US20120045692A1 - Electrical Appliance - Google Patents

Electrical Appliance Download PDF

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Publication number
US20120045692A1
US20120045692A1 US13/211,577 US201113211577A US2012045692A1 US 20120045692 A1 US20120045692 A1 US 20120045692A1 US 201113211577 A US201113211577 A US 201113211577A US 2012045692 A1 US2012045692 A1 US 2012045692A1
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Prior art keywords
dimensional carbon
electrical appliance
active material
carbon
electrode
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Abandoned
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US13/211,577
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English (en)
Inventor
Yasuhiko Takemura
Tamae Moriwaka
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Semiconductor Energy Laboratory Co Ltd
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Semiconductor Energy Laboratory Co Ltd
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Assigned to SEMICONDUCTOR ENERGY LABORATORY CO., LTD. reassignment SEMICONDUCTOR ENERGY LABORATORY CO., LTD. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: MORIWAKA, TAMAE, TAKEMURA, YASUHIKO
Publication of US20120045692A1 publication Critical patent/US20120045692A1/en
Priority to US14/471,906 priority Critical patent/US10044027B2/en
Abandoned legal-status Critical Current

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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
    • 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
    • H01M4/139—Processes of manufacture
    • H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • 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
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0407—Methods of deposition of the material by coating on an electrolyte layer
    • 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
    • H01M4/362—Composites
    • H01M4/366—Composites as layered products
    • 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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B15/00—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00
    • 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
    • H01M4/60—Selection of substances as active materials, active masses, active liquids of organic compounds
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • H01M4/625—Carbon or graphite
    • 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
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • 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
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • H01M50/491—Porosity
    • 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
    • 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

Definitions

  • the present invention relates to a variety of electrical appliances, particularly a battery, including a particulate material.
  • a particulate material is used as an active material for storing electricity.
  • a conduction auxiliary agent such as acetylene black, graphite particles, or carbon fibers is mixed into the material so as to increase the conductivity (see Patent Document 1).
  • the active material particles, the conduction auxiliary agent, and a binder are mixed, and the mixture is applied onto a current collector, molded, and then dried to be used as an electrode such as a positive electrode or a negative electrode.
  • a procedure similar to the above is applied to other electrical appliances including a particulate material, without limitation to a battery, to improve its conductivity.
  • graphite when used as a conduction auxiliary agent for a positive electrode of a battery, such as a lithium ion battery, in which charge and discharge are performed by transfer of alkali ions, there is a problem in that graphite particles absorb the alkali ions, thereby decreasing the use efficiency of current.
  • acetylene black contains fewer impurities and has a better developed chain structure than graphite particles and therefore has excellent electrolyte retention characteristics, thereby improving the use efficiency of an active material.
  • a battery including acetylene black as a conduction auxiliary agent has a disadvantage that the potential and discharge capacitance are greatly reduced, since a functional group having a high reducing property with respect to an active material exists on a surface of acetylene black.
  • FIG. 2 schematically illustrates an example where acetylene black is used as a conduction auxiliary agent.
  • particles shown by oblique lines are active material particles and black dots are acetylene black particles. The above problem is also caused in the case where graphite particles are used.
  • the conductivity can be improved by using two-dimensional carbon including 1 to 100, preferably 1 to 10 graphenes as a conduction auxiliary agent.
  • a graphene refers to a sheet of carbon molecules having sp 2 bonds with a thickness of one atomic layer.
  • FIG. 1 is a schematic view illustrating the case where such a conduction auxiliary agent extending two-dimensionally is used.
  • three sheets of two-dimensional carbon and a large number of active material particles form a complicated structure, whereby the conductivity can be increased.
  • the volume of the conduction auxiliary agent occupying the electrode can be reduced, whereby the volume of the electrode can be reduced.
  • the thickness of two-dimensional carbon including 10 graphenes is about 3 nm.
  • a graphene has a characteristic of achieving high conductivity after being subjected to doping treatment. A value of greater than or equal to 10 6 S/cm is obtained, which is higher than or equal to the conductivity of silver. This fact is advantageous in using the graphene as a conduction auxiliary agent. Doping can be performed by partly oxidizing the graphene or adding an alkali metal such as potassium to the graphene.
  • a conduction auxiliary agent including two-dimensional carbon is used for an electrical appliance, such as a lithium ion secondary battery, in which charge and discharge are performed by transfer of alkali metal ions or alkaline earth metal ions, there are some cases where doping with the two-dimensional carbon is performed automatically, whereby the conductivity is improved.
  • the conductivity of two-dimensional carbon is improved by stacking more graphenes.
  • a stack of 101 or more graphenes is not preferable because it has too strong graphitic characteristics.
  • its typical length may be greater than or equal to 100 nm and less than or equal to 100 ⁇ m, preferably greater than or equal to 1 ⁇ m and less than or equal to 20 ⁇ m.
  • two-dimensional carbon with a typical length of less than or equal to 100 nm has semiconductor characteristics and thus has low conductivity.
  • two-dimensional carbon with a typical length of greater than or equal to 100 nm has electric characteristics equivalent to those of a good conductor.
  • the typical length is preferably greater than or equal to 1 ⁇ m.
  • a typical length is defined as the square root of the area of two-dimensional carbon. Although two-dimensional carbon may actually have various shapes, here, the length is defined assuming that all two-dimensional carbon has rectangular shapes. Accordingly, a typical length of rectangular two-dimensional carbon with a long side of 2 min and a short side of 50 nm (these values are not within the above preferable range) is 10 ⁇ m (this value is within the above preferable range), for example.
  • a conduction auxiliary agent may include, in addition to two-dimensional carbon, acetylene black particles or carbon particles (such as carbon nanofibers) extending one-dimensionally, at a volume greater than or equal to 0.1 times and less than or equal to 10 times that of two-dimensional carbon.
  • the resistance of the electrical appliance can be reduced.
  • a conduction auxiliary agent according to the present invention when used for a primary battery or a secondary battery, it is more preferable that the resistance (internal resistance) of an electrode be lower, which is suitable for applications where a large amount of power is required instantaneously.
  • a power source of an electric vehicle consumes a relatively small amount of power when the electric vehicle is driven on flat ground.
  • a large amount of power is consumed under hard acceleration or in ascending a slope.
  • the power source needs to feed a large amount of current; however, when internal resistance is high, a significant voltage drop and also a loss due to internal resistance are caused.
  • part of the power which is expected to be available is lost.
  • stored power can be almost fully used if the vehicle is driven on flat ground, part of the power is lost in ascending a slope or under acceleration. Reduction in internal resistance can suppress such loss.
  • FIGS. 3A to 3D are views for describing the reason why the conductivity is not sufficiently improved by using a material extending one-dimensionally, for example, carbon fibers.
  • FIG. 3A illustrates carbon fibers 101 arranged in a certain ideal state. In other words, the plurality of carbon fibers 101 are arranged orderly in a square grid pattern. The length directions of the carbon fibers 101 are perpendicular to the paper.
  • a distance between a surface of one carbon fiber and a surface of another carbon fiber is x. That is, a diameter of a carbon fiber is obtained by subtraction of x from a grid interval. There is an optimal value for the x depending on a particle size of an active material or the like.
  • FIG. 3B illustrates the carbon fibers observed in a direction indicated by an arrow “a” in FIG. 3A .
  • an arrow “b” indicates a direction in which the carbon fibers are observed in FIG. 3A .
  • the case is considered where the carbon fibers 101 are in contact with upper carbon fibers 102 .
  • FIG. 3C it seems that the carbon fibers 101 are in close contact with the upper carbon fibers 102 , so that the resistance therebetween can be minimum.
  • the diameters of the carbon fibers 101 and 102 are set to one-tenth of the grid intervals. In that case, the probability of the carbon fibers 101 at least partly overlapping (being in contact) with the upper carbon fibers 102 is about 12.6%.
  • the probability is greatly increased when a material extending two-dimensionally is used.
  • a structure illustrated in FIG. 3E two-dimensional carbon 103
  • the bending margin is set to x. This is to obtain an effect equivalent to that in FIG. 3A .
  • FIGS. 3C and 3D show an example of a case where carbon fibers seem to be in contact with each other when seen from a certain angle but are not in contact with each other when seen from another angle. Meanwhile, a material extending two-dimensionally as in FIG. 3E seems to be in contact with an upper material seen from any angle if they seem to be in contact with each other when seen from a certain angle, and they are actually in contact with each other.
  • the volume of a material extending two-dimensionally is to be focused on here.
  • the area of the two-dimensional carbon 103 in FIG. 3E is 2.2 times as large as a surface area of the carbon fibers 101 in the corresponding region in FIG. 3A ; however, if the thickness is sufficiently small, the volume of the two-dimensional carbon 103 is smaller than that of all the carbon fibers 101 in FIG. 3A .
  • the two-dimensional carbon 103 is formed of 10 graphenes
  • its thickness is 3.4 nm
  • the two-dimensional carbon 103 is formed of a smaller number of graphenes
  • its thickness is less than 3.4 nm.
  • the radiuses of the carbon fibers 101 are greater than or equal to 3.86 nm
  • the volume is larger when the carbon fibers are used.
  • the radius of a carbon fiber or any other material extending one-dimensionally is actually greater than 5 nm; thus, even larger volume is required.
  • FIG. 3E illustrates the case where the material extending two-dimensionally has a structure bent in a special shape
  • the material extends two-dimensionally within a considerable range.
  • FIG. 3F there is a case as illustrated in FIG. 3F , where two-dimensional carbon 104 arranged at regular intervals in the direction “a” extends infinitely.
  • a contact state therebetween is examined.
  • the upper two-dimensional carbon is arranged in the same direction as the two-dimensional carbon 104 , it is difficult for the upper two-dimensional carbon to be in contact with the two-dimensional carbon 104 except in the case of overlapping with the two-dimensional carbon 104 .
  • the case where the upper two-dimensional carbon is arranged in the same direction as the two-dimensional carbon 104 hardly occurs, and usually there is a certain angle therebetween. Accordingly, contact between the upper two-dimensional carbon and the two-dimensional carbon 104 can be expected in most cases if the length of two-dimensional carbon in the direction “a” is infinite.
  • the probability of the upper two-dimensional carbon being in contact with the two-dimensional carbon 104 is sufficiently high.
  • the two-dimensional carbon 104 does not overlap with the upper two-dimensional carbon if an angle formed therebetween is greater than or equal to 0° and less than 45°, but overlaps therewith if the angle is greater than or equal to 45° and less than or equal to 90°.
  • the probability of overlapping is 50% even in such a case. This value is significantly high as compared with 12.6% in the case of carbon fibers.
  • the probability of overlapping is nearly 90% if the length of the two-dimensional carbon in the direction “a” is greater than or equal to 5 times as large as the length x. It is preferable that x be greater than or equal to 1 time and less than or equal to 5 times as large as the size of an active material particle, and the length of two-dimensional carbon can be accordingly determined.
  • a typical length of two-dimensional carbon is preferably greater than or equal to 1 time, further preferably greater than or equal to 5 times as large as an average value of the sizes of the active material particles.
  • FIG. 1 is a schematic view of two-dimensional carbon and active material particles.
  • FIG. 2 is a schematic view of acetylene black particles and active material particles.
  • FIGS. 3A to 3F are views for describing the difference between the conductivity of carbon fibers and that of two-dimensional carbon.
  • FIG. 4 illustrates an example of a secondary battery.
  • a method for manufacturing a lithium ion secondary battery which is one embodiment of the present invention will be described.
  • two-dimensional carbon which is to be used as a conduction auxiliary agent is manufactured.
  • a CVD method Patent Document 2
  • a coating method Patent Document 3
  • a method in which two-dimensional carbon is chemically separated from graphite Non-Patent Document 1
  • a metal film of nickel, iron, or the like serving as a catalyst is formed over a substrate, the substrate is placed in a chamber and heated at a temperature of 600° C. to 1100° C., and a gas containing hydrocarbon, such as methane or ethane, is introduced into the chamber, so that a two-dimensional carbon film including 1 to 10 graphene sheets is provided over the substrate.
  • a gas containing hydrocarbon such as methane or ethane
  • the metal film is etched with acid or the like, whereby a self-supported two-dimensional carbon film is obtained.
  • the obtained film is cut and processed into rectangles in which the length of one side is 1 ⁇ m to 100 ⁇ m.
  • a sulfuric acid solution of potassium permanganate, hydrogen peroxide water, or the like is mixed into single crystal graphite powder to cause oxidation reaction; thus, a graphene oxide aqueous solution is obtained.
  • the obtained graphene oxide aqueous solution is applied onto an appropriate substrate provided with a separation layer and dried.
  • a separation layer a film of a metal which is soluble in acid, with a thickness of 1 nm to 100 nm, may be used.
  • graphene oxide is reduced by high-temperature heating in vacuum, addition of a reducing agent such as hydrazine, or the like, so that a two-dimensional carbon film including 1 to 10 graphene sheets is obtained.
  • a reducing agent such as hydrazine, or the like
  • the separation layer is etched with acid or the like, whereby a self-supported two-dimensional carbon film is obtained.
  • the obtained film is cut and processed into rectangles in which the length of one side is 1 ⁇ m to 100 ⁇ m. Note that the processing into rectangles may be performed at the stage where the graphene oxide aqueous solution is applied onto the substrate and dried.
  • reduction reaction proceeds from a surface; therefore, the reduction reaction can be terminated at an appropriate depth by controlling reaction time.
  • reduced two-dimensional carbon is obtained at the surface, while graphene oxide remains in a deeper portion. Since graphene oxide is suspended in water, a self-supported film of two-dimensional carbon (insoluble in water) can be obtained by soaking the substrate in water. The graphene oxide dissolved in water can be collected and applied onto a substrate again.
  • graphite is placed in a polar solvent such as chloroform, N,N-dimethylformamide (DMF), or N-methylpyrrolidone (NMP) and bonding between graphite layers is broken by ultrasonic vibration, so that two-dimensional carbon can be obtained.
  • a polar solvent such as chloroform, N,N-dimethylformamide (DMF), or N-methylpyrrolidone (NMP)
  • planarity is not required in the case of using two-dimensional carbon as a conduction auxiliary agent, poor planarity is not a problem. On the contrary, this method is more efficient than other methods in terms of productivity.
  • a layer of a material which is to be mixed with the two-dimensional carbon later, such as active material particles, is preferably applied onto one surface of the self-supported two-dimensional carbon film with a thickness of 10 nm to 100 nm.
  • the two-dimensional carbon is likely to aggregate after being cut, aggregation can be prevented by providing a layer of another material on one surface thereof.
  • the two-dimensional carbon having an appropriate area manufactured in the above manner is mixed with a positive electrode active material and a binder, whereby a slurry is obtained.
  • Other conduction auxiliary agents such as acetylene black may be additionally mixed as appropriate.
  • the positive electrode active material lithium iron phosphate, lithium manganese phosphate, lithium manganese silicate, lithium iron silicate, or the like can be used; however, one embodiment of the present invention is not limited thereto.
  • Positive electrode active material particles preferably have sizes within the range of 20 nm to 100 nm.
  • a carbohydrate such as glucose may be mixed at the time of baking of the positive electrode active material particles, so that the positive electrode active material particles are coated with carbon. This treatment can improve the conductivity.
  • FIG. 4 shows the structure of a coin-type secondary battery.
  • the above slurry is applied onto a positive electrode current collector 228 , molded, and then dried, whereby a positive electrode active material layer 230 is formed.
  • a material of the positive electrode current collector 228 aluminum is preferably used.
  • the coin-type secondary battery includes a negative electrode 204 , a positive electrode 232 , a separator 210 , an electrolyte (not illustrated), a housing 206 , and a housing 244 .
  • the coin-type secondary battery includes a ring-shaped insulator 220 , a spacer 240 , and a washer 242 .
  • the positive electrode 232 the electrode that is obtained in the above step by forming the positive electrode active material layer 230 over the positive electrode current collector 228 is used.
  • the electrolyte in which LiPF 6 is dissolved in a mixed solvent of ethylene carbonate (EC) and diethyl carbonate (DEC) is preferably used; however one embodiment of the present invention is not limited hereto.
  • the negative electrode 204 includes a negative electrode active material layer 202 over a negative electrode current collector 200 .
  • a negative electrode current collector 200 copper is used, for example.
  • a negative electrode active material graphite, polyacene, or the like is used.
  • the negative electrode active material layer 202 is preferably formed using such a material alone or a mixture of the material and a binder. Alternatively, two-dimensional carbon obtained by any of the above methods may be used as the negative electrode active material.
  • An insulator with pores e.g., polypropylene
  • a solid electrolyte which can transmit lithium ions may be used.
  • the housing 206 , the housing 244 , the spacer 240 , and the washer 242 each of which is made of metal (e.g., stainless steel) are preferably used.
  • the housing 206 and the housing 244 have a function of electrically connecting the negative electrode 204 and the positive electrode 232 to the outside.
  • the negative electrode 204 , the positive electrode 232 , and the separator 210 are soaked in the electrolyte. Then, as illustrated in FIG. 4 , the negative electrode 204 , the separator 210 , the ring-shaped insulator 220 , the positive electrode 232 , the spacer 240 , the washer 242 , and the housing 244 are stacked in this order inside the housing 206 . The housing 206 and the housing 244 are subjected to pressure bonding. In such a manner, the coin-type secondary battery is manufactured.
  • an electrical appliance As examples of an electrical appliance according to the present invention, a variety of dry batteries, storage batteries, and the like are given.
  • a conduction auxiliary agent for a positive electrode or a negative electrode of any of these batteries the conduction auxiliary agent including two-dimensional carbon described in Embodiment 1 may be used for example.
  • an electrical appliance As examples of an electrical appliance according to the present invention, electric vehicles, electric power tools, personal computers, mobile phones, and the like can be given. Such an electrical appliance is not always supplied with power by a wire and therefore includes a storage battery inside.
  • a conduction auxiliary agent for a positive electrode or a negative electrode of the storage battery the conduction auxiliary agent including two-dimensional carbon described in Embodiment 1 may be used for example.
  • a storage battery with low internal resistance is required for applications where a large amount of current needs to be fed instantaneously or where a required current value varies greatly. Therefore, a sufficient effect can be obtained by using the present invention.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Composite Materials (AREA)
  • Materials Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Mechanical Engineering (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)
US13/211,577 2010-08-19 2011-08-17 Electrical Appliance Abandoned US20120045692A1 (en)

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JP (3) JP2012064571A (enExample)
KR (1) KR101892984B1 (enExample)
CN (2) CN106207082A (enExample)
DE (1) DE112011102750T5 (enExample)
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US9218916B2 (en) 2011-06-24 2015-12-22 Semiconductor Energy Laboratory Co., Ltd. Graphene, power storage device, and electric device
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US9252419B2 (en) 2011-09-09 2016-02-02 Semiconductor Energy Laboratory Co., Ltd. Positive electrode for lithium secondary battery, manufacturing method thereof, and lithium secondary battery
US9293770B2 (en) 2012-04-10 2016-03-22 Semiconductor Energy Laboratory Co., Ltd. Graphene oxide, positive electrode for nonaqueous secondary battery using graphene oxide, method of manufacturing positive electrode for nonaqueous secondary battery, nonaqueous secondary battery, and electronic device
US9337475B2 (en) 2011-08-30 2016-05-10 Semiconductor Energy Laboratory Co., Ltd. Power storage device
US9373834B2 (en) 2011-12-16 2016-06-21 Semiconductor Energy Laboratory Co., Ltd. Method for forming positive electrode for lithium-ion secondary battery
US9384904B2 (en) 2012-04-06 2016-07-05 Semiconductor Energy Laboratory Co., Ltd. Negative electrode for power storage device, method for forming the same, and power storage device
US9385366B2 (en) 2012-08-27 2016-07-05 Semiconductor Energy Laboratory Co., Ltd. Positive electrode for secondary battery, secondary battery, and method for fabricating positive electrode for secondary battery
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US20140370184A1 (en) 2014-12-18
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JP2012064571A (ja) 2012-03-29
JP6113309B2 (ja) 2017-04-12
TWI597888B (zh) 2017-09-01
JP2016105409A (ja) 2016-06-09
JP2017103257A (ja) 2017-06-08
CN103053055B (zh) 2016-10-12
WO2012023464A1 (en) 2012-02-23
KR101892984B1 (ko) 2018-08-30
US10044027B2 (en) 2018-08-07
CN106207082A (zh) 2016-12-07
CN103053055A (zh) 2013-04-17
KR20120018075A (ko) 2012-02-29

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