WO2022209067A1 - 回路基板アセンブリ - Google Patents

回路基板アセンブリ Download PDF

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Publication number
WO2022209067A1
WO2022209067A1 PCT/JP2021/047630 JP2021047630W WO2022209067A1 WO 2022209067 A1 WO2022209067 A1 WO 2022209067A1 JP 2021047630 W JP2021047630 W JP 2021047630W WO 2022209067 A1 WO2022209067 A1 WO 2022209067A1
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WIPO (PCT)
Prior art keywords
positive electrode
negative electrode
circuit board
battery
secondary battery
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2021/047630
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English (en)
French (fr)
Japanese (ja)
Inventor
英二 中島
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
NGK Insulators Ltd
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NGK Insulators Ltd
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Filing date
Publication date
Application filed by NGK Insulators Ltd filed Critical NGK Insulators Ltd
Priority to JP2023510254A priority Critical patent/JPWO2022209067A1/ja
Priority to EP21935216.8A priority patent/EP4318663A4/en
Publication of WO2022209067A1 publication Critical patent/WO2022209067A1/ja
Priority to US18/466,881 priority patent/US20240008185A1/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/18—Printed circuits structurally associated with non-printed electric components
    • H05K1/181—Printed circuits structurally associated with non-printed electric components associated with surface mounted components
    • 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
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • 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
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • 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
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • 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
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/425—Structural combination with electronic components, e.g. electronic circuits integrated to the outside of the casing
    • 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
    • H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/664—Ceramic materials
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/80—Porous plates, e.g. sintered carriers
    • H01M4/801—Sintered carriers
    • 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
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • 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
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/028—Positive electrodes
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
    • H01M50/105—Pouches or flexible bags
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/10—Details of components or other objects attached to or integrated in a printed circuit board
    • H05K2201/10007—Types of components
    • H05K2201/10037—Printed or non-printed battery
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/10—Details of components or other objects attached to or integrated in a printed circuit board
    • H05K2201/10007—Types of components
    • H05K2201/10098—Components for radio transmission, e.g. radio frequency identification [RFID] tag, printed or non-printed antennas
    • 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

Definitions

  • Patent Literature 1 discloses a circuit board assembly that includes a coin-type lithium secondary battery connected to a board by solder reflow, and a wireless communication device.
  • the invention of Patent Document 1 focuses on the problem that the performance of the battery deteriorates due to heating to a high temperature when fixing the battery to the substrate by solder reflow. They have also found that by adjusting the capacity of the positive electrode and the capacity of the negative electrode, it is possible to suppress deterioration in battery performance caused by heating.
  • circuit board assemblies incorporated in equipment are also required to be smaller.
  • the battery incorporated in the circuit board assembly be a highly reliable battery that can provide stable output over a long period of time even in a mode of use in which high-current pulse discharge is repeated for wireless communication or the like. ing.
  • one of the objects of the invention according to the present disclosure is to provide a circuit board assembly that is compact, has excellent durability, and has high output stability.
  • a circuit board assembly includes a wiring board, a lithium secondary battery electrically connected to the wiring board, and a wireless communication device electrically connected to the wiring board.
  • the lithium secondary battery includes a positive electrode, a negative electrode facing the positive electrode, and an electrolyte. Further, in the lithium secondary battery, the electrode area (S), which is the area where the positive electrode and the negative electrode face each other, and the battery resistance (R) are 0.08 ⁇ R/S ( ⁇ /cm 2 ) ⁇ 1. satisfies the .80 relationship.
  • circuit assembly it is possible to provide a circuit board assembly that is compact, has excellent durability, and has high output stability.
  • FIG. 1 is a schematic side view of a circuit board assembly
  • FIG. 2 is a schematic plan view showing a circuit board assembly
  • FIG. 3 is a schematic plan view showing the structure of a pouch-type lithium secondary battery.
  • FIG. 4 is a schematic cross-sectional view showing the structure of a pouch-type lithium secondary battery.
  • FIG. 5 is a graph showing the relationship between the electrode area (S) and the battery resistance (R) of the lithium secondary battery in the circuit board assembly.
  • FIG. 6 is a diagram showing the flow of manufacturing a pouch-type lithium secondary battery.
  • FIG. 7 is a diagram showing the evaluation circuit of the circuit board assembly.
  • a circuit board assembly of the present disclosure includes a wiring board, a lithium secondary battery electrically connected to the wiring board, and a wireless communication device electrically connected to the wiring board.
  • the lithium secondary battery includes a positive electrode, a negative electrode facing the positive electrode, and an electrolyte. Further, in the lithium secondary battery, the electrode area (S), which is the area where the positive electrode and the negative electrode face each other, and the battery resistance (R) are 0.08 ⁇ R/S ( ⁇ /cm 2 ) ⁇ 1. satisfies the .80 relationship.
  • the electrode area (S) refers to the area (cm 2 ) of the portion where the positive electrode and the negative electrode face each other in a lithium secondary battery. "Facing each other” includes not only a mode in which they are in direct contact with each other but also a mode in which they face each other via a separator or the like (the separator exists between the positive electrode and the negative electrode).
  • Battery resistance (R) refers to the internal resistance ( ⁇ ) of the battery measured by the method described later.
  • the circuit board assembly of the present disclosure includes a lithium secondary battery, and the ratio of the electrode area (S), which is the facing area of the positive electrode and the negative electrode in the lithium secondary battery, and the battery resistance (R), which is the internal resistance of the battery (R/S) is adjusted within a certain numerical range.
  • S the facing area of the positive electrode and the negative electrode in the lithium secondary battery
  • R the battery resistance
  • R/S the internal resistance of the battery
  • circuit board assembly of the present disclosure has an internal resistance (R/S) per electrode area of 0.08 or more, and the low resistance provides good pulse output performance, high cycle characteristics, and battery life. It is also very durable. As a result, highly functional and highly reliable circuit board assemblies suitable for a wide variety of applications and applications can be provided.
  • R/S internal resistance
  • the electrode area (S) may be 6 cm 2 or less. If the electrode area is 6 cm 2 or less, the overall size of the battery, including the exterior body, can be sufficiently reduced, and the battery is suitable for small-sized applications.
  • the lithium secondary battery may further include a separator provided between the positive electrode and the negative electrode, and may include, as the electrolyte, an electrolytic solution impregnated in the positive electrode, the negative electrode, and the separator. .
  • a separator provided between the positive electrode and the negative electrode, and may include, as the electrolyte, an electrolytic solution impregnated in the positive electrode, the negative electrode, and the separator.
  • the positive electrode includes a plate-shaped ceramic sintered body containing a lithium composite oxide in which a part of the composite oxide of lithium and a transition metal element is replaced with a replacement metal element that is another metal element. can be done.
  • a circuit board assembly having an R/S ( ⁇ /cm 2 ) of 0.08 or more and 1.80 or less can be stably and reliably obtained.
  • circuit board assembly 1 is a schematic side view of one embodiment of a circuit board assembly according to the present disclosure;
  • circuit board assembly 1 further includes battery 51 which is a lithium secondary battery, wiring board 21 , wireless communication device 22 , and other electronic components 23 .
  • the wiring board 21 is a so-called printed wiring board, and has conductive wiring on its upper surface. The wiring may be provided inside or on the lower surface of the wiring board 21 .
  • the wiring board 21 may have a structure in which a plurality of partial wiring boards are assembled.
  • a pouch-type lithium secondary battery is described as the battery 51, it is not limited to this.
  • the battery 51 may be a coin-type lithium secondary battery or an all-solid lithium secondary battery.
  • the battery 51 is fixed on the wiring board 21 .
  • a part or the whole of one surface of the exterior body 61 of the battery 51 is attached to the wiring board 21 using an adhesive or the like.
  • a positive tab terminal 57 of the battery 51 is connected to the wiring 11 by, for example, soldering.
  • Battery 51 and wiring board 21 are electrically connected by connecting positive electrode tab terminal 57 and wiring 11 .
  • the thickness of the circuit board assembly 1 is not particularly limited, it can be a thin circuit board assembly of, for example, 0.5 mm or less, more preferably 0.3 mm or less.
  • FIG. 2 is a schematic plan view showing one embodiment of a circuit board assembly according to the present disclosure.
  • the circuit board assembly 1 includes wirings 11 and 12 on which a battery 51, a wireless communication device 22, an electronic component 23 such as a capacitor, and an antenna 25 are printed on a wiring board 21. , 13 are electrically connected.
  • a battery 51 is used as a power source in the circuit board assembly 1 .
  • the size of the wiring board 21 constituting the circuit board assembly 1 is not particularly limited, it may be, for example, a rectangular resin board having a side length of about 50 mm to 80 mm. As an example, it may be a resin substrate having dimensions of about 50 mm ⁇ 80 mm.
  • the wireless communication device 22 may be an electric circuit module including an antenna and communication circuits. Terminals of the wireless communication device 22 can be connected to the wirings 12 and 13 of the wiring board 21 by solder or ACF (anisotropic conductive film). The terminals of the wireless communication device 22 and the wires are connected by soldering, for example, using a soldering iron. Also, the wireless communication device 22 may be a device that communicates using radio waves. The wireless communication device 22 may be a device dedicated to transmission or a device capable of transmitting and receiving.
  • circuits that generate signals to be transmitted include, for example, circuits that generate signals to be transmitted, circuits that process received signals, capacitors, sensors, various measuring devices, and external signals. Input terminals and the like are included.
  • the circuit board assembly 1 can be incorporated into various IoT devices. As an example, it can be embedded in a smart card with computing capabilities.
  • a smart card is a flexible card-like device.
  • a smart card is used, for example, as a card with fingerprint authentication/wireless communication functions including a wireless communication IC, a fingerprint analysis ASIC, and a fingerprint sensor.
  • FIGS. 3 and 4 show an extracted battery 51 that constitutes the circuit board assembly 1 according to the present disclosure.
  • FIG. 3 is a schematic plan view showing the configuration of the battery 51.
  • FIG. 4 is a schematic cross-sectional view showing the structure of the battery 51.
  • the actual configuration is partially enlarged, emphasized, and omitted for easy understanding. That is, the configurations shown in FIGS. 3 and 4 do not necessarily reflect actual dimensions.
  • battery 51 which is a lithium secondary battery, includes a pair of exterior films 62 and 63 forming exterior body 61, a battery body, a positive electrode tab terminal 57, and a negative electrode tab terminal 58. , provided.
  • the exterior films 62 and 63 have the same rectangular shape when viewed in the thickness direction. Peripheral edges on four sides of the exterior films 62 and 63 are joined to each other except for the portions facing each other with the positive electrode tab terminal 57 and the negative electrode tab terminal 58 interposed therebetween.
  • a specific mode of bonding is not particularly limited, but bonding can be performed, for example, by adhesion, fusion bonding, or the like.
  • the battery 51 is a small and thin battery.
  • the dimensions of the battery 51 are not particularly limited, but in plan view, the length in the vertical direction may be 10 to 46 mm, and the length in the horizontal direction may be 10 to 46 mm.
  • the thickness of the battery 51 may be, for example, 0.3 mm to 0.45 mm, preferably 0.4 mm to 0.45 mm.
  • the battery 51 is a sheet-like or flexible plate-like component as a whole.
  • the battery 51 includes a positive electrode 52 , a negative electrode 53 , a separator 54 , an electrolytic solution 55 , an exterior body 61 and two terminals 57 and 58 .
  • the positive electrode 52, the negative electrode 53, the separator 54, and the electrolytic solution 55 are collectively referred to as a battery main body.
  • the positive electrode 52, the negative electrode 53, and the separator 54 are stacked in a predetermined stacking direction. In the example shown in FIG. 4, the positive electrode 52, the separator 54 and the negative electrode 53 are stacked vertically in the figure.
  • the positive electrode 52 and the negative electrode 53 face each other with the separator 54 interposed therebetween.
  • the upper side and the lower side in FIG. 4 are referred to as the “upper side” and the “lower side” of the battery 51, respectively.
  • the vertical direction in FIG. 4 is referred to as “vertical direction” or “stacking direction”.
  • the exterior body 61 is a bag formed by joining the peripheral edges of exterior films 62 and 63 .
  • the exterior films 62 and 63 are respectively formed of laminate sheets in which metal foils 621 and 631 made of metal such as aluminum (Al) and insulating resin layers 622 and 632 are laminated.
  • metal foils 621 and 631 are arranged on the outside of the bag, and the resin layers 622 and 632 are arranged on the inside of the bag.
  • the exterior body 61 covers the entire battery body.
  • the exterior body 61 is a bag body, and accommodates the positive electrode 52, the negative electrode 53, the separator 54, and the electrolytic solution 55 inside.
  • the electrolytic solution 55 exists continuously around the positive electrode 52 , the separator 54 and the negative electrode 53 . In other words, the electrolytic solution 55 is interposed between the positive electrode 52 and the negative electrode 53 .
  • Electrolyte solution 55 impregnates positive electrode 52 , separator 54 and negative electrode 53 .
  • the positive electrode tab terminal 57 and the negative electrode tab terminal 58 extend from the inside of the exterior body 61 to the outside. Inside the exterior body 61 , the positive electrode tab terminal 57 is connected to the positive electrode current collector 521 . With this configuration, the positive tab terminal 57 is electrically connected to the positive electrode 52 .
  • the negative tab terminal 58 is connected to the negative current collector 531 . With this configuration, the negative tab terminal 58 is electrically connected to the negative electrode 53 .
  • the positive electrode tab terminal 57 and the negative electrode tab terminal 58 have a belt-like shape.
  • the positive electrode tab terminal 57 includes a main body portion made of a conductor and a protective layer made of resin arranged so as to cover the surface of the main body portion.
  • the negative electrode tab terminal 58 also includes a body made of a conductor and a protective layer made of resin arranged so as to cover the surface of the body.
  • Metals such as Al (aluminum) and Ni (nickel) can be used as the conductor forming the main body.
  • the separator 54 is arranged on the upper surface of the positive electrode 52 in the stacking direction.
  • the negative electrode 53 is arranged on the upper surface of the separator 54 . That is, the negative electrode 53 is arranged in contact with the upper surface side of the separator 54 , and the positive electrode 52 is arranged in contact with the lower surface side of the separator 54 .
  • Each of the positive electrode 52, the negative electrode 53, and the separator 54 has, for example, a rectangular shape in plan view.
  • the positive electrode 52 and the negative electrode 53 have approximately the same shape and size in plan view.
  • the separator 54 may have dimensions larger than those of the positive electrode 52 and the negative electrode 53 for the purpose of preventing internal short circuits.
  • the positive electrode 52 and the negative electrode 53 face each other almost entirely, except for misalignment that occurs during the manufacturing process or during use.
  • the dimensions and shape of the positive electrode 52 in plan view may be, for example, a rectangle with a side length of 9.75 mm to 28.5 mm. Preferably, it may be a rectangle with a side length of 18.15 mm to 25.5 mm.
  • the area of the positive electrode 52 in plan view ie, the area of the main surface of the positive electrode 52
  • the dimensions, shape and area of the negative electrode 53 may be similar to those of the positive electrode 52 .
  • the negative electrode 53 may be slightly larger (about 4 to 7%) than the positive electrode 52 . That is, the dimensions and shape of the negative electrode 53 in plan view (that is, the dimensions and shape of the main surface of the negative electrode 53) may be, for example, a rectangle with a side length of 10.45 mm to 29.2 mm. Preferably, it may be a rectangle with a side length of 18.8 mm to 26.15 mm.
  • the area of the negative electrode 53 in plan view (that is, the area of the main surface of the negative electrode 53) may be, for example, 109 mm 2 to 852 mm 2 , preferably 470 mm 2 to 852 mm 2 .
  • the area of the region where the positive electrode 52 and the negative electrode 53 face each other is defined as an electrode area (S).
  • the electrode area (S) may be, for example, between 95 mm 2 and 812 mm 2 , preferably between 329 mm 2 and 650 mm 2 . More preferably, it is 600 mm 2 (6 cm 2 ) or less. It is preferable that the positive electrode 52 and the negative electrode 53 are arranged so that the entire surfaces of the opposing surfaces face each other without any deviation from each other.
  • the electrode area (S) is preferably 90% or more, more preferably 96% or more, of the areas of the positive electrode 52 and the negative electrode 53 .
  • positive electrode 52 includes positive current collector 521 , positive electrode active material plate 522 , and conductive bonding layer 523 .
  • the positive electrode current collector 521 is a conductive sheet-like member.
  • the lower surface of the positive electrode current collector 521 is bonded to the resin layer 622 of the exterior body 61 via the positive electrode bonding layer 623 .
  • the positive electrode bonding layer 623 is made of, for example, a mixed resin of an acid-modified polyolefin resin and an epoxy resin.
  • the positive electrode bonding layer 623 may be made of other materials.
  • the thickness of the positive electrode bonding layer is, for example, 0.5 ⁇ m to 10 ⁇ m.
  • the positive electrode current collector 521 includes, for example, a metal foil made of metal such as aluminum, and a conductive carbon layer laminated on the upper surface of the metal foil. In other words, the main surface of the positive electrode current collector 521 facing the positive electrode active material plate 522 is covered with the conductive carbon layer.
  • the metal foil may be made of various metals other than aluminum (eg, copper, nickel, silver, gold, chromium, iron, tin, lead, tungsten, molybdenum, titanium, zinc, or alloys containing these). . Also, the positive electrode current collector 521 does not have to include the conductive carbon layer.
  • the positive electrode active material plate 522 is a thin plate-shaped ceramic sintered body containing lithium composite oxide. Preferably, the positive electrode active material plate 522 is substantially composed only of the lithium composite oxide. A separator 54 is laminated on the upper surface of the positive electrode active material plate 522 . Note that the positive electrode active material 522 may be sputtered with gold (Au) or the like as a current collection aid.
  • the positive electrode active material plate 522 has a structure in which a plurality of (that is, many) primary particles are bonded together.
  • the primary particles are composed of a lithium composite oxide having a layered rock salt structure.
  • a lithium composite oxide is a composite oxide of lithium and a transition metal element M (general formula: Li p MO 2 (where 0.05 ⁇ p ⁇ 1.10)), part of which is another metal element. It is substituted with a substituting metal element.
  • Transition metal element M includes, for example, one or more selected from cobalt (Co), nickel (Ni) and manganese (Mn).
  • the transition metal element M is the main one among the metals other than lithium contained in the lithium composite oxide, and is hereinafter referred to as "main transition metal element".
  • the lithium composite oxide is lithium cobalt oxide Li p CoO 2 (wherein 1 ⁇ p ⁇
  • the transition metal element M is, for example, magnesium (Mg), aluminum (Al), silicon (Si), calcium (Ca), titanium (Ti), vanadium (V), chromium (Cr), iron (Fe), copper ( Cu), zinc (Zn), gallium (Ga), germanium (Ge), strontium (Sr), yttrium (Y), zirconia (Zr), niobium (Nb), molybdenum (Mo), silver (Ag), tin ( Sn), antimony (Sb), tellurium (Te), barium (Ba), and bismuth (Bi). Titanium (Ti) or niobium (Nb) is preferred.
  • the layered rock salt structure is a crystal structure in which lithium layers and transition metal layers other than lithium are alternately laminated with oxygen layers interposed therebetween. That is, the layered rock salt structure is a crystal structure in which metal ion layers other than lithium and lithium single layers are alternately laminated via oxide ions. Typically, it has an ⁇ -NaFeO 2 type structure, that is, a structure in which a transition metal and lithium are regularly arranged in the [111] axis direction of a cubic rocksalt type structure.
  • the conductive bonding layer 523 contains conductive powder and a binder.
  • the conductive powder is, for example, powder such as acetylene black, flake natural graphite, carbon nanotube, carbon nanofiber, carbon nanotube derivative, or carbon nanofiber derivative.
  • the binder contains, for example, polyimide amide resin.
  • the polyimideamide resin contained in the binder may be of one type or two or more types. Also, the binder may contain a resin other than the polyimide amide resin.
  • the conductive bonding layer 523 is formed by coating the positive electrode current collector 521 or the positive electrode active material plate 522 with the above-described conductive powder, binder, and solvent-containing liquid or paste adhesive. and the positive electrode active material plate 522, the solvent evaporates and solidifies.
  • the thickness of the positive electrode current collector 521 is, for example, 9 ⁇ m to 50 ⁇ m, preferably 9 ⁇ m to 20 ⁇ m, more preferably 9 ⁇ m to 15 ⁇ m.
  • the thickness of the positive electrode active material plate 522 is, for example, 15 ⁇ m to 200 ⁇ m, preferably 30 ⁇ m to 150 ⁇ m, more preferably 50 ⁇ m to 100 ⁇ m.
  • the thickness of the conductive bonding layer 523 is, for example, 3 ⁇ m to 28 ⁇ m, preferably 5 ⁇ m to 25 ⁇ m.
  • negative electrode 53 includes negative electrode current collector 531 and negative electrode active material layer 532 .
  • the negative electrode current collector 531 is a conductive sheet-like member.
  • the upper surface of the negative electrode current collector 531 is bonded to the resin layer 632 of the exterior body 63 via the negative electrode bonding layer 633 .
  • the negative electrode active material layer 532 is applied on the lower surface of the negative electrode current collector 531 . That is, the negative electrode 53 is a so-called coated electrode.
  • the negative electrode active material layer 532 faces the separator 54 in the vertical direction.
  • the negative electrode bonding layer 633 is formed of, for example, a mixed resin of an acid-modified polyolefin resin and an epoxy resin.
  • the negative electrode bonding layer 633 may be formed of various other materials.
  • the negative electrode current collector 531 is, for example, a metal foil made of metal such as copper.
  • the metal foil is made of various metals other than copper (for example, copper, stainless steel, nickel, aluminum, silver, gold, chromium, iron, tin, lead, tungsten, molybdenum, titanium, zinc, or alloys containing these, etc. ) may be formed by
  • the negative electrode active material layer 532 includes a resin-based binder and a carbonaceous material that is the negative electrode active material.
  • the carbonaceous material include natural graphite, artificial graphite, pyrolytic carbon, coke, baked resin, mesophase spherules, mesophase pitch, and the like.
  • a lithium-absorbing material may be used as the negative electrode active material instead of the carbonaceous material.
  • Lithium-absorbing substances include, for example, silicon, aluminum, tin, iron, iridium, or alloys, oxides or fluorides containing these.
  • the binder is, for example, styrene-butadiene rubber (SBR), polyvinylidene fluoride (PVDF) or mixtures thereof.
  • the thickness of the negative electrode current collector 531 is, for example, 5 ⁇ m to 25 ⁇ m, preferably 8 ⁇ m to 20 ⁇ m, more preferably 8 ⁇ m to 15 ⁇ m.
  • the thickness of the negative electrode active material layer 532 is, for example, 20 ⁇ m to 300 ⁇ m, preferably 30 ⁇ m to 250 ⁇ m, more preferably 30 ⁇ m to 150 ⁇ m.
  • the separator 54 is a sheet-like or thin plate-like insulating member.
  • the separator 54 is, for example, a single layer separator made of resin.
  • the resin for example, polyimide, polyester (eg, polyethylene terephthalate (PET)), cellulose, or the like can be used.
  • PET polyethylene terephthalate
  • the thickness of the separator 54 is, for example, 15 ⁇ m or more, preferably 18 ⁇ m or more, and more preferably 20 ⁇ m or more. Also, the thickness of the separator 54 is, for example, 31 ⁇ m or less, preferably 28 ⁇ m or less, and more preferably 26 ⁇ m or less.
  • the separator By increasing the thickness of the separator, even when lithium dendrites (lithium dendrites) are deposited, short circuits between the positive electrode and the negative electrode due to the lithium dendrites can be prevented. Also, by making the separator thinner, the electrolyte and lithium ions can easily permeate, and the internal resistance of the battery 51 can be reduced.
  • the structure of the separator 54 can be changed to a known structure other than the above.
  • a mode in which two layers or three layers or more of ceramic and resin are laminated may be used.
  • it may be a microporous membrane formed only of ceramic.
  • the ceramic is, for example, at least one selected from MgO, Al2O3 , ZrO, SiC , Si3N4 , AlN and cogenerite , preferably at least one selected from MgO , Al2O3 and ZrO2. It is one type.
  • the electrolytic solution 55 is a liquid obtained by adding an electrolyte and an additive to a solvent.
  • the electrolyte is, for example, lithium hexafluorophosphate (LiPF 6 ).
  • the LiPF 6 concentration in the electrolytic solution 55 may be, for example, 0.5 to 2.0 mol/L, preferably 0.75 mol/L to 1.5 mol/L, more preferably 1.0 mol/L to 1.25 mol/L. is L.
  • the electrolyte may vary and may be, for example, lithium borofluoride (LiBF 4 ).
  • the solvent of the electrolytic solution 55 is, for example, ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), diethyl carbonate (DEC), ethyl methyl carbonate (EMC), ⁇ -butyrolactone (GBL), methyl butyrate. (MB), propyl acetate (PA) and other non-aqueous solvents.
  • Solvents may be solvents including, for example, EC and EMC.
  • the battery 51 is a pouch-type lithium secondary battery containing electrolyte as described above, the battery used in the circuit board assembly of the present disclosure may be another type of lithium secondary battery.
  • the battery used in the circuit board assembly of the present disclosure may be another type of lithium secondary battery.
  • it may be a coin-type lithium secondary battery or an all-solid lithium secondary battery.
  • the all-solid lithium secondary battery includes an oriented positive electrode plate as a positive electrode, a solid electrolyte member, and a negative electrode plate as a negative electrode.
  • the oriented positive electrode plate in the all-solid lithium secondary battery may be a lithium composite oxide sintered plate having a porosity of 0% or more and 10% or less.
  • This lithium composite oxide sintered plate contains a plurality of primary particles composed of a lithium composite oxide, and the plurality of primary particles has an average orientation angle of more than 0° and 30° or less with respect to the plate surface of the oriented positive electrode plate. It may be a so-called "low-angle oriented positive electrode plate” oriented at .
  • the solid electrolyte member may contain a solid electrolyte represented by 3LiOH ⁇ Li 2 SO 4 .
  • the negative electrode plate is a negative electrode plate capable of intercalating and deintercalating lithium ions at 0.4 V (vs. Li/Li + ) or higher, and may contain Ti.
  • Exterior films 62 and 63 constituting exterior body 61 two aluminum laminate films (manufactured by Showa Denko Packaging, thickness 61 ⁇ m, three-layer structure of polypropylene film/aluminum foil/nylon film) are used. is prepared.
  • a positive electrode active material plate 522 is prepared.
  • the main transition metal element of the lithium composite oxide of the positive electrode active material plate 522 can be Co, and the substituting metal element can be Nb.
  • the positive electrode active material plate 522 is one plate-like member.
  • the positive electrode active material plate 522 is manufactured by, for example, a so-called green sheet process.
  • a mixed powder of an oxide of lithium and an oxide of a main transition metal element eg, Co
  • Co 3 Li 4 powder manufactured by Seido Chemical Industry Co., Ltd.
  • Li 2 CO 3 powder manufactured by Honjo Chemical Co., Ltd.
  • the aforementioned Li/Co molar ratio may be changed as appropriate, for example, within the range of 1.00 to 1.05.
  • the holding temperature and holding time of the mixed powder can also be changed as appropriate.
  • Nb 2 O 5 powder (manufactured by Mitsui Kinzoku Mining Co., Ltd.) is added to the mixed powder, and pulverized and pulverized in a pot mill so that the volume-based D50 particle size becomes a particle size distribution of 0.8 ⁇ m.
  • the particle size distribution can be measured by, for example, Microtrac MT3000II (manufactured by Microtrac Bell Co., Ltd.).
  • the addition ratio of the Nb 2 O 5 powder to the raw material powder is 0.03% by mass. About 70% of the added Nb 2 O 5 corresponds to the Nb element from the atomic weight ratio of the constituent elements of Nb 2 O 5 .
  • the content of Nb in the raw material powder is 0.021% by mass.
  • the volume-based D50 particle size of the raw material powder may be changed as appropriate, for example, within the range of 0.2 ⁇ m to 10 ⁇ m.
  • the content of Nb in the raw material powder may also be appropriately changed, for example, within the range of 0.1% by mass to 2.0% by mass.
  • a dispersion medium (2-ethylhexanol)
  • a binder product number BLS, manufactured by Sekisui Chemical Co., Ltd.
  • a plasticizer DOP: diphthalic acid ( 2-ethylhexyl), manufactured by Kurogane Kasei Co., Ltd.
  • a dispersant product number Marialim SC0505K, manufactured by NOF Corporation
  • a slurry is prepared by stirring the obtained mixture under reduced pressure to remove air bubbles and adjusting the viscosity to 4000 cP to 1000 cP.
  • the composition and type of the various raw materials in the slurry may be changed as appropriate. Viscosity can be measured with an LVT viscometer manufactured by Brookfield.
  • a lithium compound other than LiCoO 2 for example, lithium carbonate
  • a lithium compound other than LiCoO 2 for example, lithium carbonate
  • a green sheet is formed by forming the slurry into a sheet on a polyethylene terephthalate (PET) film by a doctor blade method.
  • PET polyethylene terephthalate
  • the thickness of the green sheet after drying is, for example, about 105 ⁇ m.
  • the thickness of the green sheet may be changed as appropriate, for example, within the range where the thickness of the positive electrode active material plate 522 after firing is 15 ⁇ m to 200 ⁇ m as described above.
  • the green sheet peeled off from the PET film is cut into a predetermined size (eg, 68 mm square) by a cutter and placed in the center of the lower setter (eg, 90 mm square, 1 mm high).
  • An upper setter is placed on top of the green sheets on the lower setter.
  • the upper and lower setters are made of ceramics, preferably zirconia or magnesia. If the setter is made of magnesia, the pores of the positive electrode active material plate 522 tend to become smaller.
  • the upper setter may have a porous structure, a honeycomb structure, or a dense structure. If the upper setter is dense, the pores of the positive electrode active material plate 522 tend to be small and the number of pores tends to be large.
  • the green sheet is placed in, for example, a 120 mm square alumina sheath (manufactured by Nikkato Co., Ltd.) while being sandwiched between setters. At this time, the alumina sheath is not sealed, but is covered with a gap of a predetermined size (for example, 0.5 mm).
  • a predetermined size for example, 0.5 mm
  • the laminate of the green sheet and the setter is fired, for example, by raising the temperature to 900°C at a heating rate of 100°C/h and holding it for 15 hours. Thereafter, the sintered body cooled to room temperature is taken out from the alumina sheath to obtain the positive electrode active material plate 522 which is a sintered body plate.
  • the thickness of the positive electrode active material plate 522 is, for example, approximately 100 ⁇ m.
  • the sizes of the positive electrode active material plate 522 and the setter may be changed as appropriate.
  • the firing conditions for the positive electrode active material plate 522 may also be changed as appropriate.
  • the firing process may be performed in two steps, or may be performed in one step. When baking in two steps, the temperature of the first baking is preferably lower than the temperature of the second baking.
  • positive electrode active material plate 522 has a plurality of active material plate elements
  • the sintered body plate is cut into a predetermined size by a laser processing machine or the like to form a plurality of active material plate elements.
  • the average orientation angle of the primary particles in the positive electrode active material plate 522 is, for example, 16°.
  • the average orientation angle can be measured as follows. First, the positive electrode active material plate 522 was polished with a cross section polisher (IB-15000CP, manufactured by JEOL Ltd.), and the resulting cross section (that is, a cross section substantially perpendicular to the main surface of the positive electrode active material plate 522) was magnified 1000 times. EBSD measurement is performed in a field of view (125 ⁇ m ⁇ 125 ⁇ m) to obtain an EBSD image. The EBSD measurement is performed using, for example, a Schottky field emission scanning electron microscope (model JSM-7800F, manufactured by JEOL Ltd.).
  • the angle formed by the (003) plane of the primary particles and the main plane of the LiCoO 2 sintered plate (that is, the inclination of the crystal orientation from (003)) is obtained as the tilt angle, and the average value of these angles is taken as the average orientation angle of the primary particles.
  • the thickness of the positive electrode active material plate 522 is obtained by polishing the positive electrode active material plate 522 with a cross section polisher (IB-15000CP, manufactured by JEOL Ltd.), and observing the cross section obtained above with an SEM (JSM6390LA, JEOL Ltd. (manufactured). The thickness of the green sheet after drying can be measured in the same manner.
  • a cross section polisher IB-15000CP, manufactured by JEOL Ltd.
  • the porosity of the positive electrode active material plate 522 is, for example, 30%.
  • the porosity can be measured as follows. First, the positive electrode active material plate 522 was polished with a cross section polisher (IB-15000CP, manufactured by JEOL Ltd.), and the obtained cross section was observed with a SEM (125 ⁇ m ⁇ 125 ⁇ m) at a magnification of 1000 (125 ⁇ m ⁇ 125 ⁇ m). JSM6390LA). The obtained SEM image is analyzed, the area of all the pores is divided by the area of the positive electrode active material plate 522, and the obtained value is multiplied by 100 to calculate the porosity (%).
  • a cross section polisher IB-15000CP, manufactured by JEOL Ltd.
  • the average pore diameter of the positive electrode active material plate 522 is, for example, 0.8 ⁇ m.
  • the average pore diameter can be measured by a mercury intrusion method using a mercury porosimeter (manufactured by Shimadzu Corporation, Autopore IV9510).
  • the green sheets are sandwiched between the upper and lower setters. It may be calcined.
  • the calcination temperature and time are, for example, 600° C. to 850° C. and 1 hour to 10 hours.
  • the green sheet may be degreased prior to the temporary firing.
  • the upper setter is placed on the calcined body formed by calcining.
  • the raw material powder is obtained by adding the Nb 2 O 5 powder to the mixed powder of the Co 3 Li 4 powder and the Li 2 CO 3 powder and pulverizing it.
  • the raw material powder may be obtained by other methods.
  • powder of a composite oxide of lithium and a main transition metal element that is, LiCoO 2
  • Co 3 O 4 powder and Li 2 CO 3 powder are mixed and fired at 500° C. to 900° C. for 1 hour to 20 hours to synthesize LiCoO 2 powder.
  • the LiCoO 2 powder preferably comprises platelet-like particles (ie LiCoO 2 platelet-like particles).
  • the volume-based D50 particle size of LiCoO 2 powder is, for example, 0.3 ⁇ m to 30 ⁇ m.
  • LiCoO 2 powder can be obtained by a method of grain-growing a green sheet formed using a LiCoO 2 powder slurry and then pulverizing it, a flux method, a hydrothermal synthesis, a single crystal growth using a melt, a sol-gel method, etc. It can be obtained by various methods of synthesizing crystals.
  • the LiCoO 2 particles obtained by these methods are in a state in which they are easily cleaved along the cleavage plane, similarly to the LiCoO 2 particles described above. can be obtained easily.
  • Nb 2 O 5 powder 0.1% to 2.0% by mass of Nb 2 O 5 powder is added to the LiCoO 2 powder, and pulverized in a pot mill so that the volume-based D50 particle size becomes a particle size distribution of 0.2 ⁇ m to 10 ⁇ m. and pulverized to obtain a raw material powder.
  • the raw material powder plate-like LiCoO 2 particles capable of conducting lithium ions parallel to the plate surface are obtained by the above pulverization or the like.
  • Nb added before pulverization or the like is attached as Nb 2 O 5 or in another state.
  • the raw material powder may be mixed with other powder such as Co 3 O 4 particles.
  • the plate - like LiCoO2 particles function as template particles to provide orientation
  • the other powders e.g. , Co3O4 particles
  • the mixing ratio of template particles and matrix particles is preferably from 100:0 to 3:97.
  • the volume-based D50 particle size of the matrix particles is not particularly limited, but is, for example, 0.1 ⁇ m to 1.0 ⁇ m, and should be smaller than the volume-based D50 particle size of the template particles. is preferred.
  • Co 3 O 4 particles can also be obtained by heat-treating a Co(OH) 2 raw material at 500° C.-800° C. for 1-10 hours.
  • Co(OH) 2 particles may be used instead of Co 3 O 4 particles, or LiCoO 2 particles may be used.
  • LiCoO 2 particles are used as matrix particles, and when only template particles (LiCoO 2 particles) are used without matrix particles, firing produces large (e.g., 90 mm square) and flat LiCoO particles. 2 sintered plates can be obtained.
  • a conductive bonding layer 523 is formed on the positive electrode current collector 521 (for example, aluminum foil with a thickness of 9 ⁇ m).
  • the conductive bonding layer 523 is formed, for example, by dropping 2 ⁇ L of a slurry obtained by mixing acetylene black with a solution of polyamideimide (PAI) dissolved in N-methylpyrrolidone onto the positive electrode current collector 521 .
  • PAI polyamideimide
  • the positive electrode active material plate 522 is placed on the conductive bonding layer 523 and dried.
  • the positive electrode active material plate 522 is bonded to the positive current collector 521 via the conductive bonding layer 523 .
  • An end portion of the positive electrode tab terminal 57 is previously fixed to the positive electrode current collector 521 by welding.
  • electrode assembly a composite of the positive electrode current collector 521 and the positive electrode active material plate 522 is laminated on the first exterior film 62, and the positive electrode bonding layer 623 (see FIG. 4) ) to the exterior film 62 . According to these procedures, cathode assembly 20 is formed.
  • a negative electrode active material layer 532 (eg, 130 ⁇ m thick), which is a carbon layer, is applied onto the negative electrode current collector 531 (eg, 10 ⁇ m thick copper foil).
  • the negative electrode active material layer 532 is a carbon coating film containing a mixture of graphite as an active material and PVDF as a binder. The thickness and material of the negative electrode current collector 531 and the thickness and raw material of the negative electrode active material layer 532 may be changed as appropriate.
  • the composite of the negative electrode current collector 531 and the negative electrode active material layer 532 is laminated on the second exterior film 63 and bonded to the second exterior film 63 via the negative electrode bonding layer 633 (see FIG. 4). be done.
  • An end portion of the negative electrode tab terminal 58 is previously fixed to the negative electrode current collector 531 by welding. Following these procedures, the negative electrode assembly 30 is formed.
  • the separator 54 for example, a polyolefin porous film (manufactured by JNC Co., Ltd., S115) is prepared. Then, the positive electrode assembly 20 , the separator 54 and the negative electrode assembly 30 are laminated in order such that the positive electrode active material plate 522 and the negative electrode active material layer 532 face the separator 54 to form the intermediate laminate 10 .
  • the intermediate laminate 10 the upper and lower surfaces of the laminate of the positive electrode 52, the separator 54 and the negative electrode 53 (hereinafter also referred to as "battery element") are covered with an exterior body 61 (exterior films 62, 63). Exterior films 62, 63 extend around the battery element.
  • the vertical thickness of the battery element is, for example, 0.33 mm.
  • the shape of the battery element in plan view is, for example, a substantially rectangular shape of 23 mm ⁇ 32 mm.
  • the electrode area (S) in the present invention is determined in the lamination process described above.
  • the electrode area (S) is the area (cm 2 ) of the region where the positive electrode 52 and the negative electrode 53 face each other. is the area of the parts facing each other.
  • three sides out of the four sides of the substantially rectangular intermediate laminate 10 are sealed by thermal fusion bonding.
  • three sides other than the upper side in the drawing are sealed.
  • the three sides include one side from which the positive electrode tab terminal 57 and the negative electrode tab terminal 58 protrude.
  • a contact jig adjusted to have a sealing width of 2 mm is used, and the outer peripheral portion of the intermediate laminate 10 is heated at 200° C. and 1.5 MPa for 10 seconds. pressured.
  • the exterior films 62 and 63 of the exterior body 61 are heat-sealed.
  • the intermediate laminate 10 is housed in a vacuum dryer 81 to remove moisture and dry the adhesive (that is, the positive electrode bonding layer 623, the negative electrode bonding layer 633 and the conductive bonding layer 523). is done.
  • the intermediate laminate 10 is housed inside the glove box 82 .
  • An injection tool 83 is inserted between the exterior films 62 and 63 on one unsealed side of the intermediate laminate 10 , and the electrolyte 55 (see FIG. 4 ) is injected into the intermediate laminate 10 via the injection tool 83 .
  • the electrolytic solution 55 is, for example, a mixed solvent containing EC and EMC at a volume ratio of 3:7, in which LiPF 6 as an electrolyte is dissolved to a concentration of 1 mol/L, and further added as an additive. .
  • the solvent of the electrolyte solution 55, the type of electrolyte and additives, etc. may be changed variously.
  • the one unsealed side is temporarily sealed (that is, vacuum sealed) with a simple sealer under a reduced pressure atmosphere (for example, absolute pressure of 5 kPa) in the glove box 82. be.
  • a reduced pressure atmosphere for example, absolute pressure of 5 kPa
  • the intermediate laminate 10 is initially charged and aged for a predetermined period (for example, seven days).
  • a portion of the exterior films 62 and 63 near the outer edge of one temporarily sealed side is cut off. The cut is made at the end portion that does not overlap the battery element. Gas containing moisture and the like generated by aging is removed through the cut portion (Fig. 6, "venting gas").
  • the sides formed by the above cutting are sealed by thermal fusion bonding under a reduced pressure atmosphere (for example, absolute pressure of 5 kPa) in the glove box 82 .
  • a pressing jig adjusted so that the sealing width is 2 mm is used in the same manner as in the sealing of the three sides described above, and the exterior films 62 and 63 are sealed at 200° C. and 1.5 MPa. and pressure for 10 seconds.
  • the exterior films 62 and 63 are heat-sealed, and the lithium secondary battery 51 is formed.
  • the extra portion on the outer periphery of the outer package 61 is cut off, and the shape of the lithium secondary battery 1 is adjusted.
  • the lithium secondary battery 51 has a rectangular shape of 38 mm ⁇ 27 mm in plan view, a thickness of 0.45 mm or less, and a capacity of 30 mAh.
  • the substitution metal element of the positive electrode active material plate 522 is not limited to Nb, and may be Ti, for example.
  • An example of a method for manufacturing the positive electrode active material plate 522 in which the substitution metal element is Ti will be described below. First, similarly to the case where the substituting metal element is Nb, mixed powder of lithium oxide and main transition metal element (that is, Co) oxide is prepared and held at 800° C. for 5 hours.
  • TiO 2 powder (manufactured by Ishihara Sangyo Co., Ltd.) is added to the mixed powder, and pulverized and pulverized in a pot mill so that the volume-based D50 particle size has a particle size distribution of 0.8 ⁇ m. A powder is obtained.
  • the particle size distribution can be measured by Microtrac MT3000II (manufactured by Microtrac Bell Co., Ltd.).
  • the addition rate of TiO2 powder to the raw powder is 0.4% by mass.
  • About 60% of the added TiO 2 corresponds to the Ti element according to the atomic weight ratio of the constituent elements of TiO 2 . Therefore, the content of Ti in the raw material powder is 0.24% by mass.
  • the volume-based D50 particle size of the raw material powder may be appropriately changed, for example, within the range of 0.2 ⁇ m to 10 ⁇ m.
  • the content of Ti in the raw material powder may also be appropriately changed, for example, within the range of 0.1% by mass to 2.0% by mass.
  • the raw material powder, the dispersion medium, the binder, the plasticizer and the dispersant are mixed in the same manner as in Battery Production Example 1.
  • the resulting mixture is stirred under reduced pressure to remove air bubbles, and the viscosity is adjusted to prepare a slurry.
  • the composition and type of the various raw materials in the slurry may be changed as appropriate.
  • an excess lithium compound other than LiCoO 2 may be added to the slurry, as in Battery Production Example 1.
  • a positive electrode active material plate 522 containing Ti as a substitutional metal element is manufactured under the same method and under the same manufacturing conditions as in Battery Manufacturing Example 1. Specifically, first, the slurry is formed into a sheet on a PET film by a doctor blade method to form a green sheet. Subsequently, the green sheet peeled off from the PET film is cut into a predetermined size by a cutter. Then, the positive electrode active material plate 522 is obtained by firing the green sheet.
  • the obtained positive electrode active material plate 522 is combined with other members in the same manner as in Battery Production Example 1 to obtain the lithium secondary battery 51 .
  • the positive electrode 52 is not necessarily a sintered plate electrode having the positive electrode active material plate 522 which is a sintered ceramic plate, and may be a coated electrode like the negative electrode 53. good too.
  • the positive electrode 52 includes the positive electrode current collector 521 described above and a positive electrode active material layer coated on the positive electrode current collector 521 .
  • the positive electrode active material layer includes the lithium composite oxide, which is a positive electrode active material, and a resin-based binder.
  • the lithium composite oxide is a composite oxide of lithium and a main transition metal element (e.g., Co, Ni, Mn) partially substituted with a substitution metal element (e.g., Nb, Ti). It is.
  • the binder is, for example, styrene-butadiene rubber (SBR), polyvinylidene fluoride (PVDF) or mixtures thereof.
  • a method for manufacturing the positive electrode 2 when the positive electrode 52 is a coated electrode will be described below.
  • the case where the main transition metal element and the substituting metal element are Co and Nb respectively will be described.
  • a mixed powder of lithium oxide and main transition metal element (that is, Co) oxide is prepared. The mixed powder is held at 900° C. for 10 hours.
  • Nb 2 O 5 powder (manufactured by Mitsui Mining & Smelting Co., Ltd.) is added to the mixed powder, and the volume-based D50 particle size is 0 with a pot mill.
  • a raw material powder is obtained by pulverizing and pulverizing to a particle size distribution of 0.8 ⁇ m.
  • the addition ratio of the Nb 2 O 5 powder to the raw material powder was 0.03% by mass, and the content of Nb in the raw material powder was 0.021% by mass.
  • the volume-based D50 particle size of the raw material powder may be changed as appropriate, for example, within the range of 0.2 ⁇ m to 10 ⁇ m.
  • the content of Nb in the raw material powder may also be appropriately changed, for example, within the range of 0.1% by mass to 2.0% by mass.
  • the raw material powder 91% by mass of the raw material powder, 5% by mass of acetylene black, 4% by mass of polyvinylidene fluoride (PVDF), and an N-methylpyrrolidone (NMP) solution are mixed to prepare a slurry.
  • the slurry is applied onto the positive electrode current collector 521 (for example, aluminum foil with a thickness of 10 ⁇ m) and dried. After that, the dried coating layer is pressed to fabricate the positive electrode 52, which is a coated electrode.
  • the positive electrode current collector 521 for example, aluminum foil with a thickness of 10 ⁇ m
  • the obtained positive electrode 52 is combined with other members in the same manner as in Battery Production Example 1 to obtain a lithium secondary battery 51 .
  • Lithium secondary battery 51 and other parts are mounted on wiring board 21 to obtain circuit board assembly 1 .
  • a specific manufacturing process can be based on known methods and conditions, and is not particularly limited.
  • the exterior film 62 of the lithium secondary battery 51 is adhered onto the substrate, and then the positive electrode tab terminal 57 and the negative electrode tab terminal 58 of the lithium secondary battery 51 are connected to the wiring of the wiring board 21 by soldering.
  • components other than the lithium secondary battery 51, such as the terminals of the wireless communication device 22, can be connected to the wiring of the wiring board 21 by soldering.
  • Example 1 A lithium secondary battery was obtained according to the manufacturing method described in Battery Manufacturing Example 1. Aluminum was used as the conductor of the positive electrode tab terminal in the lithium secondary battery. Nickel was used as a conductor in the negative electrode tab terminal. The resulting lithium secondary battery was mounted on a wiring board to obtain a circuit board assembly. Sunbonder USM-560 and Cerasolzer Eco #155 (both manufactured by Kuroda Techno Co., Ltd.) were used as ultrasonic soldering devices for mounting the lithium secondary battery on the wiring board. Soldering was performed at 250°C.
  • the electrode area (S) is determined based on the design. It is also possible to confirm the dimension of the facing portion of the electrode and determine the electrode area by image recognition when the electrode is placed in the manufacturing process of the battery.
  • the electrode area was 6.0 cm2 .
  • a battery resistance (R) was measured for a circuit board assembly on which a lithium secondary battery or the like was mounted.
  • the internal resistance of the battery was measured by the AC impedance method using an electrochemical measurement system (model number: VMP-3, manufactured by BioLogic).
  • the resistance value ( ⁇ ) at 10 Hz was read from the obtained Cole-Cole plot.
  • the internal resistance was measured with an amplitude of 2 mV and a measurement frequency range of 250 kHz to 200 mHz.
  • the measurement was performed by pressing an Au-plated probe pin against a pad portion on the circuit board terminal side.
  • the battery resistance was 0.5 ⁇ .
  • Example 2-4 Comparative Examples 1-2
  • a circuit board assembly was produced in the same manner as in Example 1 except that the electrode area (S), battery resistance (R), and battery resistance per electrode area (R/S) were as shown in Table 1.
  • FIG. 5 is a graph showing the relationship between electrode area (S) and battery resistance (R).
  • the circuit in FIG. 7 can be configured for evaluation.
  • a resistor 92 manufactured by BECKMAN, AR500L25
  • a relay switch 93 manufactured by Omron Corporation, G2R-1-SN DC24
  • the input side of the relay switch 93 is connected to a stabilized power supply 94 (PMX500-0.1A manufactured by Kikusui Electric Industry Co., Ltd.) and an electronic load device 95 (PLZ-30F manufactured by the same company).
  • a voltmeter 96 (manufactured by Hioki Denki Co., Ltd., MR8870) is connected to the input side of the DC-DC converter 91 to check the output current of the DC-DC converter 91.
  • An ammeter 97 (manufactured by the same company, CT6700) is connected to the output side of the DC-DC converter 91 .
  • pulse output is repeated 10 times with a 1-s rest after a 1-s current of 140 mA.
  • a voltage drop amount (iR drop) of all pulse waveforms at this time is measured.
  • the capacity retention rate (%) was obtained by dividing the discharge capacity after 300 cycles of charging and discharging by the initial discharge capacity. When the capacity retention rate was 90% or more, the cycle characteristics were judged to be good ( ⁇ ). When the capacity retention rate was less than 90%, the cycle characteristics were judged to be insufficient (x).

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