WO2012086507A1 - Batterie secondaire à électrolyte non aqueux - Google Patents

Batterie secondaire à électrolyte non aqueux Download PDF

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Publication number
WO2012086507A1
WO2012086507A1 PCT/JP2011/079016 JP2011079016W WO2012086507A1 WO 2012086507 A1 WO2012086507 A1 WO 2012086507A1 JP 2011079016 W JP2011079016 W JP 2011079016W WO 2012086507 A1 WO2012086507 A1 WO 2012086507A1
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WO
WIPO (PCT)
Prior art keywords
secondary battery
negative electrode
positive electrode
electrolyte secondary
aqueous electrolyte
Prior art date
Application number
PCT/JP2011/079016
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English (en)
Japanese (ja)
Inventor
真治 山本
Original Assignee
株式会社 村田製作所
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Publication date
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Priority to JP2012549757A priority Critical patent/JPWO2012086507A1/ja
Publication of WO2012086507A1 publication Critical patent/WO2012086507A1/fr

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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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
    • 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
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • 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
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
    • 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 generally to a non-aqueous electrolyte secondary battery, and more particularly to a non-aqueous electrolyte secondary battery with improved life characteristics.
  • a nonaqueous electrolyte secondary battery generally, a nonaqueous electrolyte solution in which a lithium salt such as lithium hexafluorophosphate is dissolved as an electrolyte in a nonaqueous solvent such as ethylene carbonate or dimethyl carbonate.
  • a lithium transition metal composite oxide as a positive electrode active material, and a carbon material as a negative electrode active material.
  • the non-aqueous electrolyte contains various additives in order to improve battery characteristics.
  • a non-aqueous electrolyte in order to suppress or prevent swelling deformation of a battery in a high temperature environment, includes an electrolyte salt, boron, phosphorus, A non-aqueous electrolyte secondary battery containing an oxalato complex salt having any one selected from the group consisting of aluminum, gallium, arsenic, and antimony as a central ion or central atom and a sulfone derivative is described. Yes.
  • an object of the present invention is to provide a non-aqueous electrolyte secondary battery capable of improving life characteristics.
  • a non-aqueous electrolyte secondary battery includes a positive electrode including a positive electrode active material, a negative electrode including a negative electrode active material, and a non-aqueous electrolyte including a non-aqueous solvent.
  • the positive electrode active material includes a lithium-containing phosphate compound having an olivine structure.
  • At least one oxalato complex salt whose central ion or central atom is any one selected from the group consisting of boron, phosphorus, aluminum, gallium, arsenic, and antimony with respect to 100 parts by mass of the nonaqueous electrolytic solution. Is added in an amount of 0.5 parts by mass or more and 2.0 parts by mass or less.
  • the negative electrode active material contains graphite and soft carbon.
  • the oxalato complex salt is preferably difluorobis (oxalato) lithium phosphate.
  • the oxalato complex salt contains difluorobis (oxalato) lithium phosphate and bis (oxalato) lithium borate.
  • the positive electrode active material contains a lithium-containing phosphate compound having an olivine structure, so that the operating potential of the positive electrode is lowered. Therefore, the oxalato complex salt added to the non-aqueous electrolyte Can be largely suppressed from being oxidatively decomposed on the surface of the positive electrode. For this reason, the oxalato complex salt added to the non-aqueous electrolyte is selectively reduced and decomposed on the surface of the negative electrode. As a result, a specific amount of the oxalato complex salt is selectively reduced and decomposed on the surface of the negative electrode, and an appropriate amount of film is formed on the surface of the negative electrode. As a result, an increase in the direct current resistance (hereinafter referred to as DCR) of the battery during high temperature storage can be suppressed, and the life characteristics can be improved.
  • DCR direct current resistance
  • FIG. 1 schematically shows a configuration of a battery element housed in an outer packaging material of the non-aqueous electrolyte secondary battery shown in FIG. 1, and shows an enlarged cross section viewed from a direction along line II-II in FIG. It is a fragmentary sectional view.
  • 1 schematically shows a configuration of a battery element accommodated in an outer packaging material of the non-aqueous electrolyte secondary battery shown in FIG. 1, and shows an enlarged cross-sectional view taken along a line III-III in FIG. It is a fragmentary sectional view.
  • a non-aqueous electrolyte secondary battery comprising a positive electrode including a positive electrode active material, a negative electrode including a negative electrode active material, and a non-aqueous electrolyte including a non-aqueous solvent has the following characteristics: It was found that the life characteristics can be improved. The present invention has been made based on such knowledge of the present inventor.
  • the positive electrode active material contains a lithium-containing phosphate compound having an olivine structure, and boron, phosphorus, aluminum, gallium, arsenic, And at least 1 sort (s) of oxalate complex salt which makes any one sort chosen from the group which consists of antimony a central ion or a central atom is added 0.5 mass part or more and 2.0 mass parts or less.
  • the positive electrode active material contains a lithium-containing phosphate compound having an olivine structure, for example, lithium iron phosphate
  • the operating potential of the positive electrode is lowered.
  • the oxalato complex salt added to the electrolytic solution can be largely suppressed from being oxidatively decomposed on the surface of the positive electrode. For this reason, the oxalato complex salt added to the non-aqueous electrolyte is selectively reduced and decomposed on the surface of the negative electrode.
  • lithium difluorobis (oxalato) phosphate lithium bis (oxalato) borate, lithium tris (oxalato) phosphate, lithium difluorobis (oxalato) borate, and the like can be used.
  • by using a mixture of lithium difluorobis (oxalato) phosphate and lithium bis (oxalato) borate it is possible to further suppress an increase in DCR during high-temperature storage.
  • the lithium-containing phosphate compound having an olivine structure contained in the positive electrode active material is preferably lithium iron phosphate represented by LiFePO 4 . If it has an olivine type structure, in the lithium iron phosphate represented by LiFePO 4 , a part of Fe is replaced with Al, Ti, V, Cr, Mn, Co, Ni, Zr, Nb, etc. Also good. A part of P may be replaced with B, Si, or the like.
  • the negative electrode may include a carbon material such as acetylene black that acts as a conductive agent.
  • a carbon material such as acetylene black that acts as a conductive agent.
  • the binder for binding the negative electrode active material polyvinylidene fluoride, polyacrylonitrile or polyamideimide is used, or a mixture of a latex binder such as styrene butadiene rubber and a thickener such as carboxymethyl cellulose is used. .
  • the nonaqueous electrolytic solution is prepared by dissolving the supporting electrolyte in a nonaqueous solvent.
  • a solution obtained by dissolving LiPF 6 at a concentration of 1.0 mol / L in a non-aqueous solvent is used.
  • supporting electrolytes other than LiPF 6 include lithium salts such as LiBF 4 , LiAsF 6 , LiClO 4 , LiCF 3 SO 3 , LiN (SO 2 CF 3 ) 2 , LiC (SO 2 CF 3 ) 3 , LiAlCl 4 , and LiSiF 6. Can be mentioned.
  • LiPF 6 and LiBF 4 are particularly preferably used as the supporting electrolyte from the viewpoint of oxidation stability.
  • a supporting electrolyte is preferably used by being dissolved in a nonaqueous solvent at a concentration of 0.1 mol / L to 3.0 mol / L, and at a concentration of 0.5 mol / L to 2.0 mol / L. More preferably, it is used after being dissolved.
  • the non-aqueous solvent include cyclic carbonates such as ethylene carbonate (EC) and propylene carbonate (PC), dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), and diethyl carbonate (DEC), which are low viscosity solvents. And a lower chain carbonate of the above are used.
  • Example shown below is an example and this invention is not limited to the following Example.
  • the positive electrode, negative electrode and non-aqueous electrolyte prepared as follows, the addition amount of difluorobis (oxalato) lithium phosphate, lithium bis (oxalato) borate, or vinylene carbonate to the non-aqueous electrolyte By making it different, the non-aqueous electrolyte secondary battery of an Example and a comparative example was produced.
  • a lithium iron phosphate represented by the composition formula LiFePO 4 as a positive electrode active material, carbon powder as a conductive agent, and polyvinylidene fluoride as a binder were blended in a mass ratio of 84: 12: 4.
  • a positive electrode mixture slurry was prepared by kneading with N-methyl-2-pyrrolidone. This positive electrode mixture slurry was applied onto both surfaces of an aluminum foil as a positive electrode current collector, dried, and then rolled with a rolling roller to produce a positive electrode material.
  • the basis weight of the positive electrode mixture per unit area at this time was 4.8 mg / cm 2 , and the packing density was 1.85 g / cc.
  • the obtained positive electrode material was cut to produce a strip-shaped positive electrode member.
  • non-aqueous electrolyte a mixed solvent obtained by mixing ethylene carbonate, which is a cyclic carbonate, ethyl methyl carbonate, which is a chain carbonate, and dimethyl carbonate, which is a chain carbonate, in a volume ratio of 1: 1: 1, LiPF 6 was dissolved to a concentration of 1 mol / L to prepare a non-aqueous electrolyte.
  • a strip-shaped separator 13 made of a lithium ion-permeable polypropylene microporous membrane is interposed between the strip-shaped positive electrode member 11 and the negative electrode member 12 produced as described above.
  • 42 positive electrode members 11 and 43 negative electrode members 12 were alternately laminated to produce a battery element 10.
  • the battery element 10 was accommodated in an outer packaging material 20 made of a laminate film containing aluminum as an intermediate layer.
  • a positive electrode terminal 30 is attached to the exposed positive electrode current collector of the multiple positive electrode members 11 so as to extend from the inside of the outer packaging material 20 to the outside, and the negative electrode of the multiple negative electrode members 12 exposed as shown in FIG.
  • a negative electrode terminal 40 is attached to the current collector 41.
  • a partial surface of the positive electrode current collector was exposed by peeling off the positive electrode mixture layer located at one end of the strip-shaped positive electrode member 11.
  • An aluminum tab as the positive electrode terminal 30 was ultrasonically welded to a part of the surface of the exposed positive electrode current collector to produce a positive electrode.
  • a part of the surface of the negative electrode current collector 41 (FIG. 3) was exposed by peeling off the negative electrode mixture layer located at one end of the strip-shaped negative electrode member 12.
  • a copper tab as the negative electrode terminal 40 was ultrasonically welded to a part of the exposed negative electrode current collector 41 to produce a negative electrode.
  • the non-aqueous electrolyte secondary battery 100 of Comparative Example 1 was fabricated by sealing the opening of the outer packaging material 20. .
  • Example 1 The nonaqueous electrolyte secondary battery of Example 1 is the same as Comparative Example 1 except that 0.5 part by mass of lithium difluorobis (oxalato) phosphate is added to 100 parts by mass of the nonaqueous electrolyte. 100 was produced.
  • Example 3 The nonaqueous electrolyte secondary battery of Example 3 is the same as Comparative Example 1 except that 1.5 parts by mass of lithium difluorobis (oxalato) phosphate is added to 100 parts by mass of the nonaqueous electrolyte. 100 was produced.
  • Example 4 The nonaqueous electrolyte secondary battery of Example 4 is the same as Comparative Example 1 except that 2.0 parts by mass of lithium difluorobis (oxalato) phosphate is added to 100 parts by mass of the nonaqueous electrolyte. 100 was produced.
  • Example 5 Comparative Example 1 except that 0.5 parts by mass of lithium difluorobis (oxalato) phosphate and 0.5 parts by mass of lithium bis (oxalato) borate were added to 100 parts by mass of the non-aqueous electrolyte. Thus, a nonaqueous electrolyte secondary battery 100 of Example 5 was produced.
  • each battery was stored for 20 days in a thermostat set at a temperature of 45 ° C., the DCR before and after storage was measured, and the DCR increase rate before and after storage was calculated.
  • the DCR measurement method is as follows.
  • the voltage that changes when each battery charged at a temperature of 25 ° C. with a current value of 1 C until the SOC reaches 15% is further charged for 20 seconds and then the current value is increased by a certain amount.
  • Values were plotted against current values. The DCR was calculated by obtaining the slope of the change in the voltage value with respect to the change in the current value on the straight line connecting the two plotted points where the voltage value was around 3.5V.
  • Table 1 shows the DCR increase rates of the batteries of Examples 1 to 5 and Comparative Examples 1 to 3 obtained as described above.
  • Example 5 Compared to Example 2 in which 1.0 part by mass of lithium difluorobis (oxalato) phosphate was added, 0.5 part by mass of lithium difluorobis (oxalato) phosphate and 0. 1% of lithium bis (oxalato) borate. In Example 5 in which 5 parts by mass was added, it can be seen that the increase in DCR was further suppressed. From this, it is understood that the effect of further suppressing the increase in DCR can be obtained by mixing different kinds of oxalato complex salts. This is presumably because an SEI film that was stable and good for reduction was formed on the surface of the negative electrode by mixing two oxalate complex salts having different reductive decomposition actions.
  • the effect of suppressing the increase in DCR is particularly remarkable when the amount of lithium difluorobis (oxalato) phosphate is in the range of 0.5 to 2.0 parts by mass (Examples 1 to 4). It can be seen that when the amount added is 2.5 parts by mass (Comparative Example 3), the amount of SEI coating formed on the surface of the negative electrode becomes excessive, and as a result, the DCR increase rate increases.
  • 100 nonaqueous electrolyte secondary battery
  • 10 battery element
  • 11 positive electrode member
  • 12 negative electrode member
  • 13 separator
  • 20 outer packaging material

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

Abstract

L'invention concerne une batterie secondaire à électrolyte non aqueux qui a des caractéristiques améliorées de durée de vie. Un élément de batterie (10) de la batterie secondaire à électrolyte non aqueux comporte un élément électrode positive (11) qui contient une matière active d'électrode positive, un élément électrode négative (12) qui contient une matière active d'électrode négative et une solution d'électrolyte non aqueux qui contient un solvant non aqueux. La matière active d'électrode positive contient un composé acide phosphorique à contenant du lithium qui a une structure d'olivine. Au moins une sorte de sel de complexe oxalato qui a un élément choisi dans le groupe consistant en bore, phosphore, aluminium, gallium, arsenic et antimoine en tant que l'ion central ou l'atome central est ajoutée dans une quantité de 0,5-2,0 parties en masse (inclus) par rapport à 100 parties en masse de la solution d'électrolyte non aqueux.
PCT/JP2011/079016 2010-12-24 2011-12-15 Batterie secondaire à électrolyte non aqueux WO2012086507A1 (fr)

Priority Applications (1)

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JP2012549757A JPWO2012086507A1 (ja) 2010-12-24 2011-12-15 非水電解液二次電池

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JP2010-287610 2010-12-24
JP2010287610 2010-12-24

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2014123526A (ja) * 2012-12-21 2014-07-03 Toyota Motor Corp 非水電解液二次電池及びその製造方法
JP2015079726A (ja) * 2013-09-10 2015-04-23 株式会社村田製作所 非水電解質電池の製造方法
JP2018060672A (ja) * 2016-10-05 2018-04-12 トヨタ自動車株式会社 リチウムイオン二次電池の製造方法
US11411223B2 (en) * 2018-03-22 2022-08-09 Tdk Corporation Negative electrode and lithium ion secondary battery

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2007035354A (ja) * 2005-07-25 2007-02-08 Toyota Central Res & Dev Lab Inc リチウムイオン二次電池
JP2009070598A (ja) * 2007-09-11 2009-04-02 Hitachi Vehicle Energy Ltd リチウム二次電池
WO2010079565A1 (fr) * 2009-01-06 2010-07-15 株式会社村田製作所 Accumulateur à électrolyte non aqueux
JP2010198858A (ja) * 2009-02-24 2010-09-09 Toyota Central R&D Labs Inc リチウムイオン二次電池

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2007035354A (ja) * 2005-07-25 2007-02-08 Toyota Central Res & Dev Lab Inc リチウムイオン二次電池
JP2009070598A (ja) * 2007-09-11 2009-04-02 Hitachi Vehicle Energy Ltd リチウム二次電池
WO2010079565A1 (fr) * 2009-01-06 2010-07-15 株式会社村田製作所 Accumulateur à électrolyte non aqueux
JP2010198858A (ja) * 2009-02-24 2010-09-09 Toyota Central R&D Labs Inc リチウムイオン二次電池

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
S.S. ZHANG ET AL.: "An improved electrolyte for the LiFeP04 cathode working in a wide temperature range", JOURNAL OF POWER SOURCES, vol. 159, no. 1, 27 December 2005 (2005-12-27), pages 702 - 707, XP025084240, DOI: doi:10.1016/j.jpowsour.2005.11.042 *

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2014123526A (ja) * 2012-12-21 2014-07-03 Toyota Motor Corp 非水電解液二次電池及びその製造方法
JP2015079726A (ja) * 2013-09-10 2015-04-23 株式会社村田製作所 非水電解質電池の製造方法
WO2015076026A1 (fr) * 2013-09-10 2015-05-28 株式会社村田製作所 Procédé de fabrication d'une batterie à électrolyte non aqueux
JP2018060672A (ja) * 2016-10-05 2018-04-12 トヨタ自動車株式会社 リチウムイオン二次電池の製造方法
CN107919500A (zh) * 2016-10-05 2018-04-17 丰田自动车株式会社 锂离子二次电池的制造方法
CN107919500B (zh) * 2016-10-05 2020-03-27 丰田自动车株式会社 锂离子二次电池的制造方法
US11411223B2 (en) * 2018-03-22 2022-08-09 Tdk Corporation Negative electrode and lithium ion secondary battery

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