JP5515267B2 - Nonaqueous electrolyte secondary battery - Google Patents

Description

  The present invention relates to a non-aqueous electrolyte secondary battery. More specifically, the present invention relates to a non-aqueous electrolyte secondary battery with vehicle mounting in mind.

  In recent years, in order to cope with air pollution and global warming, reduction of the amount of carbon dioxide has been strongly desired. In the automobile industry, there is a great expectation for reducing carbon dioxide emissions by introducing electric vehicles (EV) and hybrid electric vehicles (HEV), and the development of secondary batteries for motor drive that holds the key to commercialization of these is thriving. Has been done.

  As a secondary battery for driving a motor, a non-aqueous electrolyte secondary battery having the highest theoretical energy among all the batteries is attracting attention, and is currently being developed rapidly. A non-aqueous electrolyte secondary battery represented by a lithium ion secondary battery generally has a positive electrode in which a positive electrode active material or the like is applied to both surfaces of a positive electrode current collector using a binder, and a negative electrode active material or the like using a binder. Negative electrodes applied to both sides of the current collector are connected via an electrolyte layer. And it has the structure accommodated in a battery case.

  The non-aqueous electrolyte secondary battery used as a motor drive power source for automobiles and the like as described above has extremely high output characteristics compared to consumer non-aqueous electrolyte secondary batteries used in mobile phones, notebook computers, etc. It is required to have. At present, research and development is underway to meet such demands.

  By the way, in a non-aqueous electrolyte secondary battery, particularly a lithium ion secondary battery, lithium generated by charging may react with an organic solvent of the electrolytic solution, or precipitated lithium may grow in a dendrite shape. Then, when lithium without electron conductivity is generated, there is a possibility that the charging / discharging efficiency of the lithium ion secondary battery is reduced, or the battery is short-circuited due to lithium grown in a dendrite shape from the negative electrode.

  The generation of lithium dendrite has a correlation with the charging current density and is caused by the localization of the reaction (concentration of current density). Such generation of dendrite of the lithium negative electrode appears remarkably in the peripheral portion of the negative electrode.

As means for solving such a problem, a battery composed of a plurality of opposing positive electrodes, lithium negative electrodes, and an organic electrolyte, which are alternately inserted into a rectangular battery case, is disclosed (Patent Document 1). Here, the prismatic lithium secondary battery has a structure in which the area of each negative electrode is larger than the area of the opposing positive electrode, and the peripheral edge of the negative electrode is outside the peripheral edge of the opposing positive electrode.
Japanese Patent Laid-Open No. 3-152881

  However, according to the square lithium secondary battery in such a means, since the areas of the negative electrode and the positive electrode are different, there is a problem in the strength of the edge portion when they are combined to form a battery. And the problem appears notably when many layers of a battery are laminated | stacked.

  Therefore, the problem to be solved by the present invention is to improve the mechanical strength of the battery while significantly preventing dendrite in the nonaqueous electrolyte secondary battery.

  A non-aqueous resin formed by forming a non-ion permeable resin part on the outer peripheral edge of the positive electrode active material layer or the negative electrode active material layer so that the region of the electrode reaction part is smaller or coincides with the positive electrode than the negative electrode It has been found that the above problem can be solved by providing an electrolyte secondary battery.

  According to the present invention, in order to provide a non-aqueous electrolyte secondary battery formed with a specific non-ion permeable resin part, it is possible to significantly prevent concentration of current density at the peripheral part of the negative electrode and to prevent dendrite significantly. can do.

  Hereinafter, the nonaqueous electrolyte secondary battery of the present invention will be described in detail with reference to the drawings as appropriate. Each drawing is exaggerated for convenience of explanation, and the dimensional ratio of each component in each drawing may be different from the actual one.

  The type of the battery of the present invention is not particularly limited. However, when the non-aqueous electrolyte secondary battery is distinguished by its form and structure, a conventional battery such as a stacked (flat) battery or a wound (cylindrical) battery has been used. It can be applied to any known form / structure. In addition, when viewed in terms of the electrical connection configuration (electrode structure) in the non-aqueous electrolyte secondary battery, both the above-described non-bipolar (internal parallel connection type) battery and bipolar (internal series connection type) battery It can be applied. In the bipolar battery, a single cell voltage is higher than that of a normal battery, and a battery excellent in capacity and output characteristics can be configured. In addition, by adopting a laminated (flat) battery structure, long-term reliability can be secured by a sealing technique such as simple thermocompression bonding, which is advantageous in terms of cost and workability.

<Battery configuration>
[Non-bipolar non-aqueous electrolyte secondary battery]
FIG. 1 shows a schematic cross-sectional view of a flat (stacked) non-bipolar non-aqueous electrolyte secondary battery. In the flat (laminated) nonaqueous electrolyte secondary battery 1 (laminated battery 1) shown in FIG. 1, a laminated film in which a polymer-metal composite is combined with a battery exterior material 12 is used. Then, the entire peripheral portion is joined by heat fusion. In the nonaqueous electrolyte secondary battery 1, a plurality of single battery layers having a positive electrode (positive electrode plate), an electrolyte layer 15, and a negative electrode (negative electrode plate) are stacked. In the positive electrode, positive electrode active material layers 14 are formed on both surfaces of a first current collector (hereinafter also referred to as “positive electrode current collector”) 13 (one side for the lowermost layer and the uppermost layer of the power generation element). In the negative electrode, a negative electrode active material layer 17 is formed on both surfaces of the second current collector (hereinafter also referred to as “negative electrode current collector”) 16 (one side for the lowermost layer and the uppermost layer of the power generation element).

  In the non-aqueous electrolyte secondary battery 1 of the present application, at least one of the positive electrode active material layer 14 and the negative electrode active material layer 17 includes an electrode reaction part (not shown) effective for an electrochemical reaction, and a non-ion permeable resin. And a resin infiltration portion (not shown) formed by infiltrating the resin. And in the nonaqueous electrolyte secondary battery 1 of this application, the said resin penetration part is arrange | positioned in the surface direction of the said positive electrode active material layer 14 or the said negative electrode active material layer 17, and the outer periphery of the said electrode reaction part. Furthermore, in the nonaqueous electrolyte secondary battery 1 of the present application, the outer peripheral edge of the electrode reaction portion in the positive electrode active material layer 14 is aligned or inward with respect to the outer peripheral edge of the electrode reaction portion in the negative electrode active material layer 17. Be located.

  The nonaqueous electrolyte secondary battery 1 has a configuration in which a power generation element 18 in which these are stacked is housed and sealed. Further, the positive electrode (terminal) lead 19 and the negative electrode (terminal) lead 10 that are electrically connected to the electrodes (positive electrode and negative electrode) are ultrasonically applied to the first current collector 13 and the second current collector 16 of each electrode plate. It is attached by welding or resistance welding. Thus, it has the structure which is pinched | interposed into the said heat sealing | fusion part and exposed to the exterior of said battery exterior material 12. FIG.

[Bipolar non-aqueous electrolyte secondary battery]
FIG. 2 is a schematic cross-sectional view of a bipolar nonaqueous electrolyte secondary battery (also simply referred to as a bipolar battery).

  The bipolar battery 2 shown in FIG. 2 has a structure in which a substantially rectangular battery element 21 in which a charge / discharge reaction actually proceeds is sealed inside a laminate sheet 29 that is an exterior.

  As shown in FIG. 2, the battery element 21 of the bipolar battery 2 of the present embodiment includes a positive electrode active material layer 22 and a negative electrode active material layer 23 as current collectors (first current collector and second current collector). A plurality of bipolar electrodes (not shown) formed on each surface of 24. Each bipolar electrode is stacked via an electrolyte layer 25 to form a battery element 21. At this time, each bipolar type is formed such that the positive electrode active material layer 22 of one bipolar electrode and the negative electrode active material layer 23 of another bipolar electrode adjacent to the one bipolar electrode face each other through the electrolyte layer 25. An electrode and an electrolyte layer 25 are laminated.

  The adjacent positive electrode active material layer 22, electrolyte layer 25, and negative electrode active material layer 23 constitute one unit cell layer 26. Therefore, it can be said that the bipolar battery 2 has a configuration in which the single battery layers 26 are stacked. In addition, an insulating layer 27 for insulating the adjacent current collectors 24 is provided on the outer periphery of the unit cell layer 26. The current collector (outermost layer current collector) (24a, 24b) located in the outermost layer of the battery element 21 has a positive electrode active material layer 22 (positive electrode side outermost layer current collector 24a) or a negative electrode only on one side. One of the active material layers 23 (the negative electrode side outermost layer current collector 24b) is formed.

  Current collector plates 24a 'and 24b' are provided on the outer sides of the outermost layer current collectors 24a and 24b. The current collector plates 24a 'and 24b' are extended to form a negative electrode tab 28b and a positive electrode tab 28a, respectively. Further, the current collector plates 24a 'and 24b' are formed thicker than the current collector so that the current from the plurality of stacked unit cell layers 26 can be easily taken out.

  And the electric power generation element 21 is sealed in the exterior material which consists of the laminate sheet 29 so that these positive electrode tabs 28a and negative electrode tabs 28b may lead out outside.

  Instead of the current collector plate, the outermost layer current collectors 24a and 24b may be electrically connected to the positive electrode tab 28a and the negative electrode tab 28b as they are. At this time, the outermost layer current collector (24a, 24b) and the tab (28a, 28b) may be electrically connected via a positive terminal lead and a negative terminal lead. Further, instead of the current collector plate, the outermost layer current collectors 24a and 24b may be thickened and directly extended outside the laminate sheet 29 to form the negative electrode tab 28b and the positive electrode tab 28a. Further, an electrode active material layer may be provided between the outermost layer current collectors 24a and 24b and the current collector plates 24a 'and 24b'. That is, the current collectors 24a ′ and 24b ′ dedicated to the outermost layer provided with the electrode active material only on one side are used as the current collector of the outermost layer as it is, instead of the current collector having the electrode active material on both sides. It is good.

  In the bipolar battery 2 of the present application, at least one of the positive electrode active material layer 22 and the negative electrode active material layer 23 is infiltrated with an electrode reaction part (not shown) effective for an electrochemical reaction and a non-ion permeable resin. And a resin permeation portion (not shown) formed. In the bipolar battery 2 of the present application, the resin permeation portion is disposed on the outer periphery of the electrode reaction portion in the surface direction of the positive electrode active material layer 22 or the negative electrode active material layer 23.

  Furthermore, in the bipolar battery 2 of the present application, the outer peripheral edge of the electrode reaction portion in the positive electrode active material layer 22 is positioned inward or inward with respect to the outer peripheral edge of the electrode reaction portion in the negative electrode active material layer 23. Become. The basic configuration of the bipolar battery 2 can be said to be a configuration in which a plurality of stacked single battery layers (single cells) are connected in series.

  The non-aqueous electrolyte secondary battery is particularly preferably a lithium ion secondary battery. Further, in the present specification, the “non-aqueous electrolyte secondary battery” may be simply referred to as “battery”.

  As described above, the technique described in Patent Document 1 is disclosed as a means for solving the problem of dendrite generation due to reaction localization (concentration of current density). In addition, in order to solve the problem that dendrites are generated, for example, it is conceivable to seal the periphery of the positive electrode with an insulative material that is insoluble in the electrolytic solution. However, the problem that the filling capacity is reduced and the adhesion strength of the peripheral edge of the positive electrode plate are not necessarily sufficient, and an internal short circuit may occur due to the dropping of the positive electrode mixture during the charge / discharge cycle.

  Furthermore, in the non-aqueous electrolyte secondary battery, it is conceivable to close the micropores in the portion facing the negative electrode peripheral portion of the separator. However, since the area where the negative electrode and the positive electrode face each other is determined by the area where the separator is not blocked, there is a problem that the designed capacity and the actual capacity are different. In particular, when the micropores are blocked only by the thermal fusion process after laminating the negative electrode, the separator, and the positive electrode, there is a possibility that the negative electrode and the positive electrode are short-circuited at the electrode end.

  In order to solve the above problems, the present invention provides a positive electrode active material layer formed on at least one surface of a first current collector and a negative electrode formed on at least the other surface of the second current collector. An active material layer is a non-aqueous electrolyte secondary battery including a power generation element in which a plurality of unit cell layers are stacked with an electrolyte layer interposed therebetween, wherein the positive electrode active material layer and the negative electrode active material layer At least one comprises an electrode reaction part effective for an electrochemical reaction and a resin infiltration part formed by infiltrating a non-ion permeable resin, and the resin infiltration part is the positive electrode active material layer or the negative electrode active part. The outer peripheral edge of the electrode reaction part in the positive electrode active material layer is aligned or inward with respect to the outer peripheral edge of the electrode reaction part in the negative electrode active material layer. Non-aqueous electrolyte secondary located in To provide a pond.

  Furthermore, in general, when a battery is charged, the positive electrode has a higher potential than the negative electrode, and the current collector used for the positive electrode dissolves or an oxidation reaction occurs in the electrolyte. A reduction reaction occurs. In this way, the negative electrode is generally easily deteriorated, and when the negative electrode is corroded, the positional relationship between the positive electrode and the negative electrode (strictly speaking, The positional relationship between the positive electrode active material layer and the negative electrode active material layer) changes. That is, since the negative electrode is inclined in a direction smaller than the positive electrode, dendrite is generated as a result.

  According to the present invention, even if the positive electrode active material layer and the negative electrode active material layer have the same size at the battery design stage, the non-ion permeable resin is infiltrated, and the resin infiltration portion (not effective for electrochemical reaction) The formation of the portion effective for the electrochemical reaction can be controlled. Therefore, the generation of dendrite can be easily suppressed / prevented.

  As described above, in the nonaqueous electrolyte secondary battery of the present application, at least one of the positive electrode active material layer and the negative electrode active material layer has an electrode reaction portion effective for an electrochemical reaction and a non-ion permeable resin infiltrated. And a resin permeation portion to be formed.

  In the non-aqueous electrolyte secondary battery of the present application, the resin permeation portion is formed in the surface direction of the positive electrode active material layer or the negative electrode active material layer (hereinafter also simply referred to as “active material layer”). It is arranged on the outer periphery. And in the nonaqueous electrolyte secondary battery of the present application, the outer peripheral edge of the electrode reaction part (hereinafter also referred to as “positive electrode reaction part”) in the positive electrode active material layer is the electrode reaction part (hereinafter, referred to as “positive electrode reaction part”). It is also coincident or inward with respect to the outer peripheral edge of the “negative electrode reaction part”. It is derived from the structure of such a nonaqueous electrolyte secondary battery, and dendrite can be suppressed / prevented.

  Subsequently, in order to make it easier to understand the positional relationship (coincidence or inward) between the outer peripheral edge of the positive electrode reaction part and the outer peripheral edge of the negative electrode reaction part, a description will be given with reference to FIG.

  FIG. 3 is a perspective view schematically showing a case where the positive electrode reaction part is projected. As shown in FIG. 3, it can be seen that when the positive electrode reaction part is vertically irradiated with virtual light, the outer peripheral edge of the positive electrode reaction part is projected onto the surface of the negative electrode reaction part. In other words, “the outer peripheral edge of the electrode reaction part in the positive electrode active material layer is aligned or inward with respect to the outer peripheral edge of the electrode reaction part in the negative electrode active material layer” is as follows. That is, it means that the projected outer peripheral edge of the positive electrode reaction part coincides with the outer peripheral edge of the negative electrode reaction part or is located inward from the outer peripheral edge of the negative electrode reaction part.

  That is, in the nonaqueous electrolyte secondary battery of the present invention, the outer peripheral edge (edge) of the reaction part of each electrode facing the other electrode is formed in a predetermined positional relationship.

  Thus, dendrite can be significantly suppressed / prevented by making the portion effective for the electrochemical reaction in the positive electrode active material layer smaller than the portion effective for the electrochemical reaction in the negative electrode active material layer.

  The resin permeation portion may be formed in at least one of the positive electrode active material layer and the negative electrode active material layer, more preferably formed in at least the positive electrode active material layer, and more preferably in the positive electrode active material layer. Only formed.

  Each component will be described below in summary. However, in addition to the features described above, conventionally known knowledge can be appropriately referred to or applied in combination as long as it has ordinary knowledge in the field. it can.

<Positive electrode / Negative electrode>
The positive electrode and the negative electrode are collectively referred to as a battery electrode. The positive electrode includes a first current collector (positive electrode current collector) and a positive electrode active material layer formed on the current collector. The negative electrode is composed of a second current collector (negative electrode current collector) and a negative electrode active material layer formed on the current collector.

[Current collector]
The current collector that can be used in the present invention (simply referred to as “current collector” is at least one of the first current collector and the second current collector) is not particularly limited. In addition, conventionally known ones can be used. For example, aluminum foil, stainless steel (SUS) foil, nickel-aluminum clad material, copper-aluminum clad material, SUS-aluminum clad material, or a plated material of a combination of these metals can be preferably used. Further, a current collector in which a metal surface is coated with aluminum may be used. In some cases, a current collector in which two or more metal foils are bonded together may be used (composite current collector).

  When the composite current collector is used, as a material for the first current collector, for example, a conductive metal such as aluminum, an aluminum alloy, SUS, or titanium can be used, but aluminum is particularly preferable. On the other hand, as the material of the second current collector, for example, conductive metals such as copper, nickel, silver, and SUS can be used, and SUS and nickel are particularly preferable. Further, in the composite current collector, the first current collector and the second current collector may be electrically connected to each other directly or via a conductive intermediate layer made of a third material. . Further, the first current collector and the second current collector may be used as one current collector for a bipolar nonaqueous electrolyte secondary battery.

  Although the thickness of a collector is not specifically limited, Preferably it is 10-20 micrometers. However, a current collector having a thickness outside this range may be used.

  The shape of the current collector is not particularly limited, but is preferably a rectangle such as a square or a rectangle.

[Positive electrode active material layer / Negative electrode active material layer]
The positive electrode active material layer includes a positive electrode active material. In addition, other positive electrode materials include electrolytes such as conductive additives, binders, electrolytes (electrolyte support salts and plasticizers), polymer gels or solid electrolytes (ionic conductive polymers, electrolytes, etc.). It is done. Further, when a host polymer is included, it may further include a polymerization initiator for polymerizing the polymer.

  Although there is no restriction | limiting in particular also in the thickness of a positive electrode active material layer, Preferably they are 1 micrometer-300 micrometers, More preferably, they are 5 micrometers-200 micrometers, More preferably, they are 10 micrometers-150 micrometers. A method for controlling the thickness of the positive electrode active material layer is not particularly limited, and examples thereof include a doctor blade method. In addition, various methods can be considered as a method for quantitatively obtaining the thickness of the positive electrode active material layer. For example, the thickness can be obtained by measuring with a micrometer or measuring the film thickness using radiation. .

  Moreover, there is no restriction | limiting in particular also in the shape of a positive electrode active material layer, Although it designs suitably according to the shape of a collector, Preferably it is a rectangle like a square or a rectangle.

  The negative electrode active material layer includes a negative electrode active material. In addition to this, other negative electrode materials may include those described as the positive electrode material.

  Hereinafter, the positive electrode active material and the negative electrode active material are also collectively referred to as “active material”.

  A resin infiltrating portion into which a non-ion permeable resin has permeated is formed on the outer peripheral portion of at least one of the positive electrode active material layer and the negative electrode active material layer. The non-ion permeable resin that permeates the positive electrode active material layer is referred to as “first non-ion permeable resin” for convenience, and the non-ion permeable resin that permeates the negative electrode active material layer is referred to as “second non-ion permeation” for convenience. May also be referred to as a “resin”. In addition, when only calling it "non-ion permeable resin", it is at least one of the first non-ion permeable resin and the second non-ion permeable resin.

  Although there is no restriction | limiting in particular also in the thickness of a negative electrode active material layer, Preferably they are 1 micrometer-300 micrometers, More preferably, they are 5 micrometers-200 micrometers, More preferably, they are 10 micrometers-150 micrometers. A method for controlling the thickness of the negative electrode active material layer is not particularly limited, but a method for controlling the positive electrode active material layer is equally applicable.

  The shape of the negative electrode active material layer is not particularly limited and is appropriately designed according to the shape of the current collector, but is preferably a rectangle such as a square or a rectangle.

(Electrode reaction part / resin permeation part)
At least one of the positive electrode active material layer and the negative electrode active material layer includes an electrode reaction portion effective for an electrochemical reaction and a resin infiltration portion formed by infiltrating a non-ion permeable resin. The resin penetration portion is preferably formed at least in the positive electrode active material layer, and more preferably formed only in the positive electrode active material layer.

  Here, the “electrode reaction part effective for electrochemical reaction” means that the non-ion-permeable resin does not penetrate, that is, has the same ionic conductivity as the active material layer where the resin penetration part is not formed. Say that part.

  On the other hand, the “resin permeation portion formed by infiltrating a non-ion permeable resin” refers to a portion where the non-ion permeable resin is formed in the active material layer. Such a resin penetration part functions as a part which is not effective in an electrochemical reaction among active material layers. That is, the “resin permeation portion” refers to a portion of the active material layer that is lower than the ionic conductivity of the active material layer where the resin permeation portion is not formed. The ionic conductivity of the “resin-penetrating part” should be lower than the ionic conductivity of the active material layer where the resin-penetrating part is not formed, but preferably the ionic conductivity of the active material layer where the resin-penetrating part is not formed 0.01 to 0.5 times, more preferably 0.05 to 0.1 times.

  In summary, in the active material layer, a portion other than the “resin permeation portion formed by permeating the non-ion permeable resin” functions as an “electrode reaction portion effective for electrochemical reaction”. In other words, the boundary between the electrode reaction part and the resin infiltration part can be said to be the outer peripheral edge of the electrode reaction part.

  In addition, although the method in particular of calculating | requiring ionic conductivity is not restrict | limited, The blocking electrode method is mentioned.

  The non-ion permeable resin is not particularly limited as long as it is an insulating resin. It may be a thermosetting resin or a thermoplastic resin.

  Specific examples of non-ion permeable resins include, for example, addition-condensation plastic resins having thermosetting properties such as phenol resins, urea resins, melamine resins; polyester resins, unsaturated polyester resins, polyimides, polyamides, silicone resins, etc. Polycondensation plastic: at least one solvent resistance selected from the group consisting of acrylic plastics such as polymethyl methacrylate (PMMA), polyacrylonitrile (PAN), polyacrylamide (PAA), polyvinyl acetate (PVAc), etc. The material which has can be illustrated preferably.

  The resin infiltration portion is disposed (formed) on the outer periphery of the electrode reaction portion in the surface direction of the positive electrode active material layer or the negative electrode active material layer.

  Here, “disposed on the outer periphery of the electrode reaction part” means that when the entire active material layer is used as a reference, a non-ion permeable resin in the active material from the outer peripheral edge of the active material layer toward the inside. Is formed. There is no restriction | limiting in particular in the part in which non-ion-permeable resin is formed, Non-ion-permeable resin should just be formed inward from the outer peripheral edge side of an active material layer as much as possible. However, as an example, the non-ion permeable resin is more preferably 0.1 to 100 times, more preferably 0.5 to 10 times, more preferably 0.5 to 10 times the thickness of the active material layer from the outer peripheral edge of the active material layer. Preferably, it is formed inward with a length of 1 to 5 times.

  As a method for examining whether or not the resin permeation part is arranged on the outer periphery of the electrode reaction part, for example, a method such as solid NMR or FT-IR is used to perform resin structural analysis or organic functional group analysis. To do.

(Positional relationship between positive electrode reaction part and negative electrode reaction part)
The outer peripheral edge of the electrode reaction part in the positive electrode active material layer is located on or inward of the outer peripheral edge of the electrode reaction part in the negative electrode active material layer.

  In the nonaqueous electrolyte secondary battery of the present invention, there are no particular limitations on the size of the positive electrode active material layer and the negative electrode active material layer. In addition, the outer peripheral edge of the positive electrode active material layer is preferably positioned inward or inward with respect to the outer peripheral edge of the electrode reaction portion in the negative electrode active material layer.

(Positive electrode active material)
Although it does not restrict | limit especially as a composition (material) which can be used for the positive electrode active material which comprises the lithium ion secondary battery positive electrode of this invention, Preferably the lithium nickel cobalt manganese composite shown by following Chemical formula (1) It is an oxide.

  In the above formula, 0 <a ≦ 1.2, 0.3 ≦ b ≦ 0.9, 0 ≦ c ≦ 0.6, 0.25 ≦ d ≦ 0.6, 0 ≦ e ≦ 0.3, 1. 5 ≦ f ≦ 2.2 and 0 ≦ g ≦ 0.5. M is at least one selected from the group consisting of Al or Mg, Ca, Ti, V, Cr, Fe, and Ga, and X is at least one of F, Cl, and S. The composition of these positive electrode active materials can be measured by ICP, atomic absorption method, fluorescent X-ray method, chelate titration, and particle analyzer.

  Specifically, for example, lithium-manganese composite oxide, lithium-nickel composite oxide, lithium-cobalt composite oxide, lithium-iron composite oxide, lithium-nickel-cobalt composite oxide, lithium-manganese-cobalt composite oxide , Lithium-nickel-manganese-cobalt composite oxide, lithium-metal phosphate compound, lithium-manganese phosphate, lithium-nickel phosphate, lithium-cobalt phosphate, lithium-iron phosphate, and lithium -Transition metal sulfate compounds are exemplified. In some cases, two or more positive electrode active materials may be used in combination.

  The average particle diameter of the positive electrode active material is preferably 0.05 to 20 μm, more preferably 0.1 to 10 μm, and still more preferably 0.1 to 5 μm.

The BET specific surface area of the positive electrode active material is preferably 0.5 to 10 m ² / g, more preferably 1 to 5 m ² / g, and still more preferably 2 to 3 m ² / g.

(Negative electrode active material)
The negative electrode active material layer includes a negative electrode active material. Since the contents other than the type of the negative electrode active material are the same as described above, the description thereof is omitted here.

  As the negative electrode material active material, a negative electrode active material that is also used in a conventionally known solution-type lithium ion battery can be used. Specifically, a negative electrode mainly composed of at least one selected from carbon materials such as natural graphite, artificial graphite, amorphous carbon, coke and mesophase pitch carbon fiber, graphite, and hard carbon which is amorphous carbon. Although it is desirable to use an active material, it is not particularly limited. In addition, metal oxides (especially transition metal oxides, specifically titanium oxides), metal (especially transition metals, specifically titanium) and lithium complex oxides, silica-based materials, etc. may be used. it can.

  The average particle diameter of the negative electrode active material is preferably 0.05 to 20 μm, more preferably 0.1 to 10 μm, and still more preferably 0.1 to 5 μm.

The BET specific surface area of the negative electrode active material is preferably 0.5 to 10 m ² / g, more preferably 1 to 5 m ² / g, and still more preferably 2 to 3 m ² / g.

  The active material layer may contain other materials if necessary. For example, a conductive aid, a binder, a supporting salt (lithium salt), an ion conductive polymer, and the like can be included. When an ion conductive polymer is included, a polymerization initiator for polymerizing the polymer may be included.

[Outside structure of active material layer]
In the non-aqueous electrolyte secondary battery of the present invention, the positive electrode active material layer and / or the outer structure of the negative electrode active material layer is not particularly limited, but an adhesive layer made of the non-ion permeable resin (hereinafter, It is preferable that it is disposed outside the active material layer. Such a structure of the positive electrode active material layer and / or the outer side of the negative electrode active material layer is useful in terms of improving mechanical characteristics (for example, repeated stress-strain characteristics). In particular, there is an effect that the stress becomes stronger when batteries are stacked. Furthermore, when batteries are stacked, there is an effect that displacement between electrodes is less likely to occur.

  In the nonaqueous electrolyte secondary battery of the present invention, the adhesive layer is in contact with the first current collector or the second current collector, and the positive electrode active material is between the adhesive layer and the electrolyte layer. It is preferable that a base material layer (hereinafter also simply referred to as “base material layer”) that maintains the thickness of the layer or the negative electrode active material layer is provided.

  In this case, the adhesive layer and the base material layer may be formed so as to be in contact with the outer peripheral edge of the active material layer as shown in FIGS. 10 to 14, the non-ion permeable resin is filled between the base material layer and the outer peripheral edge of the positive electrode active material layer and / or the negative electrode active material layer. Also good. 4A to 14 will be described in detail later.

  Furthermore, the total thickness of the adhesive layer and the base material layer in the battery is preferably slightly thicker than the active material layer. In that case, the battery has an effect of improving mechanical strength including durability and stackability. Here, “slightly thicker” means that the total thickness of the adhesive layer and the base material layer is preferably set to 1.01 to 1.2 times, more preferably about 1.05 to 1.1 times that of the active material layer. To do. By doing in this way, the deterioration of the electrode resulting from the stress which arises by lamination | stacking of a battery can be prevented.

(Base material)
In this specification, when attention is paid to the “base material layer” as a member that holds the non-ion-permeable resin, it may be referred to as “base material”.

  Although there is no restriction | limiting in particular as a specific example of a base material, For example, a fluorine resin, an olefin resin, etc. are mentioned. More specifically, a resin selected from a resin group having a relatively high melting point / softening point such as polyethylene terephthalate (PET), polyether nitrile (PEN), and polypropylene (PP) is preferable. The substrate may be the same resin as the binder (described above) that can be used for the positive electrode (negative electrode) mixture or a different resin.

  There is no restriction | limiting in particular also in the shape of a base material. However, since it is preferable to dispose the non-ion permeable resin held on the base material outside the active material layer, the shape surrounding the active material layer is preferable. For example, when the active material layer is a rectangle such as a square or a rectangle, the substrate is preferably frame-shaped.

  There is no restriction | limiting in particular also in the thickness of a base material. However, as will be described later, it may be adjusted as appropriate in relation to the thickness of the active material layer. For example, the thickness is preferably 1 to 300 μm, more preferably 5 to 200 μm, and still more preferably 10 to 150 μm.

  In addition, although demonstrated below, the base material used for the positive electrode side is also called "positive electrode base material" for convenience, and the base material used for the negative electrode side is also called "negative electrode base material".

(Conductive aid)
The conductive auxiliary agent that can be used in the present invention is not particularly limited, and conventionally known ones can be used.

  A conductive assistant means the additive mix | blended in order to improve electroconductivity. Examples of the conductive auxiliary agent include carbon materials such as carbon black such as acetylene black, graphite, vapor-grown carbon fiber, and graphite. Moreover, metal powder can also be used suitably as a conductive support agent.

(Binder)
The binder refers to an additive blended to play a role of binding a plurality of massive porous bodies in the active material layer. Specific examples of the binder include thermoplastic resins such as polyvinylidene fluoride (PVdF), polytetrafluoroethylene (PTFE), polyvinyl acetate, polyimide, urea resin, and thermosetting resins such as epoxy resin and polyurethane resin. Preferred are rubber materials such as butyl rubber and styrene rubber.

(Supporting salt)
Examples of the supporting salt (lithium salt) include Li (C ₂ F ₅ SO ₂ ) ₂ N, LiPF ₆ , LiBF ₄ , LiClO ₄ , LiAsF ₆ , LiCF ₃ SO _{3 and the} like.

(Ion conductive polymer)
Examples of the ion conductive polymer include polyethylene oxide (PEO) -based and polypropylene oxide (PPO) -based polymers. Here, the polymer may be the same as or different from the ion conductive polymer used in the electrolyte layer of the battery in which the electrode of the present invention is employed, but is preferably the same.

(Polymerization initiator)
The polymerization initiator is added to act on the crosslinkable group of the ion conductive polymer to advance the crosslinking reaction. Depending on the external factor for acting as an initiator, it is classified into a photopolymerization initiator, a thermal polymerization initiator and the like. Examples of the polymerization initiator include azobisisobutyronitrile (AIBN), which is a thermal polymerization initiator, and benzyl dimethyl ketal (BDK), which is a photopolymerization initiator.

  The compounding ratio of the components that can be included in the active material layer is not particularly limited, and can be adjusted by appropriately referring to known knowledge about the lithium ion secondary battery.

<Electrolyte layer>
In the present invention, the electrolyte used for the electrolyte layer is not particularly limited as long as it has Li ion conductivity, such as liquid, gel, or solid. It can be applied to any of (a) a separator impregnated with an electrolytic solution, (b) a polymer gel electrolyte, and (c) a polymer solid electrolyte depending on the purpose of use.

(A) Separator soaked with electrolyte solution As the electrolyte solution that can be soaked into the separator, the same electrolyte solution (electrolyte salt and plasticizer) contained in the polymer gel electrolyte can be used. The description in is omitted. As a preferable example of the electrolytic solution, as an _electrolyte, as _{LiClO 4, LiAsF 6, LiPF 5} , LiBOB, using at least one of LiCF ₃ SO ₃ and _{Li (CF 3 SO 2) 2} , solvent, ethylene carbonate (EC), propylene carbonate, diethyl carbonate (DEC), dimethyl carbonate, methyl ethyl carbonate, 1,2-dimethoxyethane, 1,2-diethoxyethane, tetrahydrofuran, 1,3-dioxolane and ether composed of γ-butyllactone The concentration of the electrolyte is adjusted to 0.5 to 2 mol / liter by dissolving at least one kind from the class and dissolving the electrolyte in the solvent, but the present invention is not limited to these. It shouldn't be.

(B) Polymer gel electrolyte and (c) Polymer solid electrolyte As the polymer gel electrolyte and polymer solid electrolyte, the same polymer gel electrolyte and polymer solid electrolyte can be used. Description is omitted.

  The electrolyte layers (a) to (c) may be used in one battery.

  In addition, the polymer electrolyte may be included in the polymer gel electrolyte layer, the positive electrode active material layer, and the negative electrode active material layer, but the same polymer electrolyte may be used, or different polymer electrolytes may be used depending on the layer. Good.

  By the way, a host polymer for a polymer gel electrolyte that is preferably used at present is a polyether polymer such as PEO and PPO. For this reason, the oxidation resistance on the positive electrode side under high temperature conditions is weak. Therefore, when using a positive electrode material having a high oxidation-reduction potential, the capacity of the negative electrode (active material layer) is preferably smaller than the capacity of the positive electrode (active material layer) opposed via the polymer gel electrolyte layer. When the capacity of the negative electrode (active material layer) is less than the capacity of the opposing positive electrode (active material layer), it is possible to prevent the positive electrode potential from rising excessively at the end of charging. In addition, the capacity | capacitance of a positive electrode (active material layer) and a negative electrode (active material layer) can be calculated | required from manufacturing conditions as theoretical capacity | capacitance at the time of manufacturing a positive electrode (active material layer) and a negative electrode (active material layer). You may measure the capacity | capacitance of a finished product directly with a measuring device. However, if the capacity of the negative electrode (active material layer) is smaller than the capacity of the opposing positive electrode (active material layer), the negative electrode potential will drop too much and the durability of the battery may be impaired. There is a need. For example, care should be taken not to lower the durability by setting the average charge voltage of one cell (single cell layer) to an appropriate value for the oxidation-reduction potential of the positive electrode active material.

  The thickness of the electrolyte layer constituting the battery is not particularly limited. However, in order to obtain a compact battery, it is preferable to make it as thin as possible within a range in which the function as an electrolyte can be ensured, and the thickness of the electrolyte layer is preferably 5 to 200 μm.

(Separator)
The separator is not particularly limited as long as it is an insulating porous material, fiber, or the like, and any conventionally known material can be used. For example, a porous sheet made of a polymer that absorbs and holds the electrolytic solution (for example, a polyolefin-based microporous separator), a nonwoven fabric separator, or the like can be used. The polyolefin microporous separator having the property of being chemically stable to an organic solvent has an excellent effect that the reactivity with the electrolyte (electrolytic solution) can be kept low.

  Examples of the material for the porous sheet such as the polyolefin-based microporous separator include polyethylene (PE), polypropylene (PP), a structure having a three-layer structure of PP / PE / PP, and polyimide.

  As a material of the nonwoven fabric separator, for example, conventionally known materials such as cotton, rayon, acetate, nylon, polyester, polypropylene, polyethylene such as polyethylene, polyimide, and aramid can be used. Depending on the purpose of use (such as mechanical strength required for the electrolyte layer), these are used alone or in combination.

  The bulk density of the non-woven fabric is not particularly limited as long as sufficient battery characteristics can be obtained by the impregnated polymer gel electrolyte. That is, if the bulk density of the nonwoven fabric is too large, the proportion of the non-electrolyte material in the electrolyte layer becomes too large, and the ionic conductivity and the like in the electrolyte layer may be impaired.

  The porosity of the separator (eg, polyolefin-based microporous separator) is preferably 20 to 50% by mass. The separator's porosity is within the above range, preventing output from being reduced due to the resistance of the electrolyte (electrolyte), and preventing the short circuit caused by fine particles penetrating the separator's pores (micropores). It has the effect of securing both sexes. Here, the porosity of the separator is a value obtained as a volume ratio from the density of the raw material resin and the density of the separator of the final product.

  Moreover, it is preferable that the porosity of a nonwoven fabric separator is 50-90 mass%. If the porosity is less than 50% by mass, the electrolyte retention deteriorates, and if it exceeds 90% by mass, the strength may be insufficient.

  The amount of the electrolytic solution impregnated in the separator may be impregnated to the range of the liquid retention capacity of the separator, but may be impregnated beyond the liquid retention capacity range. This can prevent impregnation of the electrolyte from the electrolyte layer by injecting a resin into the electrolyte seal portion, and therefore can be impregnated as long as the electrolyte layer can be retained. The electrolyte can be impregnated in the separator by a conventionally known method, for example, the electrolyte can be completely sealed after being injected by a vacuum injection method or the like.

<Method for producing non-aqueous electrolyte secondary battery>
An object of the present invention is to provide a nonaqueous electrolyte secondary battery in which dendrites are significantly prevented and mechanical strength is improved. Therefore, here, a method for manufacturing such a nonaqueous electrolyte secondary battery will be described.

  The technique described in Patent Document 1 not only has a problem in mechanical strength as described above, but also forms a group of electrodes by laminating a positive electrode and a negative electrode with a separator interposed therebetween. Had to be placed exactly in the middle of the. With such a technique, it is difficult to efficiently produce a battery.

  According to the method for producing a non-aqueous electrolyte secondary battery of the present invention, it is not necessary to accurately dispose the positive electrode and the negative electrode at the center of the separator, so that the battery can be manufactured efficiently.

  That is, the method for manufacturing a nonaqueous electrolyte secondary battery according to the present invention includes a positive electrode active material layer formed on the surface of the first current collector, and a negative electrode active material layer formed on the surface of the second current collector. , Is a method for manufacturing a non-aqueous electrolyte secondary battery including a power generation element formed by stacking a plurality of electrolyte layers, the surface of the first current collector and the outer periphery of the positive electrode active material layer, Forming a first non-ion permeable resin member thicker than the thickness of the positive electrode active material layer and / or the surface of the second current collector on the outer periphery of the negative electrode active material layer; A first step of forming a second non-ion permeable resin member thicker than the thickness to produce a single cell layer; and after the first step, the single cell layer is pressed in the stacking direction, and an electrode reaction in the positive electrode active material layer With respect to the outer peripheral edge of the electrode reaction part in the negative electrode active material layer. Comprising a second step of matching or located inward, and a method for producing a nonaqueous electrolyte secondary battery.

  Hereinafter, the first non-ion permeable resin member or the second non-ion permeable resin member is also simply referred to as “non-ion permeable resin member” as described above. Moreover, although a non-ion-permeable resin member may consist only of an adhesive layer, it preferably includes a base material layer and an adhesive layer.

  In the production method of the present invention, an electrode reaction part and a resin permeation part are formed on at least one of the active material layers. Preferably, at least the electrode reaction part and the resin infiltration part are formed on the positive electrode side. More preferably, it is formed only on the positive electrode side.

  As described above, in the production method of the present invention, the first non-ion permeable resin member thicker than the thickness of the positive electrode active material layer is provided on the outer surface of the positive electrode active material layer on the surface of the first current collector. A cell is formed by forming and / or forming a second non-ion permeable resin member thicker than the thickness of the negative electrode active material layer on the outer surface of the negative electrode active material layer on the surface of the second current collector A first step of forming a layer, and the single cell layer is pressed in the stacking direction after the first step, and an outer peripheral edge of the electrode reaction portion in the positive electrode active material layer is defined as an outer periphery of the electrode reaction portion in the negative electrode active material layer. And a second step of being aligned or inward with respect to the edge.

  By including these two steps, dendrites are significantly suppressed / prevented in the manufactured nonaqueous electrolyte secondary battery.

  Except for including the above characteristic steps, conventionally known knowledge may be referred to in combination.

  A method for producing the nonaqueous electrolyte secondary battery of the present invention will be described below.

<First step>
The first step is to form a first non-ion permeable resin member thicker than the thickness of the positive electrode active material layer on the outer surface of the positive electrode active material layer on the surface of the first current collector, and / or A second non-ion permeable resin member thicker than the thickness of the negative electrode active material layer is formed on the outer surface of the second current collector and on the outer periphery of the negative electrode active material layer to produce a single battery layer.

  As a premise of the first step, it is necessary to prepare an active material layer (positive electrode active material layer, negative electrode active material layer) formed on the surface of the current collector (first current collector, second current collector). Conventionally known knowledge can be appropriately referred to for the preparation method. As a precaution, a brief description will be given below, but it goes without saying that the method is not limited to the following method.

  First, an active material slurry is prepared by adding an active material and a conductive additive to a solvent (active material slurry preparation step). The active material slurry is applied to the surface of the current collector and dried to form a coating film (coating film forming step). The electrode produced through the coating film forming step is pressed in the thickness direction of the current collector (pressing step). In addition, when an ion conductive polymer is added to the active material slurry and a polymerization initiator is further added for the purpose of crosslinking the ion conductive polymer, the drying is performed simultaneously with the drying in the coating film forming step or before the drying. Or you may give a polymerization process later.

[Active material slurry preparation process]
In this step, a desired active material, a desired conductive assistant, and other components (for example, a binder, an ion conductive polymer, a supporting salt (lithium salt), a polymerization initiator, etc.) in a solvent To prepare an active material slurry. This active material slurry preparation step can be performed by appropriately referring to known knowledge or combining them. Since the specific form of each component blended in the active material slurry is as described in the column of the configuration of the electrode of the present invention, detailed description is omitted here.

  Moreover, the kind of solvent and the mixing means are not particularly limited, and conventionally known knowledge about electrode production can be appropriately referred to. As an example of the solvent, N-methyl-2-pyrrolidone (NMP), dimethylformamide, dimethylacetamide, methylformamide, and the like can be used. When adopting polyvinylidene fluoride (PVdF) as a binder, NMP is preferably used as a solvent.

[Coating film forming process]
Subsequently, a current collector is prepared, and the active material slurry prepared above is applied to the surface of the current collector and dried. Thereby, the coating film which consists of an active material slurry is formed on the surface of an electrical power collector. This coating film becomes an active material layer through a pressing step described later. The specific form of the current collector to be prepared is as described in the column of the configuration of the electrode of the present invention, and thus detailed description thereof is omitted here. The application means for applying the active material slurry is not particularly limited, and generally used means such as a comma coater and a die coater may be employed. A coating film is formed according to the desired arrangement | positioning form of the electrical power collector and active material layer in the electrode manufactured. When the electrode to be manufactured is a bipolar electrode, a coating film containing a positive electrode active material is formed on one surface of the current collector, and a coating film containing a negative electrode active material is formed on the other surface. On the other hand, when an electrode that is not a bipolar type is manufactured, a coating film containing either a positive electrode active material or a negative electrode active material is formed on both surfaces of one current collector.

  Thereafter, the coating film formed on the surface of the current collector is dried. Thereby, the solvent in a coating film is removed. The drying means for drying the coating film is not particularly limited, and conventionally known knowledge about electrode production can be appropriately referred to. For example, heat treatment is exemplified. Drying conditions (drying time, drying temperature, etc.) can be appropriately set according to the application amount of the active material slurry and the volatilization rate of the solvent of the slurry. In addition, when a coating film contains a polymerization initiator, the ion conductive polymer in a coating film is bridge | crosslinked by a crosslinkable group by performing a polymerization process further. The polymerization treatment in the polymerization step is not particularly limited, and conventionally known knowledge may be referred to as appropriate. For example, when the coating film contains a thermal polymerization initiator (AIBN or the like), the coating film is subjected to heat treatment. Moreover, when a coating film contains a photoinitiator (BDK etc.), light, such as an ultraviolet light, is irradiated. In addition, the heat processing for thermal polymerization may be performed simultaneously with said drying process, and may be performed before or after the said drying process.

[Step of forming a non-ion permeable resin member thicker than the active material layer on the surface of the current collector and on the outer periphery of the active material layer]
This step is a characteristic step in the production method of the present invention. More specifically, the step of forming a non-ion permeable resin member on the surface of the current collector and thicker than the active material layer on the outer periphery of the active material layer is as follows. That is, a first non-ion permeable resin member thicker than the thickness of the positive electrode active material layer is formed on the outer surface of the positive electrode active material layer on the surface of the first current collector, and / or the second This is a step of forming a second non-ion permeable resin member thicker than the thickness of the negative electrode active material layer on the surface of the current collector and on the outer periphery of the negative electrode active material layer.

  As described above, the non-ion-permeable resin member may be composed of only the adhesive layer, but preferably includes a base material layer and an adhesive layer. The non-ion permeable resin member is made thicker than the active material layer, and is formed on the surface of the current collector and on the outer periphery of the active material layer. When the non-ion permeable resin member includes a base material layer and an adhesive layer, the non-ion permeable resin member is preferably arranged so that the adhesive layer is on the current collector side. Hereinafter, the non-ion permeable resin member will be described mainly with respect to the form in which the adhesive layer is formed on the base material layer. However, as described above, the non-ion permeable resin member may be composed only of the adhesive layer.

  Here, the base material layer is made not only of the role of maintaining the thickness of the positive electrode active material layer or the negative electrode active material layer (maintaining the distance between the adhesive layer and the electrolyte layer), but also made of a non-ion permeable resin. It can also serve as a support for disposing the adhesive layer outside the active material layer.

  When the non-ion permeable resin portion includes a base material layer and an adhesive layer, the adhesive layer is formed on a part of the base material layer as well as a form in which the adhesive layer is formed on the entire base material layer. Also includes form.

  Here, “part” is not particularly limited, but in the second step described later, it is sufficient for the amount of the outer peripheral edge of the positive electrode reaction part to be aligned or inward with respect to the outer peripheral edge of the negative electrode reaction part. I just need it. That is, the amount of the non-ion permeable resin held on the base material can also be set so that the outer peripheral edge of the positive electrode reaction part coincides with or is inward of the outer peripheral edge of the negative electrode reaction part (that is, the positive electrode reaction part and the negative electrode reaction part). There is no particular limitation as long as it is an amount for which the positional relationship is allowed. When the non-ion permeable resin is infiltrated, the thickness of the adhesive layer may be equal to the thickness of the active material layer. In this case, needless to say, “equal” includes the concept of “substantially equal”. In addition, in the present specification, when “the same amount” is defined, “substantially” is also included.

  A non-ion-permeable resin member that includes a base material layer and an adhesive layer (for example, an adhesive layer is formed on the base material layer) is formed on the surface of the current collector and on the outer periphery of the active material layer There is no restriction on the specific position when doing so. However, it is preferable to include any one of steps (i) to (iii).

  (I) A non-ion permeable resin member in which an adhesive layer and a base material layer are disposed so as to be in contact with the outer peripheral edge of the active material layer is formed.

  (I) is represented by FIG. 4 (a), FIGS. 6-9 (positive electrode side / negative electrode side), FIG. 5 (positive electrode side), etc. which are explained in detail later, for example. In the first step, a non-ion permeable resin member that is thicker than the thickness of the active material layer is formed on the surface of the current collector and on the outer periphery of the active material layer. In (i), the non-ion permeable resin member is disposed so that the adhesive layer constituting the non-ion permeable resin member and the base material layer are in contact with the outer peripheral edge of the active material layer. As shown in FIG. 4B as a modification of FIG. 4A, the adhesive layer is in contact with the outer peripheral edge of the active material layer, but a part on the base material layer (for example, on the base material layer). A form in which an adhesive layer is formed in a half region) is also possible.

  (Ii) A non-ion permeable resin member is formed in which the adhesive layer is spaced apart from the outer peripheral edge of the active material layer and the base material layer is disposed in contact with the outer peripheral edge of the active material layer.

  (Ii) is represented, for example, in FIG. 5 (negative electrode side) described in detail later. As described above, in the first step, a non-ion permeable resin member thicker than the thickness of the active material layer is formed on the current collector surface and on the outer periphery of the active material layer. In (ii), the non-ion permeable resin member is formed such that the adhesive layer constituting the non-ion permeable resin member is separated from the outer peripheral edge of the active material layer, and the base material constituting the non-ion permeable resin member The layer is disposed so as to contact the outer peripheral edge of the active material layer.

  (Iii) A non-ion permeable resin member is formed in which the adhesive layer and the base material layer are disposed apart from the outer peripheral edge of the active material layer.

  (Iii) is represented by, for example, FIGS. 10 to 14 (positive electrode side / negative electrode side) described in detail later. As described above, in the first step, a non-ion permeable resin member thicker than the thickness of the active material layer is formed on the current collector surface and on the outer periphery of the active material layer. In (iii), the non-ion permeable resin member is disposed such that the adhesive layer constituting the non-ion permeable resin member and the base material layer are separated from the outer peripheral edge of the active material layer.

  Through the first step, a single cell layer is produced. In the second step, which will be described later, “the outer peripheral edge of the electrode reaction part (positive electrode reaction part) of the electrode reaction part (negative electrode reaction part) in the negative electrode active material layer”. You are ready to "match or inwardly align with the outer peripheral edge".

<Second step>
The manufacturing method of the present invention includes a second step after the first step. In the second step, the unit cell layer is pressed in the stacking direction, and the outer peripheral edge of the electrode reaction part (positive electrode reaction part) in the positive electrode active material layer is connected to the electrode reaction part (negative electrode reaction part) in the negative electrode active material layer. Align or inward with the outer peripheral edge.

[The cell layer is pressed in the stacking direction, and the outer peripheral edge of the positive electrode reaction part is aligned or inward with respect to the outer peripheral edge of the negative electrode reaction part]
The positive electrode and the negative electrode are applied to each other with the electrolyte applied to both the positive electrode and the negative electrode, and then bonded to each other with a separator in between as necessary. In this way, a single cell layer is produced.

  The pressing can be performed by appropriately referring to or combining conventionally known methods, and examples thereof include a hot press machine and a calendar roll press machine.

  In this way, the non-ion permeable resin is creeped by pressing the unit cell layer in the stacking direction. The creeped non-ion permeable resin is infiltrated into the active material layer to form a resin infiltration portion, and the positive electrode reaction portion and the negative electrode reaction portion are set in a desired positional relationship.

  In order to achieve this desired positional relationship, “the size of the positive electrode and / or the negative electrode reaction part” and “the size of the active material layer” may be appropriately adjusted.

  The “size of the active material layer” can be set by appropriately adjusting the area of the active material applied to the current collector.

  The “size of the resin-permeable portion” is the thickness of the non-ion permeable resin member larger than the thickness of the active material layer (the thickness of the non-ion permeable resin member is the non-ion permeable property constituting the adhesive layer). It can be set by adjusting the amount of resin, the thickness of the base material layer, etc.), the press conditions, the heating conditions, etc. as appropriate. Hereinafter, a specific example will be described.

  For example, when it is desired to form a large resin-permeable portion, the resin-permeable portion may be formed using a larger amount of non-ion permeable resin (for example, a thick non-ionic permeable resin). When it is desired to form a small resin permeation portion, the resin permeation portion may be formed using a less non-ion permeable resin (for example, a non-ion permeable resin having a small thickness). When it is desired to form a large resin penetration portion with a smaller amount, a non-ion permeable resin including an adhesive layer composed of a significantly smaller amount of the non-ion permeable resin formed on a significantly thicker substrate layer A member is arrange | positioned on the outer side of an active material layer, and a single battery layer is produced. Then, by pressing it, the non-ion permeable resin may be infiltrated into the active material layer to form a resin infiltration portion.

  Here, the amount of the non-ion permeable resin cannot be uniquely determined by the glass transition point (hot press temperature) and the pressure (creep of the non-ion permeable resin due to a load). Can be referred to.

  That is, when the non-ion permeable resin member is disposed so as to contact the outer peripheral edge of the active material layer so that the adhesive layer is on the current collector side, the creep of the thickness of the non-ion permeable resin held on the base material The decrease may be estimated in advance, and the thickness of the substrate may be increased accordingly. On the other hand, when the gap is provided (that is, separated), it is desirable to fill the gap with a non-ion permeable resin that has been creeped. Therefore, it is preferable to increase the thickness of the non-ion-permeable resin held on the base material layer as compared with the case where the active material layer is disposed so as to be in contact with the outer peripheral edge. Such adjustment can be easily performed by those skilled in the art. The thickness of the non-ion permeable resin can be appropriately selected by those skilled in the art without departing from the characteristics of the present invention. However, when it arrange | positions so that the outer peripheral edge side of an active material layer may be contact | connected, the preferable ratio of the thickness of the non-ion-permeable resin hold | maintained on the base material by the thickness ratio of an active material layer is 50%-400%. More preferably, it is 70% to 300%, and still more preferably 100% to 200%. On the other hand, when the gap is provided, the preferred ratio of the thickness of the non-ion permeable resin held on the base material is 50% to 400% in the ratio of (active material layer thickness + gap length) ratio. More preferably, it is 70% to 300%, and still more preferably 100% to 200%. It should be noted that this ratio is merely a guideline, and it goes without saying that a person skilled in the art can adjust the size of the resin infiltration portion with reference to the above description.

  If the non-ion permeable resin is a thermosetting resin, the non-ion permeable resin is allowed to penetrate into the active material layer by pressing, and then heated to cure the non-ion permeable resin. . On the other hand, if the non-ion permeable resin is a thermoplastic resin, if the non-ion permeable resin is infiltrated into the active material layer by heating in advance to soften the non-ion permeable resin and then pressing it, Good.

  When pressing or heating as necessary, for example, a scraper, a mold, a resin mold, etc. are used to prevent the non-ion permeable resin held on the substrate from flowing out. Pressing and / or heating may be performed while stopping.

  Further, in the pressing step, a positive electrode and a negative electrode are laminated via an electrolyte layer to produce a single cell layer, which is pressed in the laminating direction. At this time, heating may be appropriately performed.

  In the design of the battery, the non-ion permeable resin member having the base material holding the non-ion permeable resin for forming the resin infiltration portion is set slightly thicker than the thickness of the active material layer. Good. The reason is as follows. That is, when the electrodes are stacked and pressed, the stress applied to the electrodes becomes severe outward. Therefore, there is an effect of improving the durability by designing the non-ion permeable resin member in the manufactured battery to be slightly thicker than the thickness of the active material layer to produce the battery. That is, it is possible to improve the deterioration of the electrode due to the stress generated in the battery stacking. Here, “slightly thick” is, for example, as follows. That is, the thickness of the non-ion-permeable resin member of the battery to be manufactured is preferably set to about 1.01 to 1.2 times, more preferably about 1.05 to 1.1 times that of the active material layer.

  By passing through the second step, the nonaqueous electrolyte secondary battery of the present invention can be manufactured.

  Hereinafter, a method for producing a nonaqueous electrolyte secondary battery according to the present invention will be described in detail with reference to the drawings and more specific embodiments. However, the present invention is not limited to the specific forms described below, and those skilled in the art can make modifications by appropriately referring to or combining conventionally known knowledge.

(About Fig. 4 (a))
4 (a) A and 4 (a) B are cross-sectional views schematically showing a form before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 4 (a) B, which is a form of “later form”, for example, a manufacturing method shown in FIG. 4 (a) A can be considered.

  (1) When the electrodes are stacked, on the current collector (13, 16), the outer peripheral edge of the positive electrode active material layer 14 coincides with the outer peripheral edge of the negative electrode active material layer 17 when viewed in the stacking direction. The active material slurry is coated on the surface.

  (2) Subsequently, a frame-like positive electrode substrate 30a (first non-ion permeable resin member 50a) formed by holding the first non-ion permeable resin 40a is disposed so as to be in contact with the positive electrode active material layer 14. . At this time, the first non-ion permeable resin 40a (adhesive layer 400) and the positive electrode base material 30a (base material layer) are in contact with the outer peripheral edge of the positive electrode active material layer 14 (active material layer). An ion permeable resin member 50a is disposed. A frame-shaped negative electrode substrate 30 b (second non-ion permeable resin member 50 b) that holds the second non-ion permeable resin 40 b is disposed so as to be in contact with the negative electrode active material layer 17. At this time, the second non-ion permeable resin 40b (adhesive layer 400) and the negative electrode base material 30b (base material layer) are in contact with the outer peripheral edge of the negative electrode active material layer 17 (active material layer). An ion permeable resin member 50b is disposed.

  In this case, the positive electrode base material 30a and the negative electrode base material 30b having substantially the same thickness are used.

  At this time, the first non-ion permeable resin 40a and the second non-ion permeable resin 40b are the same type of non-ion permeable resin.

  The thickness of the first non-ion permeable resin member 50a is significantly larger than the thickness of the positive electrode active material layer 14, and the thickness of the second non-ion permeable resin member 50b is set to be negative electrode active material layer 17. Is substantially the same as the thickness. At this time, the amount of the first non-ion permeable resin 40a is set to be larger than the amount of the second non-ion permeable resin 40b. In this embodiment, the thickness of the first non-ion permeable resin 40a is set larger than the thickness of the second non-ion permeable resin 40b. As a result, a large amount of nonionic resin permeates into the outer periphery of the positive electrode active material layer 14, and the positive electrode reaction part becomes smaller than the negative electrode reaction part.

  The positive electrode and the negative electrode are applied together with the electrolyte applied to both the positive electrode and the negative electrode, and then bonded to each other with a separator interposed therebetween as needed to produce a unit cell layer.

  (3) The single cell layer is pressed and heated as necessary.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 4A can be manufactured.

  That is, in the manufactured non-aqueous electrolyte secondary battery shown in FIG. 4A, the positive electrode active material layer 14 penetrates the electrode reaction part 70 (positive electrode reaction part) and the non-ion permeable resin 40. The negative electrode active material layer 17 is composed of an electrode reaction part 70 (negative electrode reaction part). In the manufactured nonaqueous electrolyte secondary battery shown in FIG. 4A, the resin infiltration portion 60 is disposed on the outer periphery of the electrode reaction portion 70 in the surface direction of the positive electrode active material layer 14. . Further, in the manufactured nonaqueous electrolyte secondary battery shown in FIG. 4A, the outer peripheral edge of the electrode reaction part 70 (positive electrode reaction part) in the positive electrode active material layer 17 is the negative electrode active material layer 17. Is located inward with respect to the outer peripheral edge of the electrode reaction part 70 (negative electrode reaction part). In the following description, when the structure of the manufactured nonaqueous electrolyte secondary battery is the same as this, the description thereof is omitted.

(About Fig. 4 (b))
FIG. 4B is a modification of FIG.

  As shown in FIG. 4B, the first non-ion permeable resin 40a (adhesive layer 400) and the positive electrode base material 30a (base material layer) are in contact with the outer peripheral edge of the positive electrode active material layer 14 (active material layer). In this manner, the first non-ion permeable resin member 50a is disposed. However, the first non-ion permeable resin 40a (adhesive layer 400) may not be formed over the entire positive electrode base material 30a.

(About Figure 5)
FIG. 5A and FIG. 5B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 5B which is a “later form”, for example, a manufacturing method shown in FIG. 5A can be considered.

  (1) This is the same as described above with reference to FIGS.

  (2) Subsequently, a frame-like positive electrode substrate 30a (first non-ion permeable resin member 50a) formed by holding the first non-ion permeable resin 40a is disposed so as to be in contact with the positive electrode active material layer 14. . At this time, the first non-ion permeable resin 40a (adhesive layer 400) and the positive electrode base material 30a (base material layer) are in contact with the outer peripheral edge of the positive electrode active material layer 14 (active material layer). The non-ion permeable resin member 50a is disposed so that the adhesive layer 400 is on the current collector side. Note that “so that the first non-ion permeable resin member 50a is on the current collector side of the first non-ion permeable resin member 50a” is the same in any of the following embodiments, and will be omitted below.

  A frame-shaped negative electrode substrate 30 b (second non-ion permeable resin member 50 b) that holds the second non-ion permeable resin 40 b is disposed so as to be in contact with the negative electrode active material layer 17. At this time, the second non-ion permeable resin 40b (adhesive layer 400) is separated from the outer peripheral edge of the negative electrode active material layer 17 (active material layer), and the negative electrode base material 30b (base material layer) is the negative electrode active material. The second non-ion-permeable resin member 50b is disposed so that the adhesive layer 400 is on the current collector side so as to contact the outer peripheral edge of the layer 17 (active material layer). Note that “so that the second non-ion permeable resin member 50b has the adhesive layer 400 on the current collector side” is the same in any of the following embodiments, and will not be described below.

  In this case, the positive electrode base material 30a and the negative electrode base material 30b having the same thickness are used.

  At this time, the first non-ion permeable resin 40a and the second non-ion permeable resin 40b are the same type of non-ion permeable resin.

  The thickness of the first non-ion permeable resin member 50 a is significantly larger than the thickness of the positive electrode active material layer 14, and the thickness of the second non-ion permeable resin member 50 b is also equal to that of the negative electrode active material layer 17. Thicker than the thickness. At this time, the amount of the first non-ion permeable resin 40a is set to be larger than the amount of the second non-ion permeable resin 40b. In this embodiment, the thickness of the first non-ion permeable resin 40a and the thickness of the second non-ion permeable resin 40b are substantially the same, but the first non-ion permeable resin 40a is formed on the substrate 30. Set the area to be held large.

  As a result, a large amount of nonionic resin permeates into the outer periphery of the positive electrode active material layer 14, and the positive electrode reaction part becomes smaller than the negative electrode reaction part.

  The positive electrode and the negative electrode are applied together with the electrolyte applied to both the positive electrode and the negative electrode, and then bonded to each other with a separator interposed therebetween as needed to produce a unit cell layer.

  (3) The single cell layer is pressed and heated as necessary.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 4A can be manufactured.

(About Figure 6)
FIG. 6A and FIG. 6B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 6B which is the “later form”, for example, a manufacturing method shown in FIG. 6A can be considered.

  (1) This is the same as described above with reference to FIGS.

  (2) Subsequently, a frame-like positive electrode substrate 30a (first non-ion permeable resin member 50a) formed by holding the first non-ion permeable resin 40a is disposed so as to be in contact with the positive electrode active material layer 14. . At this time, the first non-ion permeable resin 40a (adhesive layer 400) and the positive electrode base material 30a (base material layer) are in contact with the outer peripheral edge of the positive electrode active material layer 14 (active material layer). An ion permeable resin member 50a is disposed. Further, a frame-shaped negative electrode substrate 30 b (second non-ion permeable resin member 50 b) that holds the second non-ion permeable resin 40 b is disposed so as to be in contact with the negative electrode active material layer 17. At this time, the second non-ion permeable resin 40b (adhesive layer 400) and the negative electrode base material 30b (base material layer) are in contact with the outer peripheral edge of the negative electrode active material layer 17 (active material layer). An ion permeable resin member 50b is disposed.

  In this case, the positive electrode base material 30a and the negative electrode base material 30b having the same thickness are used.

  At this time, the first non-ion permeable resin 40a and the second non-ion permeable resin 40b are different types of non-ion permeable resins. Specifically, the glass transition point of the first non-ion permeable resin 40a is lower than the glass transition point of the second non-ion permeable resin 40b. Hereinafter, those having a relatively high glass transition point are also referred to as “high glass transition points”, and those having a low glass transition point are also referred to as “low glass transition points”.

  The thickness of the first non-ion permeable resin member 50a is significantly larger than the thickness of the positive electrode active material layer 14, and the thickness of the second non-ion permeable resin member 50b is set to be negative electrode active material layer 17. Is substantially the same as the thickness. At this time, the amount of the first non-ion permeable resin 40a and the amount of the second non-ion permeable resin 40b are substantially the same.

  In this embodiment, the first non-ion permeable resin 40a and the second non-ion permeable resin 40b are different types of non-ion permeable resins. As a result, a large amount of nonionic resin permeates into the outer periphery of the positive electrode active material layer 14, and the positive electrode reaction part becomes smaller than the negative electrode reaction part.

  The positive electrode and the negative electrode are applied together with the electrolyte applied to both the positive electrode and the negative electrode, and then bonded to each other with a separator interposed therebetween as needed to produce a unit cell layer.

  (3) The single cell layer is pressed and heated.

  In this case, the first non-ion permeable resin 40ay (thermoplastic resin) having a low glass transition point is first softened by the second non-ion permeable resin 40bx (thermoplastic resin) having a high glass transition point. As a result, the first non-ion permeable resin 40ay having a low glass transition point penetrates into the positive electrode active material layer. Thus, the resin penetration part 60 is formed.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 6B can be manufactured.

  In addition, as a battery assembly, when a thermal load is applied, a material having similar thermophysical properties is preferable from the viewpoint of preventing deterioration (the same thermal expansion coefficient causes less mechanical deterioration). Therefore, the difference (ΔT) between the two glass transition points is preferably 100 ° C. to 200 ° C., more preferably 20 ° C. to 100 ° C., and further preferably 20 ° C. to 50 ° C.

(About Figure 7)
FIG. 7A and FIG. 7B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 7B which is a “later form”, for example, a manufacturing method shown in FIG. 7A can be considered.

  (1) This is the same as described above with reference to FIGS.

  (2) Subsequently, a frame-like positive electrode substrate 30a (first non-ion permeable resin member 50a) formed by holding the first non-ion permeable resin 40a is disposed so as to be in contact with the positive electrode active material layer 14. . At this time, the first non-ion permeable resin member 50a is formed with the first non-ion permeable resin 40ax having a high glass transition point on the frame-shaped positive electrode substrate 30a, and has a low glass transition point on the inside thereof. The first non-ion permeable resin 40ay is formed so as to have a structure. The first non-ion permeable resin 40ay (adhesive layer 400) having a low glass transition point and the positive electrode base material 30a (base material layer) are in contact with the outer peripheral edge of the positive electrode active material layer 14 (active material layer). In addition, the first non-ion permeable resin member 50a is disposed. A frame-shaped negative electrode substrate 30 b (second non-ion permeable resin member 50 b) that holds the second non-ion permeable resin 40 b is disposed so as to be in contact with the negative electrode active material layer 17. At this time, the second non-ion permeable resin 40b (adhesive layer 400) and the negative electrode base material 30b (base material layer) are in contact with the outer peripheral edge of the negative electrode active material layer 17 (active material layer). An ion permeable resin member 50b is disposed.

  In this case, the positive electrode base material 30a and the negative electrode base material 30b having the same thickness are used.

  The thickness of the first non-ion permeable resin member 50a is significantly larger than the thickness of the positive electrode active material layer 14, and the thickness of the second non-ion permeable resin member 50b is set to be negative electrode active material layer 17. Is substantially the same as the thickness. At this time, the amount of the first non-ion permeable resin 40a is set to be larger than the amount of the second non-ion permeable resin 40b. The amount of the first non-ion permeable resin 40ax having a high glass transition point and the amount of the second non-ion permeable resin 40bx having a high glass transition point are set to be substantially the same. In this embodiment, the thickness of the first non-ion permeable resin 40a is set larger than the thickness of the second non-ion permeable resin 40b. As a result, a large amount of nonionic resin permeates into the outer periphery of the positive electrode active material layer 14, and the positive electrode reaction part becomes smaller than the negative electrode reaction part.

  The positive electrode and the negative electrode are applied together with the electrolyte applied to both the positive electrode and the negative electrode, and then bonded to each other with a separator interposed therebetween as needed to produce a unit cell layer.

  (3) The single cell layer is pressed and heated.

  In this case, the first non-ion permeable resin 40ay (thermoplastic resin) having a low glass transition point is first softened by the second non-ion permeable resin 40bx (thermoplastic resin) having a high glass transition point. As a result, the first non-ion permeable resin 40ay having a low glass transition point penetrates into the positive electrode active material layer. Thus, the resin penetration part 60 is formed.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 7B can be manufactured.

(About Figure 8)
8A and 8B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 8B which is a “later form”, for example, a manufacturing method shown in FIG. 8A can be considered.

  (1) This is the same as described above with reference to FIGS.

  (2) Subsequently, a frame-like positive electrode substrate 30a (first non-ion permeable resin member 50a) formed by holding the first non-ion permeable resin 40a is disposed so as to be in contact with the positive electrode active material layer 14. . At this time, the first non-ion permeable resin 40a (adhesive layer 400) and the positive electrode base material 30a (base material layer) are in contact with the outer peripheral edge of the positive electrode active material layer 14 (active material layer). An ion permeable resin member 50a is disposed. A frame-shaped negative electrode substrate 30 b (second non-ion permeable resin member 50 b) that holds the second non-ion permeable resin 40 b is disposed so as to be in contact with the negative electrode active material layer 17. At this time, the second non-ion permeable resin 40b (adhesive layer 400) and the negative electrode base material 30b (base material layer) are in contact with the outer peripheral edge of the negative electrode active material layer 17 (active material layer). An ion permeable resin member 50b is disposed.

  At this time, the positive electrode base material 30a is thicker than the negative electrode base material 30b.

  At this time, the first non-ion permeable resin 40a and the second non-ion permeable resin 40b are the same type of non-ion permeable resin.

  The thickness of the first non-ion permeable resin member 50a is significantly larger than the thickness of the positive electrode active material layer 14, and the thickness of the second non-ion permeable resin member 50b is set to be negative electrode active material layer 17. Is substantially the same as the thickness. At this time, the amount of the first non-ion permeable resin 40a and the amount of the second non-ion permeable resin 40b are substantially the same. In this embodiment, the thickness of the first non-ion permeable resin 40a and the thickness of the second non-ion permeable resin 40b are set to be substantially the same. As a result, a large amount of nonionic resin permeates into the outer periphery of the positive electrode active material layer 14, and the positive electrode reaction part becomes smaller than the negative electrode reaction part.

  The positive electrode and the negative electrode are applied together with the electrolyte applied to both the positive electrode and the negative electrode, and then bonded to each other with a separator interposed therebetween as needed to produce a unit cell layer.

  (3) The single cell layer is pressed and heated.

  The heating at this time is set so that the temperature applied to the first current collector 13 side is higher than the temperature applied to the second current collector 16 side.

  In this case, the first non-ion permeable resin 40ay (thermoplastic resin) having a low glass transition point is first softened by the second non-ion permeable resin 40bx (thermoplastic resin) having a high glass transition point. As a result, the first non-ion permeable resin 40ay having a low glass transition point penetrates into the positive electrode active material layer. Thus, the resin penetration part 60 is formed.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 6B can be manufactured.

(About Figure 9)
FIG. 9A and FIG. 9B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 9B which is a “later form”, for example, a manufacturing method shown in FIG. 9A can be considered.

  (1) When the electrodes are stacked, the positive electrode active material layer 14 and the negative electrode active material layer 17 are arranged so that the outer peripheral edge of the positive electrode active material layer 14 is outside the outer peripheral edge of the negative electrode active material layer 17 when viewed in the stacking direction. The active material slurry is coated on the current collectors (13, 16) so as to be positioned in the direction.

  (2) Subsequently, a frame-like positive electrode substrate 30a (first non-ion permeable resin member 50a) formed by holding the first non-ion permeable resin 40a is disposed so as to be in contact with the positive electrode active material layer 14. . At this time, the first non-ion permeable resin 40a (adhesive layer 400) and the positive electrode base material 30a (base material layer) are in contact with the outer peripheral edge of the positive electrode active material layer 14 (active material layer). An ion permeable resin member 50a is disposed. A frame-shaped negative electrode substrate 30 b (second non-ion permeable resin member 50 b) that holds the second non-ion permeable resin 40 b is disposed so as to be in contact with the negative electrode active material layer 17. At this time, the second non-ion permeable resin 40b (adhesive layer 400) and the negative electrode base material 30b (base material layer) are in contact with the outer peripheral edge of the negative electrode active material layer 17 (active material layer). An ion permeable resin member 50b is disposed.

  In this case, the positive electrode base material 30a and the negative electrode base material 30b having substantially the same thickness are used.

  At this time, the first non-ion permeable resin 40a and the second non-ion permeable resin 40b are the same type of non-ion permeable resin.

  The thickness of the first non-ion permeable resin member 50a is significantly larger than the thickness of the positive electrode active material layer 14, and the thickness of the second non-ion permeable resin member 50b is set to be negative electrode active material layer 17. Is substantially the same as the thickness. At this time, the amount of the first non-ion permeable resin 40a is set to be larger than the amount of the second non-ion permeable resin 40b. In this embodiment, the thickness of the first non-ion permeable resin 40a is set larger than the thickness of the second non-ion permeable resin 40b. As a result, a large amount of nonionic resin permeates into the outer periphery of the positive electrode active material layer 14, and the positive electrode reaction part becomes smaller than the negative electrode reaction part.

  The positive electrode and the negative electrode are applied together with the electrolyte applied to both the positive electrode and the negative electrode, and then bonded to each other with a separator interposed therebetween as needed to produce a unit cell layer.

  (3) The single cell layer is pressed and heated as necessary.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 4A can be manufactured.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 9B can be manufactured. That is, in the manufactured non-aqueous electrolyte secondary battery shown in FIG. 9B, the positive electrode active material layer 14 is formed by infiltrating the electrode reaction part 70 (positive electrode reaction part) and the non-ion permeable resin 40. The negative electrode active material layer 17 includes an electrode reaction unit 70 (negative electrode reaction unit). In the manufactured nonaqueous electrolyte secondary battery shown in FIG. 9B, the resin infiltration portion 60 is disposed on the outer periphery of the electrode reaction portion 70 in the surface direction of the positive electrode active material layer 14. Furthermore, in the manufactured nonaqueous electrolyte secondary battery shown in FIG. 9B, the outer peripheral edge of the electrode reaction part 70 (positive electrode reaction part) in the positive electrode active material layer 17 is the electrode reaction part in the negative electrode active material layer 17. It corresponds to the outer peripheral edge side of 70 (negative electrode reaction part). In the following description, when the structure of the manufactured nonaqueous electrolyte secondary battery is the same as this, the description thereof is omitted.

  FIG. 9 shows a case where the sizes of the active material layers (14, 16) are different. In such a case, the positive electrode reaction part and the negative electrode reaction part can be formed in the present invention by a method other than setting the amount of the first non-ion permeable resin 40a larger than the amount of the second non-ion permeable resin 40b. Needless to say, the allowable positional relationship can be set (for example, FIGS. 5 to 8).

(About Figure 10)
FIG. 10A and FIG. 10B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 10B which is a “later form”, for example, a manufacturing method shown in FIG. 10A can be considered. That is, the present embodiment corresponds to FIG. 4A (FIG. 5), and in the above description, in FIG. 4A (FIG. 5) (2), the non-ion-permeable resin member. 50 can be performed by a method similar to the method described in FIGS. 4A and 5 except that a gap is provided between the outer peripheral edge of the active material layer and the outer peripheral edge side.

  More specifically, a frame-shaped base material 30 (non-ion permeable resin member 50) that holds the non-ion permeable resin 40 is disposed so as to be separated from the positive electrode active material layer 14. That is, the non-ion permeable resin 40 (adhesive layer 400) and the base material 30 (base material layer) are separated from the outer peripheral edge of the active material layer (14, 17) (active material layer). The conductive resin member 50 is disposed. The non-ion permeable resin 40 includes a first non-ion permeable resin 40a and a second non-ion permeable resin 40b, and the base material 30 includes a positive electrode base material 30a and a negative electrode base material 30b, and an active material layer Is a concept including the positive electrode active material layer 14 and the negative electrode active material layer 17 as described above.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 10B can be manufactured. That is, the non-ion permeable resin member 50 is positioned with a gap between the positive electrode active material layer 14 and the outer peripheral edge of the negative electrode active material layer 17, and the non-ion permeable resin 40 fills the gap. Thus, a non-aqueous electrolyte secondary battery can be manufactured.

(About Figure 11)
FIG. 11A and FIG. 11B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 11B which is a “later form”, for example, a manufacturing method shown in FIG. 11A can be considered. That is, this embodiment corresponds to FIG. 6, and in FIG. 6 (2) described above, the non-ion permeable resin member 50 is placed between the outer peripheral edge of the active material layer. 6 can be performed by a method similar to the method described in FIG.

  More specifically, the frame-shaped base material 30 (non-ion permeable resin member 50) formed by holding the non-ion permeable resin 40 is disposed so as to be separated from the active material layers (14, 17). That is, the non-ion permeable resin 40 (adhesive layer 400) and the base material 30 (base material layer) are separated from the outer peripheral edge of the active material layer (14, 17) (active material layer). The conductive resin member 50 is disposed.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 11B can be manufactured. That is, the non-ion permeable resin member 50 is positioned with a gap between the positive electrode active material layer 14 and the outer peripheral edge of the negative electrode active material layer 17, and the non-ion permeable resin 40 fills the gap. Thus, a non-aqueous electrolyte secondary battery can be manufactured.

(About Figure 12)
FIG. 12A and FIG. 12B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 12B which is a “later form”, for example, a manufacturing method shown in FIG. 12A can be considered. That is, this embodiment corresponds to FIG. 7, and in FIG. 7 (2) described above, the non-ion permeable resin member 50 is placed between the outer peripheral edge of the active material layer. 7 can be performed by the same method as described in FIG.

  More specifically, the non-ion permeable resin 40 (adhesive layer 400) and the positive electrode base material 30 (base material layer) are separated from the outer peripheral edge of the active material layer (14, 17) (active material layer). In addition, the non-ion permeable resin member 50 is disposed. That is, the non-ion permeable resin 40 (adhesive layer 400) and the base material 30 (base material layer) are separated from the outer peripheral edge of the active material layer (14, 17) (active material layer). The conductive resin member 50 is disposed.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 12B can be manufactured. That is, the non-ion permeable resin member 50 is positioned with a gap between the positive electrode active material layer 14 and the outer peripheral edge of the negative electrode active material layer 17, and the non-ion permeable resin 40 fills the gap. Thus, a non-aqueous electrolyte secondary battery can be manufactured.

(About Figure 13)
FIG. 13A and FIG. 13B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 13B which is a “later form”, for example, a manufacturing method shown in FIG. 13A can be considered. In other words, this embodiment corresponds to FIG. 8, and in FIG. 8 (2) described above, the non-ion permeable resin member 50 is spaced from the outer peripheral edge of the active material layer. The method can be performed by a method similar to the method described in FIG.

  More specifically, the frame-shaped base material 30 (non-ion permeable resin member 50) formed by holding the non-ion permeable resin 40 is disposed so as to be separated from the active material layers (14, 17). That is, the non-ion permeable resin 40 (adhesive layer 400) and the base material 30 (base material layer) are separated from the outer peripheral edge of the active material layer (14, 17) (active material layer). The conductive resin member 50 is disposed.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 13B can be manufactured. That is, the non-ion permeable resin member 50 is positioned with a gap between the positive electrode active material layer 14 and the outer peripheral edge of the negative electrode active material layer 17, and the non-ion permeable resin 40 fills the gap. Thus, a non-aqueous electrolyte secondary battery can be manufactured.

(About Figure 14)
FIG. 14A and FIG. 14B are cross-sectional views schematically showing forms before and after manufacturing an embodiment of the nonaqueous electrolyte secondary battery according to the present invention, respectively. In order to manufacture the non-aqueous electrolyte secondary battery shown in FIG. 14B which is the “later form”, for example, a manufacturing method shown in FIG. 14A can be considered. In other words, this embodiment corresponds to FIG. 9, and in FIG. 9 (2) described above, the non-ion permeable resin member 50 is spaced from the outer peripheral edge of the active material layer. 9 can be performed by a method similar to the method described in FIG.

  More specifically, the frame-shaped base material 30 (non-ion permeable resin member 50) formed by holding the non-ion permeable resin 40 is disposed so as to be in contact with the active material layers (14, 17). That is, the non-ion permeable resin 40 (adhesive layer 400) and the base material 30 (base material layer) are separated from the outer peripheral edge of the active material layer (14, 17) (active material layer). The conductive resin member 50 is disposed.

  By including the above steps, the nonaqueous electrolyte secondary battery shown in FIG. 14B can be manufactured. That is, the non-ion permeable resin member 50 is positioned with a gap between the positive electrode active material layer 14 and the outer peripheral edge of the negative electrode active material layer 17, and the non-ion permeable resin 40 fills the gap. Thus, a non-aqueous electrolyte secondary battery can be manufactured.

<Insulating layer>
The insulating layer is mainly used in the case of a bipolar battery. This insulating layer is formed around each electrode for the purpose of preventing adjacent collectors in the battery from contacting each other and short-circuiting due to slight unevenness at the end of the laminated electrode. It is. In this invention, you may provide an insulating layer around an electrode as needed. When this is used as a vehicle driving or auxiliary power source, it is necessary to completely prevent a short circuit (liquid junction) due to the electrolytic solution. Furthermore, vibrations and impacts on the battery are loaded for a long time. Therefore, from the viewpoint of prolonging battery life, it is desirable to install an insulating layer in order to ensure longer-term reliability and safety, and to provide a high-quality, large-capacity power supply. .

  The insulating layer only needs to have insulating properties, sealing properties against falling off of the solid electrolyte, sealing properties against moisture permeation from the outside (sealing properties), heat resistance at the battery operating temperature, and the like. For example, epoxy resin, rubber, polyethylene, polypropylene, polyimide and the like can be used, but epoxy resin is preferable from the viewpoint of corrosion resistance, chemical resistance, ease of production (film forming property), economy, and the like.

  FIG. 15 schematically shows a cross-sectional view of a nonaqueous electrolyte secondary battery in which an insulating layer 27 that can be used in the present invention is formed.

  FIG. 15A is a diagram showing a form in which an insulating layer 27 is provided around an electrode in the nonaqueous electrolyte secondary battery described in FIGS. 4A to 14. In order to fix the insulating layer 27, insulation is performed. An adhesive layer 400 is provided on the surface of the layer 27. FIG. 15B shows a form in which the base material layer 30 and the insulating layer 27 described above are used as an integrated type. FIG. 15C shows a form in which the adhesive layer 400 is embedded in the separator (not shown) when the electrolyte 15 is impregnated.

  As described above, various forms of the insulating layer 27 are assumed and are not limited to those illustrated in FIG. 15, and can be applied by appropriately referring to known knowledge or combining them. .

<Positive electrode and negative electrode lead>
The positive electrode and the negative electrode lead are not limited to the bipolar type, and the same leads as those used in conventionally known non-bipolar lithium ion batteries can be used. In addition, the part taken out from the battery exterior material (battery case) does not affect the product (for example, automobile parts, especially electronic devices, etc.) by contacting with peripheral devices or wiring and leaking electricity. It is preferable to coat with a heat-resistant insulating heat-shrinkable tube or the like.

<Battery exterior material (battery case)>
Lithium ion batteries are not limited to bipolar types, but in order to prevent external impact and environmental degradation during use, the battery non-ion permeable resin member that is the battery body or the entire battery wound body is not It is desirable to house it in a battery case. From the viewpoint of weight reduction, a polymer-metal composite laminate film in which both surfaces of metals (including alloys) such as aluminum, stainless steel, nickel, and copper are covered with an insulator (preferably a heat-resistant insulator) such as a polypropylene film. A conventionally known battery exterior material may be used. And it is preferable to make it the structure which accommodated and sealed the battery non-ion-permeable resin member by joining a part or all of the peripheral part by heat sealing | fusion. In this case, the positive electrode and the negative electrode lead may be structured to be sandwiched between the heat-sealed portions and exposed to the outside of the battery exterior material. In addition, it is preferable to use a polymer-metal composite laminate film having excellent thermal conductivity because heat can be efficiently transmitted from a heat source of an automobile and the inside of the battery can be quickly heated to the battery operating temperature. The polymer-metal composite laminate film is not particularly limited, and a conventionally known film in which a metal film is disposed between polymer films and the whole is laminated and integrated can be used. As specific examples, for example, an outer protective layer made of a polymer film (laminate outermost layer), a metal film layer, a heat-sealing layer made of a polymer film (laminate innermost layer), and the whole is laminated and integrated. The thing which becomes. Specifically, in the polymer-metal composite laminate film used for the exterior material, a heat-resistant insulating resin film is first formed as a polymer film on both surfaces of the metal film, and heat fusion is performed on at least one heat-resistant insulating resin film. An insulating insulating film is laminated. Such a laminate film is heat-sealed by an appropriate method, whereby the heat-welding insulating film portion is fused and joined to form a heat-sealing portion. An example of the metal film is an aluminum film. Further, as the non-ion permeable resin 40 film, a polyethylene tetraphthalate film (heat-resistant insulating film), a nylon film (heat-resistant insulating film), a polyethylene film (heat-bonding insulating film), a polypropylene film (heat-bonding insulation) For example. However, the exterior material of the present invention should not be limited to these. In such a laminate film, it is possible to easily and surely join one to one (bag-like) laminate films by heat fusion using a heat fusion insulating film by ultrasonic welding or the like. In order to maximize the long-term reliability of the battery, metal films that are constituent elements of the laminate sheet may be directly joined. Ultrasonic welding can be used to join the metal films by removing or destroying the heat-fusible resin between the metal films.

<External configuration of lithium-ion battery>
FIG. 16 is a perspective view showing the appearance of a stacked flat (non-bipolar) lithium ion secondary battery (flat battery) which is a typical embodiment of the lithium ion battery according to the present invention.

  As shown in FIG. 16, the laminated flat lithium ion secondary battery 8 has a rectangular flat shape, and a positive electrode tab 81 and a negative electrode tab 82 for taking out electric power from both sides thereof. Has been pulled out. The power generation element (battery element) 83 is wrapped by the battery exterior material 84 of the lithium ion secondary battery 8. The periphery thereof is heat-sealed, and the power generation element (battery element) 83 is sealed with the positive electrode tab 81 and the negative electrode tab 82 drawn to the outside.

  As described above, the lithium ion battery of the present invention is not limited to the stacked flat shape as shown in FIG. 16, and the wound lithium ion battery has a cylindrical shape. It may be. Such a cylindrical shape may be deformed into a rectangular flat shape. In the said cylindrical shape thing, a laminate film may be used for the exterior material, and the conventional cylindrical can (metal can) may be used, for example, It does not restrict | limit.

  Further, the taking out of the tabs 81 and 82 shown in FIG. 16 is not particularly limited, and the positive electrode tab 81 and the negative electrode tab 82 may be pulled out from the same side. The positive electrode tab 81 and the negative electrode tab 82 may be divided into a plurality of parts and taken out from each side, and the present invention is not limited to the one shown in FIG. Further, in a wound type lithium ion battery, instead of a tab, for example, a terminal may be formed using a cylindrical can (metal can).

  The following are mentioned as a use of the lithium ion secondary battery which concerns on this invention. For example, as a large-capacity power source for an electric vehicle (EV), a hybrid electric vehicle (HEV), a fuel cell vehicle, a hybrid fuel cell vehicle, etc. Can be used. In this case, it is desirable that the assembled battery is constructed by connecting a plurality of lithium ion secondary batteries of the present invention. That is, in the present embodiment, a plurality of lithium ion secondary batteries according to the present invention are assembled using at least one of a parallel connection, a series connection, a parallel-series connection, or a series-parallel connection. ). This makes it possible to meet the demands for capacity and voltage for various types of vehicles by combining basic batteries. As a result, it becomes possible to facilitate the design selectivity of required energy and output. For this reason, it is not necessary to design and produce different batteries for various vehicles, and it becomes possible to mass-produce basic batteries and to reduce costs by mass production. Hereinafter, a representative embodiment of the assembled battery (vehicle submodule) will be briefly described with reference to the drawings.

  The assembled battery of the present invention is constituted by connecting a plurality of lithium ion batteries of the present invention. Specifically, at least two or more are used, and are configured by serialization, parallelization, or both. Capacitance and voltage can be freely adjusted by paralleling in series. In the assembled battery of the present invention, the non-bipolar lithium ion battery and the bipolar lithium ion battery of the present invention are used, and a plurality of these are combined in series, in parallel, or in series and in parallel. Can also be configured.

  17 is an external view of a typical embodiment of the assembled battery according to the present invention, FIG. 17A is a plan view of the assembled battery, FIG. 17B is a front view of the assembled battery, and FIG. 17C is an assembled battery. FIG.

  As shown in FIG. 17, the assembled battery 9 according to the present invention forms a small assembled battery 91 that can be attached and detached by connecting a plurality of lithium ion batteries of the present invention in series or in parallel. A plurality of these detachable small assembled batteries 91 are further connected in series or in parallel. Thereby, the assembled battery 9 having a large capacity and a large output suitable for a vehicle driving power source and an auxiliary power source that require a high volume energy density and a high volume output density can be formed. FIG. 17A is a plan view of the assembled battery, FIG. 17A is a front view, and FIG. 17C is a side view. The small assembled batteries 91 that can be attached and detached are connected to each other using an electrical connection means such as a bus bar, and the assembled batteries 91 are stacked in multiple stages using a connection jig 92. How many non-bipolar or bipolar lithium-ion batteries are connected to produce the assembled battery 91, and how many assembled batteries 91 are stacked to produce the assembled battery 9 depends on the vehicle on which the battery is mounted. What is necessary is just to determine according to the battery capacity and output of (electric vehicle).

  When the lithium ion secondary battery using the nonaqueous electrolyte secondary battery of the present invention or a battery pack formed by combining a plurality of them is used in a vehicle, a vehicle having the effects described above is obtained.

  The vehicle is not particularly limited. For example, in the case of a car, a hybrid car, a fuel cell car, an electric car (all are four-wheeled vehicles (passenger cars, commercial vehicles such as trucks and buses, light vehicles, etc.), and two-wheeled vehicles (motorcycles). ) And tricycles). Further, it can be applied to various power sources for other vehicles such as a moving body such as a train, and can also be used as a mounting power source for an uninterruptible power supply.

  FIG. 18 is a conceptual diagram of a vehicle equipped with the assembled battery of the present invention.

  As shown in FIG. 18, in order to mount the assembled battery 100 in a vehicle such as the electric vehicle 200, the battery pack 100 is mounted under the seat at the center of the vehicle body of the electric vehicle 200. This is because if it is installed under the seat, the interior space and the trunk room can be widened. The place where the assembled battery 100 is mounted is not limited to the position under the seat, but may be a lower part of the rear trunk room or an engine room in front of the vehicle. The electric vehicle 200 using the assembled battery 100 as described above has high durability and can provide sufficient output even when used for a long period of time. Furthermore, it is possible to provide electric vehicles and hybrid vehicles that are excellent in fuel efficiency and running performance. A vehicle equipped with the assembled battery of the present invention can be widely applied to a hybrid vehicle, a fuel cell vehicle and the like in addition to an electric vehicle as shown in FIG.

  The effects of the embodiments of the present invention are summarized as follows.

  -A dendrite can be prevented significantly and the mechanical strength of a battery can be improved.

  -The filling capacity is maintained, the adhesion strength of the peripheral edge of the positive electrode plate is sufficiently maintained, and the positive electrode mixture is prevented from dropping off during the charge / discharge cycle.

  ・ The design capacity and the actual capacity are the same.

  -The positive electrode active material layer and the negative electrode active material layer can be made equal in size at the battery design stage.

  -It is not necessary to arrange the positive electrode and the negative electrode accurately at the center between the separators, and the battery can be efficiently manufactured.

1 is a schematic cross-sectional view of a flat (stacked) non-bipolar lithium ion secondary battery. It is the schematic sectional drawing which represented typically the whole structure of the bipolar lithium ion secondary battery. FIG. 6 is a plan view schematically showing an outer peripheral edge when an electrode active material layer is projected. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. It is sectional drawing which represents typically the form before and after manufacturing one Embodiment of the nonaqueous electrolyte secondary battery which concerns on this invention. 1 schematically illustrates a cross-sectional view of a nonaqueous electrolyte secondary battery in which an insulating layer that can be used in the present invention is formed. 1 is a perspective view showing an appearance of a stacked flat (non-bipolar) lithium ion secondary battery that is a typical embodiment of a lithium ion battery according to the present invention. 17A is a plan view of the assembled battery according to the present invention, FIG. 17B is a front view of the assembled battery according to the present invention, and FIG. 17C is a side view of the assembled battery according to the present invention. It is a schematic diagram which shows the vehicle carrying the assembled battery of this invention.

Explanation of symbols

Stacked battery 1,
Battery exterior material 12,
First current collector 13,
Positive electrode active material layer 14,
Electrolyte layer 15,
Second current collector 16,
Negative electrode active material layer 17,
Power generation element 18,
Positive electrode (terminal) lead 19,
Negative electrode (terminal) lead 10,
Bipolar battery 2,
Battery element 21,
Positive electrode active material layer 22,
Negative electrode active material layer 23,
Current collector 24,
Outermost layer current collector 24a, 24b
Current collector 24a ', 24b'
Electrolyte layer 25,
Unit cell layer 26,
Insulating layer 27,
Positive electrode tab 28a,
Negative electrode tab 28b,
Laminate sheet 29,
Base material 30,
Non-ion permeable resin 40,
First non-ion permeable resin 40a,
First non-ion permeable resin 40ax having a high glass transition point,
First non-ion permeable resin 40ay having a low glass transition point,
Second non-ion permeable resin 40b,
A second non-ion permeable resin 40bx having a high glass transition point,
Adhesive layer 400,
Non-ion permeable resin member 50,
First non-ion permeable resin member 50a,
Second non-ion permeable resin member 50b,
Resin penetration part 60,
Electrode reaction part 70,
Flat battery 8,
Positive electrode tab 81,
Negative electrode tab 82,
Power generation element (battery element) 83,
Battery pack 9
Small assembled battery 91,
Connecting jig 92,
Battery pack 100,
Electric vehicle 200.

Claims (4)

A positive electrode active material layer formed on at least one surface of the first current collector and a negative electrode active material layer formed on at least the other surface of the second current collector are laminated with an electrolyte layer interposed therebetween. A non-aqueous electrolyte secondary battery including a power generation element formed by laminating a plurality of unit cell layers,
At least one of the positive electrode active material layer and the negative electrode active material layer includes an electrode reaction portion effective for an electrochemical reaction and a resin infiltration portion formed by infiltrating a non-ion permeable resin,
The resin infiltration portion is disposed on the outer periphery of the electrode reaction portion in the surface direction of the positive electrode active material layer or the negative electrode active material layer,
The outer peripheral edge of the electrode reaction part in the positive electrode active material layer is located on or inward with respect to the outer peripheral edge of the electrode reaction part in the negative electrode active material layer,
The positive electrode active material layer and / or the negative electrode active material layer is disposed outside the adhesive layer, and includes an adhesive layer made of the non-ion permeable resin.
The adhesive layer is in contact with the current collector;
Between the adhesive layer and the electrolyte layer, a base material layer that holds the thickness of the positive electrode active material layer or the negative electrode active material layer is provided,
A non-aqueous electrolyte secondary battery in which the non-ion permeable resin is filled between the base material layer and an outer peripheral edge of the positive electrode active material layer and / or the negative electrode active material layer. The resin infiltrating portion extends inward from the outer peripheral edge of the positive electrode active material layer and / or the negative electrode active material layer to a length of 1 to 100 times the thickness of the positive electrode active material layer and / or the negative electrode active material layer. It headed formed, a non-aqueous electrolyte secondary battery according to claim 1. A positive electrode active material layer formed on at least one surface of the first current collector and a negative electrode active material layer formed on at least the other surface of the second current collector are laminated with an electrolyte layer interposed therebetween. A non-aqueous electrolyte secondary battery including a power generation element formed by laminating a plurality of unit cell layers,
The positive electrode active material layer is composed of an electrode reaction part effective for an electrochemical reaction and a resin infiltration part formed by infiltrating a non-ion permeable resin,
The resin infiltration portion is disposed on the outer periphery of the electrode reaction portion in the surface direction of the positive electrode active material layer,
The outer peripheral edge of the electrode reaction part is aligned or inward with respect to the outer peripheral edge of the negative electrode active material layer,
The positive electrode active material layer and / or the negative electrode active material layer is disposed outside the adhesive layer, and includes an adhesive layer made of the non-ion permeable resin.
The adhesive layer is in contact with the current collector;
Between the electrolyte layer and the adhesive layer, the positive active material layer or the negative electrode active base layer for holding the thickness of the material layer is Re et al comprises
A non- aqueous electrolyte secondary battery in which the non -ion permeable resin is filled between the base material layer and an outer peripheral edge of the positive electrode active material layer and / or the negative electrode active material layer . 4. The non-aqueous electrolyte 2 according to claim 3 , wherein the resin infiltration portion is formed inward from the outer peripheral edge of the positive electrode active material layer to a length of 1 to 100 times the thickness of the positive electrode active material layer. Next battery.

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