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WO2008015779A1 - Materiau électroconducteur carboné destiné à une batterie et batterie - Google Patents

Materiau électroconducteur carboné destiné à une batterie et batterie Download PDF

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Publication number
WO2008015779A1
WO2008015779A1 PCT/JP2007/000806 JP2007000806W WO2008015779A1 WO 2008015779 A1 WO2008015779 A1 WO 2008015779A1 JP 2007000806 W JP2007000806 W JP 2007000806W WO 2008015779 A1 WO2008015779 A1 WO 2008015779A1
Authority
WO
WIPO (PCT)
Prior art keywords
battery
boron
conductive material
carbonaceous conductive
carbonaceous
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/JP2007/000806
Other languages
English (en)
Japanese (ja)
Inventor
Tsunemi Ochiai
Takayuki Kawarada
Masaharu Takehara
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.)
Nippon Steel Chemical and Materials Co Ltd
Original Assignee
Nippon Steel Chemical Co Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Nippon Steel Chemical Co Ltd filed Critical Nippon Steel Chemical Co Ltd
Priority to JP2008527650A priority Critical patent/JPWO2008015779A1/ja
Publication of WO2008015779A1 publication Critical patent/WO2008015779A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • 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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B21/00—Nitrogen; Compounds thereof
    • C01B21/06—Binary compounds of nitrogen with metals, with silicon, or with boron, or with carbon, i.e. nitrides; Compounds of nitrogen with more than one metal, silicon or boron
    • C01B21/064—Binary compounds of nitrogen with metals, with silicon, or with boron, or with carbon, i.e. nitrides; Compounds of nitrogen with more than one metal, silicon or boron with boron
    • C01B21/0641—Preparation by direct nitridation of elemental boron
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C1/00—Treatment of specific inorganic materials other than fibrous fillers; Preparation of carbon black
    • C09C1/44—Carbon
    • C09C1/48—Carbon black
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2002/00—Crystal-structural characteristics
    • C01P2002/50—Solid solutions
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/80—Particles consisting of a mixture of two or more inorganic phases
    • C01P2004/82—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases
    • C01P2004/84—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases one phase coated with the other
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/19—Oil-absorption capacity, e.g. DBP values
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/40—Electric properties
    • 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
    • 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 carbonaceous conductive material for a battery and a battery used by blending with a positive electrode or a negative electrode of the battery.
  • a battery is required to have high conductivity in an electrode, and a carbonaceous conductive material (hereinafter sometimes referred to as a conductive aid) in order to improve the conductivity of the active material of the electrode. Is used.
  • high-structure one-by-one pump racks such as acetylene black and ketjen black are widely used.
  • acetylene black As a general conductive aid, high-structure one-by-one pump racks such as acetylene black and ketjen black are widely used.
  • acetylene black As a general conductive aid, high-structure one-by-one pump racks such as acetylene black and ketjen black are widely used.
  • acetylene black as a conductive assistant for the positive electrode active material.
  • boron is contained in the carbon material or conductive material used for the positive electrode or the negative electrode.
  • a lithium secondary battery has been proposed (see Patent Document 2).
  • a force pump rack is used as a carbon material or a conductive material, specifically, for example, acetylene brick and trimethyl borate are mixed in advance in a predetermined amount and sprayed on a reaction layer at about 200 ° C.
  • One pump rack is supposed to be obtained.
  • the force pump rack in this case also seems to be in a form in which boron is dissolved in the same manner as in Patent Document 1 above.
  • Patent Document 1 Japanese Patent Laid-Open No. 2 0 00 _ 2 8 1 9 3 3
  • Patent Document 2 JP 2 0 0 3 _ 0 4 5 4 3 4
  • the present invention has been made in view of the above problems, and an object of the present invention is to provide a carbonaceous conductive material for a battery and a battery that can suppress a reaction between an electrode and an electrolytic solution.
  • Another object of the present invention is to provide a carbonaceous conductive material for a battery and a battery that can increase the voltage at which the battery can be used to increase the energy density and can improve safety.
  • the carbonaceous conductive material for a battery according to the present invention is a carbon base material whose surface is coated with a metal compound or a boron compound in a carbonaceous conductive material for a battery that is used in a positive electrode or a negative electrode of a battery. It is characterized by being.
  • the carbonaceous conductive material for a battery according to the present invention is characterized in that the carbon base material is carbon black.
  • the carbonaceous conductive material for a battery according to the present invention contains a nitrogen element together with boron.
  • the atomic ratio of boron element to nitrogen element is 1 ⁇ 10.
  • the carbonaceous conductive material for a battery according to the present invention is characterized by being fired at 15500 to 200 ° C.
  • the carbonaceous conductive material for a battery according to the present invention is such that the battery is a lithium ion secondary battery, the carbon black whose surface is coated with boron or a boron compound is blended in a positive electrode, It is characterized by a voltage exceeding 4.2 V.
  • a battery according to the present invention is characterized by using the above-described carbonaceous conductive material for a battery.
  • the carbonaceous conductive material for a battery according to the present invention is a carbon substrate whose surface is coated with a metal compound or a boron compound, and the battery according to the present invention includes the carbonaceous conductive material for a battery described above. Therefore, the reaction between the electrode and the electrolytic solution can be suppressed. In addition, this makes it possible to increase the usable voltage of the battery to increase the energy density, and to improve the safety.
  • FIG. 1 is a diagram showing CV curves measured using CV evaluation cells adjusted in Example 1, Example 6, and Comparative Example 1.
  • FIG. 2 is a diagram showing CV curves measured using the CV evaluation cell adjusted in Example 8 and Comparative Example 4.
  • the carbonaceous conductive material for a battery according to the present embodiment is a carbonaceous conductive material for a battery that is used by being blended with a positive electrode or a negative electrode of a battery, and a carbon substrate whose surface is coated with a metal compound or a boron compound. It is.
  • the carbonaceous conductive material for a battery is a positive electrode or a negative electrode mixed with an active material. It is used to increase the electrode conductivity.
  • the material for coating the surface of the carbon base material is more preferably a boron compound, and the carbon base material is preferably a force pump rack.
  • a part of the boron element may penetrate into the surface layer of the bonbon black.
  • the following is an example of a force pump rack coated with a boron compound.
  • the aggregator which is evaluated by the DBP oil absorption amount of the force pump rack having the aggregate structure (structure 1), contributes to the battery reaction described above.
  • the effect of the boron compound being uniformly coated on the surface of carbon black having an appropriate specific surface area due to the presence of the aggregate structure is also considered.
  • the reactivity with the electrolyte can be suppressed while moderately increasing or decreasing the conductivity as the conductive material.
  • an appropriate carbon base material and surface coating material can be used.
  • the boron compound is, for example, boron nitride, boron carbide or the like, and the boron compound contains 0.1 to 10 parts by mass with respect to 100 parts by mass of carbon black on the basis of boron. Further, it is more preferable to contain 0.5 to 5 parts by mass. Content of boron compound is 0.1 based on boron If the amount is less than the amount, the surface of the carbon black cannot be sufficiently covered, and a preferable function is not manifested.If the amount exceeds 10 parts by mass, the carbon black containing boron or a fluorine compound is baked. In either case, the DBP oil absorption is reduced, so neither is preferred.
  • the type of carbon black is not particularly limited, and is appropriately selected from furnace black, channel black, acetylene black, thermal black, lamp black, ketjen black, and the like. be able to.
  • the carbonaceous conductive material for a battery according to the present embodiment is blended with a positive electrode of a lithium ion secondary battery and the withstand voltage exceeds 4.2 V, lithium ion with high energy density is used. It is suitable as a secondary battery.
  • the withstand voltage is the maximum voltage that can be used as a battery.
  • the battery according to the present embodiment is obtained by blending the carbonaceous conductive material for a battery according to the present embodiment with a positive electrode or a negative electrode of the battery.
  • the effect of the carbonaceous conductive material for a battery is obtained. It can be suitably obtained.
  • a method for producing a carbonaceous conductive material for a battery is as follows. Carbon black is mixed with an appropriate boron source such as boron, boron oxide or boron carbide, preferably by induction heating.
  • an appropriate boron source such as boron, boron oxide or boron carbide, preferably by induction heating.
  • Baking is performed at 5 0 to 2 0 0 0 ° C.
  • the carbonaceous conductive material for a battery having the above characteristics is more suitable for the effect of the carbonaceous conductive material for a battery according to the above-described embodiment. Can get to.
  • the frequency of the current applied in the induction heating is not particularly limited, and an alternating current having a wide frequency range from a so-called low frequency to a high frequency can be used. In particular, it is more preferable to apply a current having a frequency of 1 0000 Hz or less. Heating is preferably performed within 10 minutes from the start of power application, more preferably within 8 minutes, under such conditions that the temperature of the pump rack rises to over 1850 ° C. Since the induction heating method allows self-combustion synthesis using reaction heat, the reaction proceeds more effectively in a short time.
  • the atmosphere during induction heating is not limited. Although the reaction in the atmosphere (air) is preferable because of its low cost, when controlling the activity of the carbon black surface, a suitable amount of argon or nitrogen is allowed to flow into the reaction system to produce (boron of carbonaceous conductive material for batteries). : B) / (Nitrogen: N) It is effective to adjust the ratio.
  • Nitrogen analysis is performed with the following analytical method and measuring instrument.
  • the analysis of metals and boron is performed with the following analysis method and measuring instrument.
  • ICP-OES Inductively coupled plasma optical emission spectrometry
  • a conductive auxiliary agent and polyvinylidene fluoride (PVD F) as a binder were blended in a ratio of 4/1 to obtain a mixture for an evaluation electrode.
  • PVD F polyvinylidene fluoride
  • NMP N-methylpyrrolidone
  • a sheet electrode was obtained by pressing. The obtained sheet electrode was shaped to a size that fits the coin cell and used as an evaluation electrode.
  • Metal lithium was used for the counter electrode, and a polypropylene porous film was used for the separator. These were also sized to fit the coin cell, similar to the evaluation electrode.
  • a non-aqueous electrolyte (1 M_L i P F6 (EC: DMC) in which 1 mol / liter of lithium hexafluorophosphate was dissolved in a 1: 1 mixed organic solvent of ethylene force monoponate and dimethyl carbonate as an electrolyte. )
  • coin cell CR20 32
  • the CV evaluation cell is scanned at an oxidation / reduction potential in the range of 3 V to 5 V at a scanning speed of 5 mV / min and the current value is measured.
  • a mixture of 99% by weight of a force pump rack and 1% by weight of boron powder has a thickness of 5mm and a diameter of 100mm in a cylindrical force with an outer diameter of 1 20mm, an inner diameter of 100mm, and a height of 80mm. It was filled with a Pon disc so that it covers the top and bottom of the luppo, and this ruppo was placed in a medium frequency induction furnace, and 2150 Hz, 40 kW of power was applied for 5 minutes. At this time, atmosphere control was not performed, but it was performed in the air.
  • Table 1 shows the physical properties of the obtained conductive additive (carbon conductive material for batteries), and Fig. 1 shows the CV measurement results. The same applies to the other examples below.
  • Conductive aid was carried out in the same way as in Example 1 except that a mixture of 99.5% by mass of Niteron # 3350, manufactured by Nippon Kaigaibon Co., Ltd., and 0.5% by mass of boron powder was used as the starting material. Got.
  • Conductive aid was obtained in the same manner as in Example 1 except that a mixture of 97% by mass of Nitteron Power Ichibon Co., Ltd. “Niteron # 3350” and 3% by mass of boron powder was used as a starting material. .
  • Example 2 Use “HTC # 20” manufactured by Nippon Kayaku Co., Ltd. as a starting material.
  • a conductive additive was obtained in the same manner as in Example 1 except that a mixture of 99% by mass of carbon black and 1% by mass of boron powder was used.
  • Example 2 Implemented in the same manner as in Example 1 except that “Niteron # 4 10” manufactured by Shin-Nikka Kaichibon Co., Ltd. was used as a starting material, and a mixture of 99% by mass of the carbon black and 1% by mass of boron powder was used. As a result, a conductive assistant was obtained.
  • Nitteron # 3350 manufactured by Shin-Nichi Kaichi Bonn Co., Ltd. using a mixture of 99% by mass of the carbon black and 1% by mass of boron powder, and passing through a magnetic tube with an inner diameter of 5mm. was conducted in the same manner as in Example 1 except that it was allowed to flow into the crucible at 100 cc / min to obtain a conductive additive.
  • Example 2 Using Niteron # 3350 manufactured by Nippon Kayaku Co., Ltd. as a starting material, a mixture of 99% by mass of the carbon black and 1% by mass of boron powder was used, and nitrogen was passed through a magnetic tube with an inner diameter of 5 mm. Was conducted in the same manner as in Example 1 except that it was allowed to flow into the crucible at 1 OO cc / min to obtain a conductive additive.
  • Conductive auxiliary agent was carried out in the same manner as in Example 1 except that powdery acetylene black (AB) was used as a starting material and a mixture of 97% by mass of the acetylene black and 3% by mass of boron oxide powder was used.
  • Table 1 shows the physical properties of the conductive aid obtained, and Figure 2 shows the CV measurement results.
  • Table 2 shows the physical properties of “Niteron # 3350” untreated product (carbon black base material not containing boron powder) used in Examples 1 to 3, 6 and 7 as a conductive additive.
  • Figure 1 shows. The same applies to the following other comparative examples.
  • a conductive additive was obtained in the same manner as in Example 1 except that a mixture of 90% by mass of the carbon black and 10% by mass of boron powder was used.
  • the evaluation cell using the conductive additive of Examples 1 to 8 has a 0 oxidation potential rise by CV measurement compared to the evaluation cell using the conductive additive shown in Comparative Examples 1 to 3.
  • the powder resistance value tends to be lower than that of the untreated product (carbon black base material not containing boron), and the DBP absorption amount greatly changes compared to the untreated product. You can see that they are not.
  • Comparative Example 4 is acetylene black, which is generally used as a conductive additive for batteries, but the rise in oxidation potential by CV measurement is 4.2 V. It can be seen that it is the same as the force one pump rack group (Comparative Examples 1 to 3) manufactured by Co., Ltd. On the other hand, in Example 8, in which boron powder was mixed with acetylene black and processed, as in the other examples, oxidation by CV measurement was performed. It can be seen that the rising voltage of the potential is increasing.
  • the conductive additive according to the present embodiment (the carbonaceous conductive material for a battery) has a high voltage while maintaining the conductivity and structure of the power pump rack as the carbon substrate. Since it is considered that it does not react with the electrolyte in the region, it is suitable as a conductive additive for high-voltage type batteries. In particular, it is suitable as a conductive additive for high voltage type lithium-ion secondary batteries.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

La présente invention concerne un matériau électroconducteur carboné pour une batterie, capable d'augmenter une tension utilisable pour augmenter la densité d'énergie, ainsi qu'une batterie. Le matériau électroconducteur carboné pour une batterie est, en cours d'utilisation, inclus dans une électrode positive ou négative d'une batterie et c'est un noir de carbone ayant une surface recouverte d'un composé de bore. De préférence, un élément d'azote, associé à un élément de bore, est contenu dans la surface du matériau électroconducteur carboné pour une batterie. Le rapport entre le nombre d'atomes de l'élément de bore et celui de l'élément d'azote est de 1 à 10. De plus et de préférence, le matériau électroconducteur carboné pour une batterie est utilisé pour une électrode positive dans une batterie ion-lithium rechargeable et possède une tension de maintien de plus de 4,2 V. Le matériau électroconducteur carboné pour une batterie est produit en incluant du bore dans du noir de carbone et par le déclenchement du mélange de 1500 à 2000 ºC.
PCT/JP2007/000806 2006-08-02 2007-07-30 Materiau électroconducteur carboné destiné à une batterie et batterie Ceased WO2008015779A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP2008527650A JPWO2008015779A1 (ja) 2006-08-02 2007-07-30 電池用炭素質導電材および電池

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2006210803 2006-08-02
JP2006-210803 2006-08-02

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WO2008015779A1 true WO2008015779A1 (fr) 2008-02-07

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2012221799A (ja) * 2011-04-11 2012-11-12 Kaneka Corp 非水電解質二次電池
JP2017091657A (ja) * 2015-11-04 2017-05-25 トヨタ自動車株式会社 非水電解液二次電池および非水電解液二次電池の製造方法

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH1121116A (ja) * 1997-06-30 1999-01-26 Nippon Steel Corp 窒化ホウ素で被覆された炭素質粉末および炭素質繊維
WO2001006583A1 (fr) * 1999-07-21 2001-01-25 Mitsubishi Materials Corporation Poudre de carbone dont les caracteristiques electriques sont renforcees et mode d'utilisation
JP2002203551A (ja) * 2000-12-28 2002-07-19 Gs-Melcotec Co Ltd 非水電解質電池
JP2003308844A (ja) * 2002-04-18 2003-10-31 Hitachi Maxell Ltd 非水二次電池とその正極

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH1121116A (ja) * 1997-06-30 1999-01-26 Nippon Steel Corp 窒化ホウ素で被覆された炭素質粉末および炭素質繊維
WO2001006583A1 (fr) * 1999-07-21 2001-01-25 Mitsubishi Materials Corporation Poudre de carbone dont les caracteristiques electriques sont renforcees et mode d'utilisation
JP2002203551A (ja) * 2000-12-28 2002-07-19 Gs-Melcotec Co Ltd 非水電解質電池
JP2003308844A (ja) * 2002-04-18 2003-10-31 Hitachi Maxell Ltd 非水二次電池とその正極

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2012221799A (ja) * 2011-04-11 2012-11-12 Kaneka Corp 非水電解質二次電池
JP2017091657A (ja) * 2015-11-04 2017-05-25 トヨタ自動車株式会社 非水電解液二次電池および非水電解液二次電池の製造方法

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