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CN112020790A - Nonaqueous electrolyte secondary battery - Google Patents

Nonaqueous electrolyte secondary battery Download PDF

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Publication number
CN112020790A
CN112020790A CN201980028125.6A CN201980028125A CN112020790A CN 112020790 A CN112020790 A CN 112020790A CN 201980028125 A CN201980028125 A CN 201980028125A CN 112020790 A CN112020790 A CN 112020790A
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CN
China
Prior art keywords
positive electrode
container
negative electrode
secondary battery
nonaqueous electrolyte
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Granted
Application number
CN201980028125.6A
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Chinese (zh)
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CN112020790B (en
Inventor
二川秀史
森绫香
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Honda Motor Co Ltd
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Honda Motor Co Ltd
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/531—Electrode connections inside a battery casing
    • H01M50/534—Electrode connections inside a battery casing characterised by the material of the leads or tabs
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/572—Means for preventing undesired use or discharge
    • H01M50/574—Devices or arrangements for the interruption of current
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/531—Electrode connections inside a battery casing
    • H01M50/536—Electrode connections inside a battery casing characterised by the method of fixing the leads to the electrodes, e.g. by welding
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Inorganic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)
  • Connection Of Batteries Or Terminals (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

The invention provides a nonaqueous electrolyte secondary battery capable of reliably operating an electric conduction cut-off mechanism during overcharge without reducing battery performance. The nonaqueous electrolyte secondary battery 1 includes a positive electrode 41, container positive electrode terminals 21 and 23, a negative electrode 42, container negative electrode terminals 22 and 24, a nonaqueous electrolytic solution, and an energization shutoff mechanism 68b capable of shutting off energization to the outside of the container when the container internal pressure rises, in the container 2. The positive electrode mixture layer unformed portion 41b or at least one of the positive electrode terminals 21 and 23 in the container is provided with a positive electrode active material layer capable of generating a gas capable of operating the current interruption mechanism 68 b.

Description

Nonaqueous electrolyte secondary battery
Technical Field
The present invention relates to a nonaqueous electrolyte secondary battery.
Background
Conventionally, there has been known a nonaqueous electrolyte secondary battery including a positive electrode having a positive electrode mixture layer and a positive electrode current collector, a negative electrode having a negative electrode mixture layer and a negative electrode current collector, and a nonaqueous electrolytic solution in a container. In the nonaqueous electrolyte secondary battery, for example, lithium ions are used as charge carriers that carry out battery reactions.
When the nonaqueous electrolyte secondary battery is overcharged, a nonaqueous solvent or the like of the electrolyte is electrolyzed to generate gas, and the internal pressure rises. Therefore, there is known a nonaqueous electrolyte secondary battery provided with an electricity cut-off mechanism that cuts off the current supply from the outside to the positive electrode or the negative electrode when the internal pressure rises due to overcharge (see, for example, patent document 1).
Further, there is known a nonaqueous electrolyte secondary battery in which a gas generating agent is contained in an electrolyte solution in order to reliably operate the current cutoff mechanism at the time of overcharge, and the gas generating agent reacts to generate a gas by a voltage equal to or higher than the maximum operating power of the nonaqueous electrolyte secondary battery (see, for example, patent document 2). According to the nonaqueous electrolyte secondary battery containing the gas generating agent in the electrolytic solution, the internal pressure of the nonaqueous electrolyte secondary battery can be increased by the gas generated from the gas generating agent before the gas is generated by electrolysis of the nonaqueous solvent or the like at the time of overcharge, and the current interruption mechanism can be reliably operated.
Documents of the prior art
Patent document
Patent document 1: international publication No. 2014/049848
Patent document 2 Japanese patent laid-open publication No. 2013-69490
Disclosure of Invention
Problems to be solved by the invention
However, in the nonaqueous electrolyte secondary battery described in patent document 2, since the gas generating agent is added to the electrolytic solution, the gas generating agent interferes with the battery reaction, and there is a problem that the battery performance such as input/output characteristics and energy density is lowered.
In the nonaqueous electrolyte secondary battery, it is also conceivable to add the gas generating agent to the positive electrode mixture layer or the negative electrode mixture layer, but in this case, the generated gas may be enclosed in the positive electrode mixture layer or the negative electrode mixture layer and the current interruption mechanism may not be operated.
The present invention aims to provide a nonaqueous electrolyte secondary battery capable of solving the above-described problems and reliably operating an electric current cutoff mechanism during overcharge without degrading battery performance.
Means for solving the problems
In order to achieve the above object, a nonaqueous electrolyte secondary battery according to the present invention includes: a positive electrode having a positive electrode mixture layer and a positive electrode current collector; an in-container positive electrode terminal electrically connected to the positive electrode mixture layer non-formed portion of the positive electrode current collector; a negative electrode having a negative electrode mixture layer and a negative electrode current collector; an in-container negative electrode terminal electrically connected to the negative electrode mixture layer unformed portion of the negative electrode current collector; a non-aqueous electrolyte; and an energization shutoff mechanism capable of shutting off energization between the positive electrode terminal in the container or the negative electrode terminal in the container and an outside of the container when an internal pressure of the container rises, wherein at least one of the positive electrode mixture layer unformed portion and the positive electrode terminal in the container includes a positive electrode active material layer that reacts with a voltage equal to or higher than a maximum operating power of the nonaqueous electrolyte secondary battery to generate a gas capable of raising the internal pressure of the container and operating the energization shutoff mechanism.
According to the nonaqueous electrolyte secondary battery of the present invention, when the battery voltage becomes a voltage equal to or higher than the maximum operating power of the nonaqueous electrolyte secondary battery due to overcharge, the positive electrode active material forming the positive electrode active material layer capable of generating a gas is decomposed or changed in quality, and an element in the composition of the positive electrode active material is gasified to generate a gas. Alternatively, the positive electrode active material or the modified positive electrode active material reacts with the conductive auxiliary agent, the binder, or the electrolyte at the interface thereof, so that the conductive auxiliary agent, the binder, or the electrolyte is decomposed to generate a gas.
As a result, the internal pressure in the container rises, and the current cutoff mechanism operates to cut off the current from the inside of the container to the outside of the container through the positive electrode terminal or the negative electrode terminal, thereby preventing overcharging.
In this case, since the nonaqueous electrolyte secondary battery of the present invention includes the positive electrode active material layer in the positive electrode mixture layer non-formation portion or in at least one member of the positive electrode terminal in the container, battery reaction in the positive electrode mixture layer, the negative electrode mixture layer, or the nonaqueous electrolyte solution is not hindered by the positive electrode active material, and a decrease in battery performance such as energy density can be prevented. Further, the current interruption mechanism can be reliably operated because there is no case where gas generated by decomposition or alteration of the positive electrode active material or decomposition of the conductive additive, binder, or electrolyte solution after reaction with the positive electrode active material or altered positive electrode active material is encapsulated in the positive electrode material mixture layer or the negative electrode material mixture layer.
In the nonaqueous electrolyte secondary battery of the present invention, it is preferable that the gas-generating positive electrode active material layer contains LiNi as a positive electrode active material0.5Mn1.5O4(LNMO)。LiNi0.5Mn1.5O4(LNMO) can easily generate gas because of high reaction potential and high reactivity with the electrolyte.
Drawings
Fig. 1 is a perspective view showing one configuration example of the nonaqueous electrolyte secondary battery of the present embodiment.
Fig. 2 is an exploded perspective view of the nonaqueous electrolyte secondary battery shown in fig. 1.
Fig. 3 is an exploded perspective view of an electrode body element of the nonaqueous electrolyte secondary battery shown in fig. 1.
Fig. 4 is a partial sectional view showing the configuration of the current interruption mechanism of the nonaqueous electrolyte secondary battery shown in fig. 1.
Fig. 5 is an exploded perspective view of the components of the configuration shown in fig. 4.
Detailed Description
Next, embodiments of the present invention will be described in further detail with reference to the drawings.
As shown in fig. 1 and 2, a nonaqueous electrolyte secondary battery 1 of the present embodiment includes a battery case 2, and the battery case 2 includes: a battery can 4 having a square deep drawn shape; and a battery lid 3 that seals the opening 4a of the battery can 4. The battery case 2 accommodates a power generating element therein. The power generating element includes an electrode body element 40 wound in a flat shape with separators 43 and 44 interposed between a positive electrode 41 and a negative electrode 42 and stacked. The electrode assembly 40 is inserted into the battery case 4 together with the positive electrode collector plate 21 and the negative electrode collector plate 31 in a state of being covered with an insulating sheet (not shown) from the outside thereof.
The battery can 4 and the battery cover 3 are made of aluminum alloy, and the battery cover 3 is joined to the battery can 4 by laser welding to seal the opening 4 a. The battery lid 3 is provided with a positive-electrode-side terminal constituent part 60 and a negative-electrode-side terminal constituent part 70 to form a lid assembly.
The positive electrode-side terminal component 60 and the negative electrode-side terminal component 70 have a positive electrode terminal 61 and a negative electrode terminal 71 disposed so as to sandwich the 1 st insulators 64 and 74 with the battery cover 3. The battery cover 3 is provided with, in addition to the positive electrode terminal 61 and the negative electrode terminal 71: a gas discharge valve 13 that opens when the pressure in the battery container 2 is higher than a predetermined value to discharge the gas in the battery container 2; an injection port 12 for injecting an electrolyte into the battery case 2; and a filling plug 11 that seals the filling port 12 after the electrolyte is filled. The liquid pouring plug 11 is joined to the battery lid 3 by laser welding in a state where the liquid pouring port 12 is closed, and the liquid pouring port 12 is sealed.
The positive electrode terminal 61 and the negative electrode terminal 71 are disposed outside the rectangular battery cover 3 at positions separated from each other on one side and the other side in the longitudinal direction. The positive electrode terminal 61 and the negative electrode terminal 71 hold terminal bolts 63 and 73 for fixing the bus bar connection terminals, and are disposed to the inside of the battery cover 3 to achieve conductive connection. The positive electrode terminal 61 is made of aluminum or an aluminum alloy, and the negative electrode terminal 71 is made of a copper alloy.
The positive electrode terminal 61 is electrically insulated from the battery cover 3 by a gasket 66 and a 1 st insulator 64 on the outside of the battery cover 3 and a 2 nd insulator 65 (see fig. 4) on the inside of the battery cover 3. The positive electrode terminal 61 is fixed to the battery lid 3 by caulking together with the 2 nd insulator 65 and the connection electrode 67.
Positive electrode terminal 61 is electrically connected to positive electrode collector plate 21 with the current cutoff mechanism interposed between it and positive electrode collector plate 21. The configuration of the energization interrupting mechanism will be described in detail later. Negative electrode terminal 71 is electrically connected to negative electrode collector plate 31 with a connection terminal (not shown) interposed therebetween and negative electrode collector plate 31.
The positive electrode collector plate 21 and the negative electrode collector plate 31 have a pair of flat joint pieces 23 and 33 extending toward the bottom of the battery can 4 and conductively connected to the electrode element 40. Positive electrode collector plate 21 and joint piece 23 constitute an in-container positive electrode terminal, and negative electrode collector plate 31 and joint piece 33 constitute an in-container negative electrode terminal. The respective joining sheets 23 and 33 are joined by welding to a positive electrode 41 and a negative electrode 42 provided at both ends in the winding axial direction of the electrode body element 40. As the welding method, ultrasonic welding, resistance welding, laser welding, or the like can be used.
The electrode assembly 40 is disposed between the joining piece 23 of the positive electrode collector plate 21 and the joining piece 33 of the negative electrode collector plate 31, supported at both ends, and the cover assembly and the electrode assembly 40 constitute the power generating element assembly 5.
The electrode body element 40 is configured by: in a state where the winding end side is unwound, as shown in fig. 3, the negative electrode 42 and the positive electrode 41 are respectively disposed between the 1 st and 2 nd separators 43 and 44 and are wound in a flat shape. The positive electrode 41 includes a positive electrode mixture layer 41a and a positive electrode mixture layer unformed portion 41b formed on a positive electrode collector, not shown, and the negative electrode 42 includes a negative electrode mixture layer 42a and a negative electrode mixture layer unformed portion 42b formed on a negative electrode collector, not shown. As shown in fig. 3, the outermost electrode of the electrode body element 40 is a negative electrode 42, and a separator 44 is wound around the outer side thereof.
The separators 43 and 44 have a function of insulating the positive electrode 41 and the negative electrode 42. The negative electrode mixture layer 42a of the negative electrode 42 is larger than the positive electrode mixture layer 41a of the positive electrode 41 in the width direction, and therefore the positive electrode mixture layer 41a is inevitably sandwiched between the negative electrode mixture layers 42 a.
The positive electrode mixture layer non-formed portion 41b and the negative electrode mixture layer non-formed portion 42b are bundled at the flat surface portion, and are connected to the positive electrode collector plate 21 and the negative electrode collector plate 31 of each of the electrodes to which the positive electrode terminal 61 and the negative electrode terminal 71 are connected by welding or the like. The separators 43 and 44 are wider than the negative electrode mixture layer 42a in the width direction, but are wound around the positions where the positive electrode mixture layer unformed portions 41b and the negative electrode mixture layer unformed portions 42b are exposed on the metal foil surface, and therefore do not become an obstacle in the binding welding.
In the present embodiment, the electrode body element 40 is configured by disposing the long negative electrode 42 and the long positive electrode 41 between the long 1 st and 2 nd separators 43 and 44, respectively, and winding them in a flat shape, but the following configuration may be adopted: a plurality of units are stacked, and a 2 nd separator 44 is disposed between the units, with the 1 st separator 43 disposed between the elongated positive and negative electrodes 41, 42 as a unit.
Next, the details of the current interruption mechanism will be described with reference to fig. 4 and 5.
The current interruption mechanism is provided in a current path from the positive electrode terminal 61 of the positive electrode-side terminal forming unit 60 to the positive electrode current collector plate 21.
The positive electrode side terminal constituting part 60 is constituted by a positive electrode terminal 61, a positive electrode terminal bolt 63, a 1 st insulator 64, a 2 nd insulator 65, a gasket 66, a positive electrode connecting electrode 67, a conductive plate 68 deformed by an increase in the battery internal pressure, and a positive electrode current collecting plate 21. The positive electrode terminal 61, the 1 st insulator 64, the 2 nd insulator 65, the gasket 66, and the positive electrode connecting electrode 67 are integrally fixed to the battery lid 3 by caulking at the battery inner end surface portion of the positive electrode terminal 61. The positive current collector plate 21 is integrally fixed to the 2 nd insulator 65.
The positive electrode terminal 61 has: a plate-shaped body portion 61a disposed along an upper surface that is an outer side of the battery cover 3; a bolt insertion hole 61b that penetrates the main body portion 61a and that receives and supports the positive terminal bolt 63; and a shaft portion 61c that is inserted into the opening portion 3a of the battery cover 3 and protrudes inward of the battery cover 3, and the shaft portion 61c is provided with a through hole 61d that penetrates in the axial direction along the center thereof.
The positive terminal bolt 63 includes: a shaft portion 63a inserted into the bolt insertion hole 61b of the positive electrode terminal 61; and a head portion (bottom flat portion) 63b interposed and supported between the main body portion 61a and the 1 st insulator 64.
The 1 st insulator 64 is formed of an insulating plate-like member interposed between the positive electrode terminal 61 and the upper surface of the battery lid 3, and has an opening 64a (see fig. 5) communicating with the opening 3a of the battery lid 3 to allow the shaft portion 61c of the positive electrode terminal 61 to be inserted therethrough.
The gasket 66 is inserted in the opening portion 3a of the battery cover 3 to insulate and seal between the shaft portion 61c of the positive electrode terminal 61 and the battery cover 3.
The positive electrode connecting electrode 67 is formed of a conductive flat plate member disposed inside the battery cover 3, and is provided at the center thereof with an opening 67a communicating with the opening 3a of the battery cover 3 and through which the shaft portion 61c of the positive electrode terminal 61 is inserted. The positive electrode connecting electrode 67 is disposed along the lower surface of the battery cover 3 with the 2 nd insulator 65 interposed between the battery cover 3 and the electrode, and the opening 67a is opened in the planar lower surface (planar portion) 67b, and the tip of the shaft portion 61c of the positive electrode terminal 61 protruding from the opening 67a is expanded radially outward and caulked, whereby the positive electrode connecting electrode is electrically connected to the positive electrode terminal 61 and is integrally fixed to the battery cover 3 in a state of being insulated from the battery cover 3. The caulking portion 61e of the shaft portion 61c of the positive electrode terminal 61 protrudes to the lower surface 67b of the positive electrode connection electrode 67, and the through hole 61d communicating with the outside of the battery opens toward the inside of the battery.
The 2 nd insulator 65 is formed of an insulating plate-like member disposed along the lower surface of the battery cover 3, and is interposed between the battery cover 3 and the positive electrode connecting electrode 67 and between the battery cover 3 and the positive electrode current collecting plate 21 so as to insulate these members from each other. The 2 nd insulator 65 has a predetermined plate thickness, and is provided with a through hole 65a communicating with the opening 3a of the battery cover 3 and through which the shaft portion 61c of the positive electrode terminal 61 is inserted. The 2 nd insulator 65 is integrally caulked and fixed to the battery cover 3 together with the positive electrode connecting electrode 67 by the caulking portion 61 e.
The 2 nd insulator 65 is provided with a recess 65b communicating with the through hole 65a and accommodating the positive electrode connecting electrode 67 and the conductive plate 68. The recess 65b is provided in a recessed manner on the lower surface of the 2 nd insulator 65, and communicates with the other space portion inside the battery.
The conductive plate 68 has: a dome-shaped diaphragm portion 68a that gradually decreases in diameter as it moves in the axial direction; and an annular flange portion 68b that extends radially outward from the outer peripheral edge portion of the diaphragm portion 68 a. The diaphragm portion 68a gradually decreases in diameter as it moves in the axial direction in a direction away from the lower surface 67b of the positive electrode connecting electrode 67, and has a curved surface portion having an arc shape with a convex cross section at least in a part in the axial direction, and in the present embodiment, has a hemispherical shape with a semi-elliptical cross section. The diaphragm portion 68a covers the through hole 61d opened in the lower surface 67b of the positive electrode connecting electrode 67 so as to face the opening end of the through hole 61d, and the flange portion 68b is joined to and hermetically sealed with the lower surface 67b of the positive electrode connecting electrode 67 to partition a space outside the battery and a space inside the battery, which are communicated with each other through the through hole 61 d.
When the internal pressure of the battery container 2 is higher than a preset upper limit value, the diaphragm portion 68a deforms in a direction to decrease the protruding height thereof due to a pressure difference with the outside of the battery container 2, breaks the fragile portion 25 of the positive electrode current collector plate 21, separates the joint portion 24 joined to the conductive plate 68 from the base portion 22 of the positive electrode current collector plate 21, and cuts off the current path, thereby functioning as the current cutoff mechanism of the present invention.
The flange portion 68b provided on the outer peripheral edge portion of the diaphragm portion 68a has a ring shape, extends along a single plane toward the radial outside, is continuous with a constant width over the entire circumference, and is connected to the lower surface of the positive electrode connecting electrode 67, and is continuously joined to the lower surface 67b of the positive electrode connecting electrode 67 over the entire circumference by laser welding to achieve hermetic sealing.
The material, plate thickness, cross-sectional shape, and the like of the diaphragm portion 68a are set so that the joint portion 24 can be held at the position separated from the positive current collector plate 21 by plastic deformation even after the internal pressure of the battery container 2 is reduced. The top portion of the diaphragm portion 68a, i.e., the center portion 68c, is joined to the joint 24 of the positive current collector plate 21 by laser welding. The joining of the central portion 68c may be performed by resistance welding or ultrasonic welding, in addition to laser welding.
The positive current collector plate 21 is attached and fixed to the 2 nd insulator 65. As shown in fig. 5, the positive electrode current collector plate 21 has a flat plate-shaped base portion (upper surface flat portion) 22 extending in parallel to the lower surface of the battery cover 3, and a plurality of support holes 22b are formed therethrough so as to be arranged at predetermined intervals from each other. The base portion 22 is provided with a pair of edges 22a, and the pair of edges 22a are formed by bending in a direction separating from the battery cover 3 along a pair of long sides to improve rigidity and maintain a planar shape. The pair of bonding tabs 23 of the positive electrode collector plate 21 are provided so as to protrude continuously from the respective edges 22 a.
The positive current collector plate 21 is joined to and fixed integrally with the 2 nd insulator 65 by inserting a plurality of projecting portions 65c projecting toward the lower surface of the 2 nd insulator 65 into the respective support holes 22b of the base 22 and thermally fusing the tips of the projecting portions 65 c.
The positive electrode current collector plate 21 is provided with a joint portion 24 joined to the central portion 68c of the conductive plate 68. The joint portion 24 is formed of a thin portion obtained by thinning a part of the base portion 22. The weak portion 25 is configured by providing a groove portion in the thin portion so as to surround the periphery of the joint portion 24, and is blocked by the conductive plate 68 that deforms outward of the battery when the battery is pressurized, so that the joint portion 24 can be separated from the base portion 22.
The dimension and shape of the fragile portion 25 are set so as to have the following strength: when a force in a direction extending toward the battery cover 3 is applied along with the deformation of the conductive plate 68 caused by the increase in the internal pressure of the battery container 2, the battery is broken, and the battery is not broken in a normal use environment such as vibration during traveling. The center portion 68c of the conductive plate 68 and the joint portion 24 of the positive current collecting plate 21 are joined by laser welding, but resistance welding, ultrasonic welding, or the like may be used in addition thereto.
In the nonaqueous electrolyte secondary battery 1 of the present embodiment, a positive electrode active material layer (not shown, hereinafter simply referred to as a gas generation layer) that reacts to generate a gas when the battery voltage becomes equal to or higher than the maximum operating power of the nonaqueous electrolyte secondary battery 1 is provided in the positive electrode mixture layer unformed portion 41b or in one of the positive electrode current collecting plate 21 and the bonding sheet 23, which is a positive electrode terminal in the container. The current cut-off mechanism operates when the internal pressure of the battery container 2 rises due to the gas generated by the reaction of the gas generation layer.
In the nonaqueous electrolyte secondary battery 1 of the present embodiment, the positive electrode 41 is formed of a positive electrode current collector, a positive electrode mixture layer 41a formed on one surface or both surfaces of the positive electrode current collector, and a positive electrode mixture layer non-formed portion 41 b.
As the positive electrode current collector, a foil or plate, a carbon sheet, a carbon nanotube sheet, or the like of copper, aluminum, nickel, titanium, or stainless steel can be used as a single body. As the positive electrode current collector, a clad foil or the like made of 2 or more kinds of materials may be used as needed. The positive electrode current collector can have a thickness of 5 to 100 μm, and preferably has a thickness of 7 to 20 μm from the viewpoint of structure and performance.
The positive electrode mixture layer 41a is formed of the 1 st positive electrode active material, a conductive auxiliary agent, and a binder. As the 1 st positive electrode active material, a material selected from lithium composite oxides (LiNi) can be usedxCoyMnzO2(x+y+z＝1)、(LiNixCoyAlzO2(x + y + z ═ 1)), lithium iron phosphate (LiFePO)4(LFP)), and the like.
As the conductive auxiliary agent, at least one material selected from carbon black such as Acetylene Black (AB) and Ketjen Black (KB), carbon materials such as graphite powder, conductive metal powder such as nickel powder, and the like can be used.
As the binder, at least one material selected from the group consisting of cellulose-based polymers, fluorine-based resins, vinyl acetate copolymers, rubbers, and the like can be used. As the binder, specifically, at least one material selected from polyvinylidene fluoride (PVdF), Polyimide (PI), polyvinylidene chloride (PVdC), polyethylene oxide (PEO), and the like can be used.
The positive electrode mixture layer 41a can be formed by applying a positive electrode mixture slurry obtained by mixing the positive electrode active material, the conductive auxiliary agent, and the binder in an organic solvent such as N-methylpyrrolidone (NMP) to one surface or both surfaces of the positive electrode current collector and drying the applied positive electrode mixture slurry. The drying may also be carried out under reduced pressure.
The thickness and density of the positive electrode mixture layer 41a can be adjusted by appropriately applying pressure after the drying. The positive electrode mixture layer 41a formed on the positive electrode current collector is preferably set to 2.0 to 4.2g/cm in terms of good balance between energy density and input/output characteristics3The density of (b) is more preferably 2.6 to 3.2g/cm3The density of (c).
The negative electrode 42 is formed of a negative electrode current collector, a negative electrode mixture layer unformed portion 42b, and a negative electrode mixture layer 42a formed on one surface or both surfaces of the negative electrode current collector.
As the negative electrode current collector, a foil or plate, a carbon sheet, a carbon nanotube sheet, or the like of copper, aluminum, nickel, titanium, or stainless steel can be used in the form of a single body. As the negative electrode current collector, a clad foil made of 2 or more kinds of materials may be used as needed. The negative electrode current collector can have a thickness of 5 to 100 μm, and preferably has a thickness of 7 to 20 μm from the viewpoint of structure and performance.
The negative electrode mixture layer 42a is formed of a negative electrode active material, a conductive assistant, and a binder. As the negative electrode active material, one selected from soft carbon (graphitizable carbon), hard carbon (graphitizable carbon), and stone can be usedCarbon powder (amorphous carbon) such as ink (graphite), and Silica (SiO)x) Titanium composite oxide (Li)4Ti5O7、TiO2、Nb2TiO7) At least one material selected from tin composite oxide, lithium alloy, metallic lithium, and the like.
As the conductive auxiliary agent, at least one material selected from carbon black such as Acetylene Black (AB) and Ketjen Black (KB), carbon materials such as graphite powder, conductive metal powder such as nickel powder, and the like can be used.
As the binder, at least one material selected from the group consisting of cellulose-based polymers, fluorine-based resins, vinyl acetate copolymers, rubbers, and the like can be used. As the binder in the case of using an organic solvent as a solvent of the negative electrode mixture slurry described later, specifically, at least one material selected from polyvinylidene fluoride (PVdF), Polyimide (PI), polyvinylidene chloride (PVdC), polyethylene oxide (PEO), and the like can be used. In the case where an aqueous solvent is used as the solvent of the negative electrode mixture slurry, specifically, at least one material selected from styrene-butadiene rubber (SBR), acrylic-modified SBR resin (SBR-based latex), carboxymethyl cellulose (CMC), polyvinyl alcohol (PVA), Polytetrafluoroethylene (PTFE), hydroxypropyl methyl cellulose (HPMC), tetrafluoroethylene-hexafluoropropylene copolymer (FEP), and the like can be used.
The negative electrode mixture layer 42a can be formed by applying a negative electrode mixture slurry obtained by mixing the negative electrode active material, the conductive auxiliary agent, and the binder in an organic solvent such as N-methylpyrrolidone (NMP) or an aqueous solvent such as pure water to one surface or both surfaces of the negative electrode current collector and drying the applied slurry. The drying may also be carried out under reduced pressure.
The thickness and density of the negative electrode mixture layer 42a can be adjusted by appropriately applying pressure after the drying. The negative electrode mixture layer 42a formed on the negative electrode current collector is preferably set to 0.7 to 2.0g/cm in terms of good balance between energy density and input/output characteristics3The density of (b) is more preferably 1.0 to 1.7g/cm3The density of (c).
The electrolyte solution can be composed of a nonaqueous solvent and an electrolyte, and the concentration of the electrolyte is preferably in the range of 0.1 to 10 mol/L.
The nonaqueous solvent may be at least one aprotic solvent selected from carbonates, ethers, sulfones, lactones, and the like. As the aprotic solvent, specifically, at least one compound selected from Ethylene Carbonate (EC), Propylene Carbonate (PC), diethyl carbonate (DEC), dimethyl carbonate (DMC), Ethyl Methyl Carbonate (EMC), 1, 2-Dimethoxyethane (DME), 1, 2-Diethoxyethane (DEE), Tetrahydrofuran (THF), 2-methyltetrahydrofuran, dioxane, 1, 3-dioxolane, diethylene glycol dimethyl ether, ethylene glycol dimethyl ether, Acetonitrile (AN), propionitrile, nitromethane, N-Dimethylformamide (DMF), dimethyl sulfoxide, sulfolane, y-butyrolactone, and the like can be used.
As the electrolyte, a material selected from LiPF can be used6、LiBF4、LiClO4、LiN(SO2CF3)、LiN(SO2C2F5)2、LiCF3SO3、LiC4F9SO3、LiC(SO2CF3)3、LiF、LiCl、LiI、Li2O、Li3N、Li3P、Li10GeP2S12(LGPS)、Li3PS4、Li6PS5Cl、Li7P2S8I、LixPOyNz(x＝2y+3z－5、LiPON)、Li7La3Zr2O12(LLZO)、Li3xLa2/3- xTiO3(LLTO)、Li1+xAlxTi2-x(PO4)3(LATP)、Li1.5Al0.5Ge1.5(PO4)3(LAGP)、Li1+x+yAlxTi2-xSiyP3- yO12、Li1+x+yAlx(Ti，Ge)2-xSiyP3-yO12、Li4-2xZnxGeO4(LISICON) and the like, preferablyLiPF (selective catalytic reduction)6、LiBF4Or mixtures thereof.
Examples of the separators 43 and 44 include films made of resins such as Polyethylene (PE), polypropylene (PP), polyester, cellulose, and polyamide, porous resin sheets such as nonwoven fabrics, and porous structures obtained by sintering inorganic materials or mixing inorganic materials with binders. As the inorganic material used in the porous structure, alumina (Al) can be used2O3) Silicon dioxide (SiO)2)、LiF、LiCl、LiI、Li2O、Li2S、Li3N、Li3P、Li10GeP2S12(LGPS)、Li3PS4、Li6PS5Cl、Li7P2S8I、LixPOyNz(x＝2y+3z－5、LiPON)、Li7La3Zr2O12(LLZO)、Li3xLa2/3-xTiO3(LLTO)、Li1+ xAlxTi2-x(PO4)3(LATP)、Li1.5Al0.5Ge1.5(PO4)3(LAGP)、Li1+x+yAlxTi2-xSiyP3-yO12、Li1+x+yAlx(Ti，Ge)2-xSiyP3-yO12、Li4-2xZnxGeO4(LISICON) and the like.
The separators 43 and 44 can be formed using at least one material selected from the porous resin sheet and the porous structure. The separators 43 and 44 have a single-layer structure when formed of only 1 of the above-mentioned materials, and may have a structure in which the materials are laminated or may be mixed when formed of 2 or more materials.
The gas generation layer is formed of a 2 nd positive electrode active material that generates a gas, a conductive auxiliary agent, and a binder. As the 2 nd positive electrode active material, the same material as that of the 1 st positive electrode active material, particularly, the material having a high reaction potential and being the same as that of the electrolyte solution, can be usedFrom the viewpoint of high reactivity of (A) and easy generation of gas, LiNi is preferred0.5Mn1.5O4(LNMO). As the conductive aid or the binder used for the gas generation layer, the same one as that used for the positive electrode mixture layer 41a can be used.
The gas generation layer can be formed by applying a gas generation slurry obtained by mixing the 2 nd positive electrode active material, the conductive auxiliary agent, and the binder in an organic solvent such as N-methylpyrrolidone (NMP) to the positive electrode mixture layer non-formed portion 41b of the positive electrode current collector and drying the applied gas generation slurry. The drying may also be carried out under reduced pressure.
The gas generation layer may be formed by bonding the crystal or sintered body of the 2 nd positive electrode active material to the positive electrode mixture layer unformed portion 41b of the positive electrode current collector or at least one member of the positive electrode terminals 21 and 23 in the container.
In the present embodiment, the nonaqueous electrolyte secondary battery 1 has the following structure: an electrode body element 40 is housed in a battery container 2 made of an aluminum alloy including a battery can 4 having a square deep-drawn shape and a battery cover 3 sealing an opening 4a of the battery can 4. However, the nonaqueous electrolyte secondary battery 1 is not limited to the configuration of the present embodiment, and aluminum, steel, stainless steel, or the like can be used as a material, and a cylindrical shape, a rectangular shape, a button battery, a pouch shape (laminate type), or the like can be used as a container shape.
In the present embodiment, the diaphragm portion 68a that deforms in response to an increase in the internal pressure of the battery container 2 to break the frangible portion 25 of the positive electrode current collector plate 21 is used as the current interruption means, but the current interruption means may be any configuration as long as it can interrupt the current supply to the container exterior from the container internal positive electrode terminals 21 and 23 or the container internal negative electrode terminals 22 and 24 in response to an increase in the internal pressure of the battery container 2. The operating pressure of the current cutoff mechanism may be, for example, in the range of 0.1 to 5MPa, preferably in the range of 0.5 to 2.2 MPa.
Next, examples of the present invention and comparative examples will be described.
Examples
[ example 1]
In this example, first, LiNi as the 1 st positive electrode active material was usedxCoyMnzO2(x + y + z is 1, x: y: z is 6: 2: 2, hereinafter abbreviated as NCM622), Acetylene Black (AB) as a conductive aid, and polyvinylidene fluoride (PVdF) as a binder to be NCM 622: AB: PFdV 94: 3: 3 (mass ratio) was mixed with N-methylpyrrolidone (NMP), and the solid content ratio was adjusted to 55 mass%, thereby preparing a positive electrode mixture slurry. Next, an aluminum foil 15 μm thick was used as a positive electrode current collector, and the positive electrode mixture slurry was applied to the positive electrode current collector and dried to form a positive electrode mixture slurry of 24mg/cm2The positive electrode mixture layer 41 a.
Next, LiNi, which is the 2 nd positive electrode active material of the generated gas, was used0.5Mn1.5O4(LNMO), Acetylene Black (AB) as a conductive aid, and polyvinylidene fluoride (PVdF) as a binder to become LNMO: AB: PFdV 94: 3: 3 (mass ratio) was mixed with N-methylpyrrolidone (NMP), and the solid content ratio was adjusted to 55 mass%, thereby preparing a gas generating slurry. Then, the gas generation slurry was applied to the positive electrode mixture layer non-formation portion 41b of the positive electrode collector and dried to form a positive electrode mixture layer of 12mg/cm2The gas generating layer of (1).
Next, the positive electrode current collector including the positive electrode mixture layer 41a and the gas generation layer was dried and pressurized, and the electrode density of the positive electrode mixture layer 41a was adjusted to 3.2g/cm3And a positive electrode 41 is formed.
Next, graphite powder (Gr.) as a negative electrode active material, Styrene Butadiene Rubber (SBR) as a binder, and carboxymethyl cellulose (CMC) were mixed so as to be Gr.: SBR: CMC 98: 1: 1 (mass ratio) was mixed with pure water, and the solid content ratio was adjusted to 50 mass% to prepare a negative electrode mixture slurry. Next, a copper foil having a thickness of 8 μm was used as a negative electrode current collector, and the negative electrode mixture slurry was applied to the negative electrode current collector and dried to form a negative electrode mixture slurry of 2mg/cm2The negative electrode mixture layer 42 a. Next, the negative electrode current collector provided with the negative electrode mixture layer 42a was dried and pressed, and the electrode density of the negative electrode mixture layer 42a was adjusted to 1.5g/cm3And a negative electrode 42 is formed.
Next, as shown in FIG. 3, the alumina (Al) is added2O3) And a separator 43, 44 formed of a two-layer structure of Polyethylene (PE), and a positive electrode 41 and a negative electrode 42 are respectively disposed between them and wound in a flat shape, thereby forming an electrode body element 40. Next, the positive electrode collector end of the electrode element 40 and the joining piece 23 of the positive electrode collector plate 21 and the negative electrode collector end and the joining piece 24 of the negative electrode collector plate 22 were joined by ultrasonic welding, respectively, to form the power generating element assembly 5.
Next, the periphery of the electrode body element 40 is covered with an insulating sheet (not shown) and inserted into the battery can 4, the opening 4a of the battery can 4 is closed with the battery cover 3, and the battery cover 3 and the battery can 4 are joined and sealed by laser welding. Then, an electrolyte solution is injected into the battery container 2 from the injection port 12, the injection port 12 is closed with the injection plug 11, and the battery cover 3 is joined and sealed by laser welding, thereby forming the lithium ion secondary battery 1. As the electrolyte, a solution prepared by mixing Ethylene Carbonate (EC), Ethyl Methyl Carbonate (EMC), and dimethyl carbonate (DMC) in an amount of EC: EMC: DMC 3: 4: 3 in a mixed solvent obtained by mixing the components in a volume ratio of LiPF as a supporting electrolyte6And a nonaqueous electrolytic solution obtained by dissolving the compound in a concentration of 1.2 mol/L.
Next, the device energy density of the lithium ion secondary battery 1 obtained in the present example was calculated from the battery capacity in the range of 2.5 to 4.2V at a current value corresponding to 0.33C. The results are shown in Table 1.
Next, the lithium ion secondary battery 1 obtained in the present example was subjected to an overcharge test of 2 times the maximum battery capacity (SOC 200%) at a current value corresponding to 1C, and the overcharge SOC and voltage at the time when the pressure at which the current cut-off mechanism was operated was reached were measured. The results are shown in Table 1.
[ example 2 ]
In this example, a lithium ion secondary battery 1 was formed in exactly the same manner as in example 1, except that the negative electrode 42 and the electrolytic solution were prepared as follows.
First, Lithium Titanate (LTO) as a negative electrode active material, Acetylene Black (AB) as a conductive additive, and polyvinylidene fluoride (PVdF) as a binder are mixed to become LTO: AB: PVdF 96: 2: 2 (mass ratio) was mixed with N-methylpyrrolidone (NMP), and the solid content ratio was adjusted to 55 mass%, thereby preparing a negative electrode mixture slurry. Next, an aluminum foil 15 μm thick was used as a negative electrode current collector, and the negative electrode mixture slurry was applied to the negative electrode current collector to form 42mg/cm2The negative electrode mixture layer 42 a. Next, the negative electrode current collector provided with the negative electrode mixture layer 42a was dried and pressed, and the electrode density of the negative electrode mixture layer 42a was adjusted to 2.1g/cm3And a negative electrode 42 is formed.
Next, as an electrolyte, Propylene Carbonate (PC) and diethyl carbonate (DEC) were mixed in a ratio of PC: DEC ═ 2: 1 volume ratio of LiPF as a supporting electrolyte in a mixed solvent6Dissolved at a concentration of 1.2 mol/L to form a nonaqueous electrolytic solution.
Next, the lithium ion secondary battery 1 obtained in the present example was measured for overcharge SOC and voltage at the time when the current cutoff mechanism reached the operating pressure, while calculating the device energy density from the battery capacity in the range of 1.5 to 2.7V at the current value corresponding to 0.33C, in exactly the same manner as in example 1. The results are shown in Table 1.
[ comparative example 1]
In this comparative example, a lithium ion secondary battery 1 was formed in exactly the same manner as in example 1, except that the gas generating layer was not formed at all.
Next, the lithium ion secondary battery 1 obtained in this comparative example was measured for overcharge SOC and voltage at the time when the energization shutoff mechanism reached the operating pressure, while calculating the cell energy density in exactly the same manner as in example 1. The results are shown in Table 1.
[ comparative example 2 ]
In this comparative example, a lithium ion secondary battery 1 was formed in exactly the same manner as in example 2, except that the gas generating layer was not formed at all.
Next, the lithium ion secondary battery 1 obtained in this comparative example was measured for overcharge SOC and voltage at the time when the energization shutoff mechanism reached the operating pressure, while calculating the cell energy density in exactly the same manner as in example 2. The results are shown in Table 1.
[ Table 1]
Figure BDA0002740420430000161
NCM622：LiNixCoyMnzO2(x+y+z＝1，x：y：z＝6：2：2)
Gr.: graphite powder
LTO: lithium titanate
LMNO：LiNi0.5Mn1.5O4
Element volume energy density: Wh/L
Working SOC: is based on
Working voltage: v
As is apparent from table 1, in the lithium ion secondary batteries of examples 1 and 2 including the gas generation layer in the positive electrode mixture layer non-formation portion 41b, the operating SOC and operating voltage of the current interruption mechanism are lower than those of the lithium ion secondary batteries of comparative examples 1 and 2 including no gas generation layer, although the volumetric energy densities of the respective elements are the same, and the current interruption mechanism can be reliably operated during overcharge without degrading the battery performance.
Description of the reference numerals
1 … nonaqueous electrolyte secondary battery, 2 … battery container, positive electrode terminal in container 21, 23 …, negative electrode terminal in container 22, 24 …, positive electrode 41 …, positive electrode mixture layer 41a …, positive electrode mixture layer 41b …, negative electrode 42 …, negative electrode 42a …, negative electrode mixture layer 42b …, and diaphragm portion 68b … (current cut-off mechanism).

Claims (5)

1. A nonaqueous electrolyte secondary battery is characterized by comprising, in a container: a positive electrode having a positive electrode mixture layer and a positive electrode current collector; an in-container positive electrode terminal electrically connected to the positive electrode mixture layer non-formed portion of the positive electrode current collector; a negative electrode having a negative electrode mixture layer and a negative electrode current collector; an in-container negative electrode terminal electrically connected to the negative electrode mixture layer unformed portion of the negative electrode current collector; a non-aqueous electrolyte; and an energization shutoff mechanism capable of shutting off energization between the positive electrode terminal in the container or the negative electrode terminal in the container and an outside of the container when an internal pressure of the container rises,
the positive electrode mixture layer non-formation portion or at least one member of the positive electrode terminal in the container is provided with a positive electrode active material layer that reacts at a voltage equal to or higher than the maximum operating power of the nonaqueous electrolyte secondary battery to generate a gas that can raise the internal pressure of the container and activate the current cutoff mechanism.
2. The nonaqueous electrolyte secondary battery according to claim 1, wherein the current interruption mechanism includes a shape variable member that is capable of deforming a shape when an internal pressure of the container rises, and the fragile portion is broken along with the deformation of the shape variable member, thereby interrupting the current supply from the inside of the container positive electrode terminal or the inside of the container negative electrode terminal to the outside of the container.
3. The nonaqueous electrolyte secondary battery according to claim 1, characterized in that the shape variable member is a diaphragm.
4. The nonaqueous electrolyte secondary battery according to claim 1, wherein the gas-generating positive electrode active material layer contains a positive electrode active material selected from lithium composite oxides (LiNi)xCoyMnzO2(x+y+z＝1)、(LiNixCoyAlzO2(x + y + z ═ 1)), lithium iron phosphate (LiFePO)4(LFP)).
5. According to claimThe nonaqueous electrolyte secondary battery according to claim 1, wherein the gas-generating positive electrode active material layer contains LiNi as a positive electrode active material0.5Mn1.5O4(LNMO)。
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