region has a low content of binder resin and a high content of inorganic particles, and therefore has relatively low adhesion and cohesion with the electrode compared to the second region. In the case of the second region, the separator and the electrode show relatively higher adhesion compared to the first region, which may hinder the electrolyte from penetrating between them. For this reason, the electrolyte flows in through the first region relatively faster and easier than the electrolyte flows in through the second region. In the manufacture of the battery, the top and bottom surfaces of the separator are in contact with the electrodes, so the electrolyte flows in through the side of the separator. Therefore, when the entire area around the first region is surrounded by the second region, i.e., when the side surfaces of the first region are entirely covered by the second region, it is difficult to achieve the effect of promoting the flow of electrolyte.

[0055] In one embodiment of the present invention, the second region may be formed as a single, integrated region. In another embodiment, the second region may be divided into two or more units, and one of the units may be disposed apart from the remaining other unit. On the other hand, when the second region is divided into two or more units and a plurality of units are disposed, the units may be disposed apart from each other to ensure uniform adhesive strength with the electrodes throughout the separator.

[0056] In a specific embodiment of the present invention, the first region is disposed in a rectangular shape inside the surface of the polymer substrate, and the second region may have units disposed on one side of the first region and the other side opposite thereto, and the second region may not be disposed on the remaining two sides. When the second region is disposed in such a shape, the flow of the electrolyte is promoted through the side of the first region where the second region is not disposed, and the electrode and the separator can be bonded with high adhesive force at both ends in the width direction or both ends in the length direction of the separator. In one embodiment of the present invention, in consideration of the side of the electrolyte flow, when the separator is a rectangle with an aspect ratio of more than 1, the second region may be disposed on each of the two short sides of the separator, so that the long side of the separator is exposed. In one embodiment of the present invention, as described below, when the separator is manufactured, it is manufactured in a strip shape whose length in the MD direction is longer than that in the TD direction, so that the second region can be formed on the long side of the separator strip during the manufacturing process. However, the separator strip thus produced is cut to a predetermined width using a tool such as a cutter to obtain a separator, and the separator thus obtained is used to assemble a battery, so that a separator having a rectangular shape with a short MD direction and a long TD direction (during the manufacturing process) can be finally provided. In this case, the second region may be disposed on the short side of the separator thus produced.

[0057] FIG. 1 is a schematic diagram showing a separator according to an embodiment of the present invention. Referring to the figure, the first region is formed in a rectangular shape having four sides, and the second region is arranged in a portion of the periphery of the first region. More specifically, the second region is composed of two units, one of which is arranged so as to contact one side of the first region, and the other unit is arranged on the other side opposite to the first region. In addition, the side surfaces of the first region are exposed to the remaining two sides where the second region is not arranged.

[0058] 2 is a schematic diagram showing a method for producing a separator according to one embodiment of the present invention, which will be described with reference to the drawing.

[0059] The separator can be manufactured by a continuous process using a roll-to-roll method. Referring to FIG. 2, a long, rectangular polymer substrate 110 is continuously supplied by a traveling roll of a roll-to-roll device, and a slurry for forming a coating layer is applied to the surface of the polymer substrate. The application of the slurry can be performed by a typical application device 300 such as a slot die. Meanwhile, the slurry is divided into a slurry for forming a first region and a slurry for forming a second region, and each slurry can be prepared by adding inorganic particles and a binder material to an appropriate solvent.

[0060] Once each slurry is prepared, the slurry for forming the second region is applied to both ends of the width direction (TD direction) perpendicular to the running direction (MD direction) of the polymer substrate, and the slurry for forming the first region is applied to the portion between the second regions. The application of the slurries for forming the first and second regions may be performed simultaneously using a double slot die, or by applying the slurry for forming the first or second region and then sequentially applying the remaining slurries. For example, the slurry for forming the first region may be applied to a predetermined position on the inside of the polymer substrate, and the slurry for forming the second region may be applied to both ends of the width direction where the slurry for the first region has been applied continuously.

[0061] The applied slurry is then dried to obtain a separator strip including a composite coating layer having a first region and a second region. The drying can be performed by applying heat or air while passing through a dryer 500. The separator strip is then cut to a predetermined width using a tool such as a cutter 400 to obtain a separator, in which the side of the first region is exposed at both ends in the MD direction of the polymer substrate.

[0062] According to another aspect of the present invention, there is provided an electrochemical device, in which the above-mentioned separator for a lithium secondary battery is interposed between a positive electrode and a negative electrode.

[0063] In one embodiment of the present invention, the electrochemical device may be a lithium ion secondary battery.

[0064] In a specific embodiment of the present invention, the electrochemical device can be manufactured by injecting a non-aqueous electrolyte into an electrode assembly including a positive electrode, a negative electrode, and a separator interposed between the positive electrode and the negative electrode, in that order, as required. In this case, any of the positive electrode, negative electrode, and non-aqueous electrolyte that are commonly used in the manufacture of lithium secondary batteries can be used as the positive electrode, negative electrode, and non-aqueous electrolyte that constitute the electrode assembly.

[0065] In a specific embodiment of the present invention, the positive electrode may be manufactured by forming a positive electrode mixture layer on a positive electrode current collector, the positive electrode mixture layer being formed by coating a positive electrode slurry including a positive electrode active material, a binder, a conductive material, and a solvent on the positive electrode current collector, followed by drying and rolling.

[0066] In a specific embodiment of the present invention, the positive electrode current collector is not particularly limited as long as it does not cause a chemical change in the battery and has conductivity. For example, stainless steel, aluminum, nickel, titanium, baked carbon, or aluminum or stainless steel whose surface is treated with carbon, nickel, titanium, silver, or the like can be used.

[0067] In a specific embodiment of the present invention, the positive electrode active material may be a compound capable of reversible intercalation and deintercalation of lithium (lithiated intercalation compound (intercalation compound)).

[0068] In a specific embodiment of the present invention, the positive electrode active material may include, for example, lithium transition metal oxide; lithium metal iron phosphate; lithium nickel-manganese-cobalt oxide; an oxide in which a part of lithium nickel-manganese-cobalt oxide is replaced with another transition metal; or two or more of these, but is not limited thereto. Specifically, the positive electrode active material may include, for example, lithium cobalt oxide (LiCoO 2 ), lithium nickel oxide (LiNiO 2 ) and compounds substituted with one or more transition metals; 1+x Mn 2-x O 4 (where x is 0 to 0.33), LiMnO 3 , LiMn 2 O 3 , LiMnO 2 Lithium manganese oxides such as lithium copper oxide (Li 2 CuO 2 );LiV 3 O 8 , LiV 3 O 4 , V 2 O 5 , Cu 2 V 2 O 7 Vanadium oxides such as LiNi 1-x M x O 2 (wherein M=Co, Mn, Al, Cu, Fe, Mg, B or Ga, and x=0.01 to 0.3); Ni-site type lithium nickel oxide represented by the chemical formula LiMn 2-x M x O 2 (wherein M=Co, Ni, Fe, Cr, Zn or Ta, and x=0.01 to 0.1) or Li 2 Mn 3 MO 8 (wherein M is Fe, Co, Ni, Cu, or Zn); lithium metal phosphate LiMPO 4 (wherein M is Fe, CO, Ni, or Mn); lithium nickel-manganese-cobalt oxide Li1+x (Ni a Co b Mn c ) 1-x O 2 (x = 0 to 0.03, a = 0.3 to 0.95, b = 0.01 to 0.35, c = 0.01 to 0.5, a + b + c = 1); Oxide in which part of lithium nickel-manganese-cobalt oxide is substituted with aluminum Li a [Ni b Co c Mn d Al e ) 1-f M1 f O 2 (M1 is any one or more selected from the group consisting of Zr, B, W, Mg, Ce, Hf, Ta, La, Ti, Sr, Ba, F, P, and S, 0.8 ≤ a ≤ 1.2, 0.5 ≤ b ≤ 0.99, 0 < c < 0.5, 0 < d < 0.5, 0.01 ≤ e ≤ 0.1, 0 ≤ f ≤ 0.1); Oxide in which part of lithium nickel-manganese-cobalt oxide is substituted with other transition metals Li 1+x (Ni a Co b Mn c M d ) 1-x O 2 (x = 0 to 0.03, a = 0.3 to 0.95, b = 0.01 to 0.35, c = 0.01 to 0.5, d = 0.001 to 0.03, a + b + c + d = 1, M is any one selected from the group consisting of Fe, V, Cr, Ti, W, Ta, Mg, and Mo.). Disulfide compound; Fe 2 (MoO 4 ) 3 etc. are mentioned, but are not limited thereto at all.

[0069] In a specific embodiment of the present invention, the positive electrode may further include a conductive material. The conductive material may be porous. Therefore, the conductive material may be any material having porosity and conductivity, and may be, for example, a porous carbon-based material. Examples of such carbon-based materials include carbon black, graphite, graphene, activated carbon, carbon fiber, and carbon nanotubes (CNTs). In addition, examples of the conductive material include metallic conductive materials such as metal fibers and metal meshes; metallic powders such as copper, silver, nickel, and aluminum; and organic conductive materials such as polyphenylene derivatives. The conductive materials may be used alone or in combination.

[0070] In a specific embodiment of the present invention, the positive electrode may further include a binder. The binder may be a thermoplastic resin or a thermosetting resin. More specifically, examples of the binder include polyethylene, polypropylene, polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), styrene-butadiene rubber, tetrafluoroethylene-perfluoroalkyl vinyl ether copolymer, vinylidene fluoride-hexafluoropropylene copolymer, vinylidene fluoride-chlorotrifluoroethylene copolymer, ethylene-tetrafluoroethylene copolymer, polychlorotrifluoroethylene, vinylidene fluoride-pentafluoropropylene copolymer, propylene-tetrafluoroethylene copolymer, ethylene-chlorotrifluoroethylene copolymer, vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene copolymer, vinylidene fluoride-perfluoromethyl vinyl ether-tetrafluoroethylene copolymer, and ethylene-acrylic acid copolymer, which may be used alone or in combination, but are not necessarily limited to these. Any binder that can be used in the relevant technical field may be used.

[0071] In one specific embodiment of the present invention, the positive electrode active material may be included in an amount of 80 wt % to 99 wt % based on the total weight of solids in the positive electrode slurry.

[0072] In a specific embodiment of the present invention, the solvent used in the positive electrode slurry may include an organic solvent such as N-methyl-2-pyrrolidone (NMP), and may be used in an amount that provides a preferred viscosity when the positive electrode active material and, optionally, a binder and a conductive material are included. For example, the solvent may be included so that the solids concentration in the slurry containing the positive electrode active material and, optionally, a binder and a conductive material is 50 wt % to 95 wt %, preferably 70 wt % to 90 wt %.

[0073] In a specific embodiment of the present invention, the positive electrode can be manufactured by mixing a positive electrode active material, a selective conductive material (referred to as a conductive material), and a selective binder to prepare a composition for forming a positive electrode active material layer, applying the composition to at least one surface of the positive electrode current collector, drying, and rolling. As another method, the composition for forming a positive electrode active material layer can be cast on a separate support, and then peeled off from the support to obtain a film, which can be laminated on the positive electrode current collector.

[0074] In a specific embodiment of the present invention, the negative electrode may be manufactured by forming a negative electrode mixture layer on a negative electrode current collector, the negative electrode mixture layer being formed by coating a negative electrode slurry including a negative electrode active material, a binder, a conductive material, a solvent, etc., on the negative electrode current collector, followed by drying and rolling.

[0075] In a specific embodiment of the present invention, the negative electrode active material may include lithium metal, a carbon material capable of reversibly intercalating / deintercalating lithium ions, a metal or an alloy of these metals with lithium, a metal composite oxide, a material capable of doping and dedoping lithium, a transition metal oxide, or a mixture of two or more of these.

[0076] The carbonaceous material capable of reversibly intercalating / deintercalating lithium ions, which is an example of the negative electrode active material, may be any carbonaceous negative electrode active material commonly used in lithium ion secondary batteries, and representative examples thereof include crystalline carbon, amorphous carbon, or a combination of these. Examples of the crystalline carbon include graphite such as amorphous, plate-like, flake-like, spherical, or fibrous natural graphite or artificial graphite, and examples of the amorphous carbon include soft carbon (low-temperature calcined carbon), hard carbon, mesophase pitch carbide, and calcined coke.

[0077] As an example of the negative electrode active material, the metal or the alloy of these metals with lithium can be Cu, Ni, Na, K, Rb, Cs, Fr, Be, Mg, Ca, Sr, Si, Sb, Pb, In, Zn, Ba, Ra, Ge, Al, Sn, or a mixture of two or more of these metals or an alloy of these metals with lithium.

[0078] An example of the negative electrode active material is a metal composite oxide, such as 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 , 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, Group 1, Group 2, Group 3 elements of the periodic table, halogen; 0 < x ≤ 1; 1 ≤ y ≤ 3; 1 ≤ z ≤ 8), or a mixture of two or more of these can be used.

[0079] An example of the negative electrode active material, and substances capable of doping and undoping lithium include Si, SiO x (0 < x ≤ 2), Si-Y alloy (where Y is an alkali metal, alkaline earth metal, Group 13 element, Group 14 element, transition metal, rare earth element, a mixture of two or more of these, and not Si), Sn, SnO 2 , Sn-Y (where Y is an alkali metal, alkaline earth metal, Group 13 element, Group 14 element, transition metal, rare earth element, a mixture of two or more of these, and not Sn), etc., and at least one of these and SiO 2 can also be mixed and used. Examples of the element Y include Mg, Ca, Sr, Ba, Ra, Sc, Y, Ti, Zr, Hf, Rf, V, Nb, Ta, Db, Cr, Mo, W, Sg, Tc, Re, Bh, Fe, Pb, Ru, Os, Hs, Rh, Ir, Pd, Pt, Cu, Ag, Au, Zn, Cd, B, Al, Ga, Sn, In, Ti, Ge, P, As, Sb, Bi, S, Se, Te, Po, and a mixture of two or more of these.

[0080] An example of the negative electrode active material, and examples of the transition metal oxide include lithium-containing titanium composite oxide (LTO), vanadium oxide, lithium vanadate, etc.

[0081] In a specific embodiment of the present invention, the negative electrode active material may be contained at 80% to 99% by weight based on the total weight of the solid content in the negative electrode slurry.

[0082] In a specific embodiment of the present invention, the negative electrode may further include a binder. The binder is a component that assists in binding between the active material and the current collector, or between the active material, the conductive material, and the current collector, and is usually added in an amount of 1 to 30% by weight based on the total weight of the solid content in the negative electrode slurry. Examples of such binders include polyvinylidene fluoride (PVDF), polyvinyl alcohol, carboxymethyl cellulose (CMC), starch, hydroxypropyl cellulose, regenerated cellulose, polyvinylpyrrolidone, tetrafluoroethylene, polyethylene, polypropylene, ethylene-propylene-diene terpolymer (EPDM), sulfonated EPDM, styrene-butadiene rubber, fluororubber, and various copolymers thereof.

[0083] In a specific embodiment of the present invention, the negative electrode may further include a conductive material. The conductive material is a component for further improving the conductivity of the negative electrode active material, and when included, it can be added in an amount of 1 to 20% by weight based on the total weight of the solid content in the negative electrode slurry. As such a conductive material, the same or different conductive material used in the manufacture of the positive electrode can be used, and examples of such conductive materials include carbon powders such as carbon black, acetylene black (or denka black), ketjen black, channel black, furnace black, lamp black, and summer black; graphite powders such as natural graphite, artificial graphite, and graphite with highly developed crystal structures; conductive fibers such as carbon fibers and metal fibers; metal powders such as carbon fluoride, aluminum, and nickel powder; conductive whiskers such as zinc oxide and potassium titanate; conductive metal oxides such as titanium oxide; and conductive materials such as polyphenylene derivatives.

[0084] In a specific embodiment of the present invention, the solvent used in the negative electrode slurry may include water or an organic solvent such as NMP or alcohol, and may be used in an amount that provides a preferred viscosity when the negative electrode active material and, optionally, a binder and a conductive material are included. For example, the slurry may be included so that the solid content concentration in the slurry containing the negative electrode active material and, optionally, a binder and a conductive material is 50% by weight to 95% by weight, preferably 70% by weight to 90% by weight.

[0085] In a specific embodiment of the present invention, when a non-aqueous electrolyte is used, the non-aqueous electrolyte may include a lithium salt and an organic solvent, and may further include additives commonly used in the art.

[0086] In one specific embodiment of the present invention, the lithium salt has Li as a cation. + Contains F as an anion - , Cl - , Br - , I - , NO 3 - , N(CN) 2 - , ClO 4 - , B.F. 4 - , AlO 4 - , AlCl 4 - , P.F. 6 - , SbF 6 - , AsF 6 - , B.F. 2 C 2 O 4 - , B.C. 4 O 8 - , (CF 3 ) 2 PF 4 - , (CF 3 ) 3 PF 3 - , (CF 3 ) 4 PF2 - , (CF 3 ) 5 PF - , (CF 3 ) 6 P - , C.F. 3 SO 3 - , C 4 F 9 SO 3 - , C.F. 3 CF 2 SO 3 - , (CF 3 SO 2 ) 2 N - , (FSO 2 ) 2 N - , C.F. 3 CF 2 (CF 3 ) 2 CO - , (CF 3 SO 2 ) 2 CH - ,(SCIENCE FICTION 5 ) 3 C - , (CF 3 SO 2 ) 3 C - , C.F. 3 (CF 2 ) 7 SO 3 - , C.F. 3 CO 2 - , C.H. 3 CO 2 - , SCN - , (CF 3 CF 2 SO 2 ) 2 N - Or it may contain a mixture of two or more of these.

[0087] In a specific embodiment of the present invention, the lithium salt can be used alone or in combination of two or more kinds as necessary. The lithium salt can be appropriately changed within a range that is normally usable, but can be contained in the non-aqueous electrolyte at a concentration of 0.01M to 5M, 0.1M to 5M, or 0.1M to 3M.

[0088] In a specific embodiment of the present invention, the organic solvent is not particularly limited as long as it is capable of minimizing decomposition due to oxidation reactions or the like during charging and discharging of the secondary battery and exhibiting the desired properties together with the additives. For example, ether-based solvents, ester-based solvents, amide-based solvents, etc. can be used alone or in combination of two or more.

[0089] In a specific embodiment of the present invention, the ether-based solvent among the organic solvents may be, but is not limited to, dimethyl ether, diethyl ether, dipropyl ether, methyl ethyl ether, methyl propyl ether, ethyl propyl ether, or a mixture of two or more thereof.

[0090] In a specific embodiment of the present invention, the ester solvent may include a cyclic carbonate compound, a linear carbonate compound, a linear ester compound, a cyclic ester compound, or a mixture of two or more thereof.

[0091] In one specific embodiment of the present invention, specific examples of the cyclic carbonate compound include ethylene carbonate (EC), propylene carbonate (PC), 1,2-butylene carbonate, 2,3-butylene carbonate, 1,2-pentylene carbonate, 2,3-pentylene carbonate, vinylene carbonate, fluoroethylene carbonate (FEC), or a mixture of two or more of these.

[0092] In one embodiment of the present invention, typical examples of the linear carbonate compound that can be used include, but are not limited to, dimethyl carbonate (DMC), diethyl carbonate (DEC), dipropyl carbonate, ethyl methyl carbonate (EMC), methyl propyl carbonate, ethyl propyl carbonate, or a mixture of two or more of these.

[0093] In one specific embodiment of the present invention, the linear ester compound may be, for example, methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate, propyl propionate, butyl propionate, or a mixture of two or more of these, but is not limited thereto.

[0094] In a specific embodiment of the present invention, the cyclic ester compound may be, for example, γ-butyrolactone, γ-valerolactone, γ-caprolactone, σ-valerolactone, ε-caprolactone, or a mixture of two or more of these, but is not limited thereto.

[0095] In a specific embodiment of the present invention, the cyclic carbonate-based compound is a high-viscosity organic solvent with a high dielectric constant, which sufficiently dissociates the lithium salt in the electrolyte. Therefore, by mixing such a cyclic carbonate-based compound with a linear carbonate-based compound and a linear ester-based compound having a low viscosity and a low dielectric constant, such as dimethyl carbonate and diethyl carbonate, in an appropriate ratio, a non-aqueous electrolyte solution having high electrical conductivity can be produced.

[0096] The separator for a lithium secondary battery according to one aspect of the present invention can effectively transfer lithium ions, reduce side reactions at the interface between the separator for a lithium secondary battery containing an ion-conductive polymer material and an electrode, and significantly reduce the increase rate of the initial resistance inside the battery. As a result, a battery using the separator can improve the output density characteristics of the battery and improve the rate characteristics with a reduced irreversible capacity, thereby shortening the time required for charging or discharging the battery and improving the charge and discharge life. Therefore, the separator can be suitably used in portable devices such as mobile phones, notebook computers, digital cameras, and camcorders that require a high charging speed, electric vehicles such as hybrid electric vehicles (HEVs) and plug-in hybrid electric vehicles (PHEVs), and medium- and large-sized energy storage systems.

[0097] In order to deepen understanding of the contents of the present invention, examples, comparative examples and experimental examples are presented below. However, the following test examples are merely test examples relating to the configuration and effects of the present invention, and the scope and effects of the present invention are not limited to these.

[0098] Example: Manufacture of separator [Example 1] Polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP) (molecular weight (Mw) 500,000 g / mol, HFP content 15 wt%) and alumina (particle size 0.5 μm) were added to acetone in a weight ratio of 22.5:77.5 to prepare a slurry for forming the first region with a solid content of 20 wt%.

[0099] Next, PVDF-HFP (molecular weight (Mw) 500,000 g / mol, HFP content 15 wt%) and alumina (particle size 0.5 μm) were added to acetone in a weight ratio of 25:75 to prepare a slurry for forming a second region with a solid content of 20 wt%.

[0100] A polymer film made of polyethylene (film thickness 9 μm, porosity 45 vol%, ventilation time 60 sec / 100 cc) was prepared, and the slurries for forming the first and second regions were applied in that order as shown in Figure 1. The film was then dried under humidified conditions at 23°C and a relative humidity of 45% to obtain a separator.

[0101] [Example 2] PVDF-HFP (molecular weight (Mw) 500,000 g / mol, HFP content 15 wt%) and alumina (particle size 0.5 μm) were added to acetone in a weight ratio of 20:80 to prepare a slurry for forming a first region with a solid content of 20 wt%.

[0102] Next, PVDF-HFP (molecular weight (Mw) 500,000 g / mol, HFP content 15 wt%) and alumina (particle size 0.5 μm) were added to acetone in a weight ratio of 25:75 to prepare a slurry for forming a second region with a solid content of 20 wt%.

[0103] A polymer film made of polyethylene (film thickness 9 μm, porosity 45 vol%, ventilation time 60 sec / 100 cc) was prepared, and the slurries for forming the first and second regions were applied in that order as shown in Figure 1. The film was then dried under humidified conditions at 23°C and a relative humidity of 45% to obtain a separator.

[0104] [Comparative Example 1] PVDF-HFP (molecular weight (Mw) 500,000 g / mol, HFP content 15 wt%) and alumina (particle size 0.5 μm) were added to acetone in a weight ratio of 25:75 to prepare a slurry for forming a coating layer with a solid content of 20 wt%.

[0105] A polyethylene polymer film (film thickness 9 μm, porosity 45 vol%, ventilation time 60 sec / 100 cc) was prepared, the slurry was applied, and the film was dried under humidified conditions of 23° C. and relative humidity 45% to obtain a separator.

[0106] Experimental example: Evaluation of separator properties The physical properties of the separator produced above were evaluated according to the following evaluation methods, and the results are shown in Table 1 below and in FIGS. [Evaluation Results]

[0107] [Table 1]

[0108] [Evaluation method] 1. Ventilation time The air permeability of the separator was measured using an air permeability meter (EGO-IT, manufactured by Asahi Seiko Co., Ltd.) in accordance with JIS P8117. On the other hand, in order to measure the air permeability of each of the first and second regions, after the separator was produced, a knife was used to divide the first and second regions to obtain a sample for measuring the air permeability time.

[0109] 2. Electrode adhesion strength The active material [natural graphite and artificial graphite (weight ratio 5:5)], conductive material [Super P], and binder [polyvinylidene fluoride (PVDF)] were mixed in a weight ratio of 92:2:6, dispersed in water, and then coated onto copper foil with a width of 250 mm to produce the negative electrode.

[0110] Separators were produced and prepared according to Examples 1 and 2 and Comparative Example 1. The prepared separator was divided into a first region and a second region using a knife.

[0111] The prepared separator and negative electrode were stacked, sandwiched between 100 μm PET films, and then laminated using a roll lamination machine under the conditions of 60° C., a pressure of 2.4 kgf / mm, and a speed of 5 m / min.

[0112] The bonded separator and negative electrode were cut to a size of 25 mm wide and 70 mm long, and the ends of the separator and negative electrode were attached to a universal material testing machine (Instron Corporation). A force was then applied at 180° at a measurement speed of 300 mm / min to measure the force required to peel off the negative electrode and the separator attached to the negative electrode.

[0113] 3. Check the wettability of the electrolyte (1) Manufacturing of negative electrodes Anode slurry was prepared by mixing artificial graphite as anode active material, carbon black as a conductive material, carboxymethyl cellulose (CMC) as a dispersant, and styrene-butadiene rubber (SBR, Zeon Corporation BM-L301) as a binder with water in a weight ratio of 95.8:1:1.2:2. The anode slurry was coated on copper foil (Cu-foil) to a thickness of 50 μm to form a thin electrode plate, which was then dried at 135° C. for 3 hours or more and pressed to prepare anode.

[0114] (2) Manufacturing of positive electrodes LiCoO as a positive electrode active material 2 A positive electrode slurry was prepared by mixing carbon black as a conductive material, polyvinylidene fluoride (PVDF) as a binder with N-methyl-2-pyrrolidone (NMP) in a weight ratio of 98:1:1. The positive electrode slurry was coated on an aluminum foil to a thickness of 20 μm to form a thin electrode plate, which was then dried at 135° C. for 3 hours or more and pressed to prepare a positive electrode.

[0115] (3) Manufacture of lithium secondary batteries Next, the prepared separator was sandwiched between the negative electrode and the positive electrode, and then stacked to prepare a stack-type electrode assembly, which was then inserted into a pouch exterior material, and 1M LiPF was dissolved in a solvent in which ethylene carbonate (EC) and diethyl carbonate (DEC) were mixed in a volume ratio of 30:70. 6 An electrolyte solution in which the above was dissolved was injected to prepare a lithium secondary battery.

[0116] The secondary battery manufactured as described above was disassembled at SOC 60, and the negative electrode surface was observed to check wetting. When wetting was good, the entire surface of the negative electrode showed a uniform charged state (FIGS. 3 and 4), but when wetting was poor, uncharged dark areas were observed on the negative electrode surface (FIG. 5).

[0117] Although the present invention has been described above using limited embodiments and drawings, the present invention is not limited thereto, and it goes without saying that various modifications and variations can be made by a person having ordinary knowledge in the technical field to which the present invention pertains within the scope of the technical concept of the present invention and the scope of the claims. [Explanation of symbols]

[0118] 100…Separator 110...Polymer base material 120...Organic / inorganic composite coating layer 121…First Area 122...Second Area 300... Coating device 500...Dryer 400…Cutter

Claims

1. The present invention includes a porous polymer substrate and a porous organic / inorganic composite coating layer formed on both surfaces or on at least one surface of the polymer substrate, The organic / inorganic composite coating layer is defined into a first region and a second region, The first region and the second region each independently contain inorganic particles and a binder material, and the content ratio of the inorganic particles in the first region based on the following formula 1 is higher than the content ratio of the inorganic particles in the second region based on the following formula 2: A separator for an electrochemical element, wherein the porosity of the first region in the coating layer is higher than the porosity of the second region. [Formula 1] Inorganic particle content ratio (wt%) of the first region = [amount of inorganic particles in the first region / (amount of inorganic particles in the first region + amount of binder material in the first region)] × 100 ... (1) [Formula 2] Content ratio (wt%) of inorganic particles in the second region = [amount of inorganic particles in the second region / (amount of inorganic particles in the second region + amount of binder material in the second region)] × 100 ... (2)

2. 2. The separator for an electrochemical element according to claim 1, wherein a content ratio of the inorganic particles in the first region is higher than that in the second region and is 70 wt % or more and 90 wt % or less.

3. 2. The separator for an electrochemical element according to claim 1, wherein a content ratio of inorganic particles in the second region is lower than that in the first region and is 85 wt % or less.

4. 2. The separator for electrochemical elements according to claim 1, wherein the second region is disposed in a section around the first region such that at least a portion of a side surface of the first region is exposed to the outside, and the second region is disposed so as to be in contact with a boundary of the first region.

5. 5. The separator for an electrochemical element according to claim 4, wherein the second region is an integral single region or is divided into two or more units, any one of the units being disposed apart from the other units.

6. 5. The separator for electrochemical elements according to claim 4, wherein the first region is arranged in a rectangular shape on the inside of a surface of the polymer substrate, and the second region has units arranged on one side of the first region and on another side opposite thereto, and no second region is arranged on the remaining two sides.

7. 6. The separator for an electrochemical element according to claim 5, wherein the separator is a rectangle having an aspect ratio of greater than 1, and the second regions are disposed on each of two shorter sides of the separator.

8. The battery includes an electrode assembly including a positive electrode, a negative electrode, and a separator sandwiched between the positive electrode and the negative electrode, An electrochemical element, wherein the separator is the separator according to any one of claims 1 to 7.

9. The electrochemical device according to claim 8 , wherein the electrochemical device is a lithium ion secondary battery.

10. A method for producing the separator according to any one of claims 1 to 7, comprising the steps of: The method is carried out by a roll-to-roll process in which a long, rectangular polymer substrate is continuously supplied, A method for producing a separator for an electrochemical element, comprising the steps of forming second regions having a predetermined width on both ends of the polymer substrate in a width direction (TD direction) perpendicular to the running direction (MD direction), and forming a first region between the second regions to obtain a separator strip including a composite coating layer having a first region and a second region.

11. The method for manufacturing a separator for an electrochemical element according to claim 10, wherein the formation of the first region and the second region is performed by applying slurries for forming the first region and the second region to the defined portions, respectively, using a double slot die.

12. 11. The method for manufacturing a separator for an electrochemical element according to claim 10, wherein the separator strip is cut to a predetermined width to obtain a separator, and side surfaces of the first region are exposed at both ends in an MD direction of the polymer substrate.

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