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WO2015075785A1 - Système et procédé pour batterie secondaire au lithium-ion permettant de diagnostiquer la détérioration d'une batterie secondaire au lithium-ion - Google Patents

Système et procédé pour batterie secondaire au lithium-ion permettant de diagnostiquer la détérioration d'une batterie secondaire au lithium-ion Download PDF

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Publication number
WO2015075785A1
WO2015075785A1 PCT/JP2013/081226 JP2013081226W WO2015075785A1 WO 2015075785 A1 WO2015075785 A1 WO 2015075785A1 JP 2013081226 W JP2013081226 W JP 2013081226W WO 2015075785 A1 WO2015075785 A1 WO 2015075785A1
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Prior art keywords
negative electrode
secondary battery
ion secondary
electrode potential
potential
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English (en)
Japanese (ja)
Inventor
井上　亮
亮平 中尾
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Hitachi Ltd
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Hitachi Ltd
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    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
    • G01R31/00—Arrangements for testing electric properties; Arrangements for locating electric faults; Arrangements for electrical testing characterised by what is being tested not provided for elsewhere
    • G01R31/36—Arrangements for testing, measuring or monitoring the electrical condition of accumulators or electric batteries, e.g. capacity or state of charge [SoC]
    • G01R31/382—Arrangements for monitoring battery or accumulator variables, e.g. SoC
    • G01R31/3835—Arrangements for monitoring battery or accumulator variables, e.g. SoC involving only voltage measurements
    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
    • G01R31/00—Arrangements for testing electric properties; Arrangements for locating electric faults; Arrangements for electrical testing characterised by what is being tested not provided for elsewhere
    • G01R31/36—Arrangements for testing, measuring or monitoring the electrical condition of accumulators or electric batteries, e.g. capacity or state of charge [SoC]
    • G01R31/392—Determining battery ageing or deterioration, e.g. state of health

Definitions

  • the present invention relates to a lithium ion secondary battery system and a lithium ion secondary battery deterioration diagnosis method.
  • Lithium ion secondary batteries change state of charge (SOC: State of Charge) or deteriorated state (SOH: State of Health) when stored in a high temperature environment or at a deep charge depth or after a charge / discharge cycle. . It is known that when the secondary battery deteriorates, the battery charge / discharge capacity decreases and the battery internal resistance increases. Therefore, the output of the system gradually decreases with deterioration.
  • Power storage means used for vehicle power supplies, smart house power supplies, etc. are large and require large capacity, and the battery cost is high in the overall system, and control that takes advantage of battery performance is necessary. Moreover, it is desirable that the replacement period of the storage battery is long. Since the input / output of the storage battery changes according to the deterioration, it is necessary to appropriately detect the deterioration state and perform various controls.
  • Patent Document 1 describes a method for quantitatively evaluating the deterioration states of the positive electrode, the negative electrode, and the electrolytic solution, respectively, by using the charge / discharge curves of the secondary battery.
  • Patent Document 2 discloses a technique for determining a deterioration state based on a capacity retention rate of a positive electrode of a lithium ion secondary battery, a capacity retention rate of a negative electrode, and a variation amount of the battery capacity.
  • Patent Document 3 discloses in advance that a rapid decrease in the life performance of a secondary battery occurs by using a value obtained from an electric quantity corresponding to each of a plurality of potential flat portions appearing in the negative electrode potential characteristics. A technique that can be perceived is disclosed.
  • Patent Document 1 describes a method for determining the state of a secondary battery. Based on the charge / discharge curves of a positive electrode and a negative electrode stored in advance, the charge / discharge curve of the secondary battery is reproduced by calculation. It describes a method for obtaining the effective weight of the positive electrode active material, the effective weight of the negative electrode active material, the amount of change in the use position between the positive electrode and the negative electrode, or the value of the parameter corresponding to these.
  • the state determination method described in Patent Document 1 it is necessary to eliminate as much as possible the influence of internal resistance included in the charge / discharge curve of the secondary battery. For that purpose, the current value at the time of measuring the charge / discharge curve must be reduced, and the measurement takes a long time. For this reason, it is difficult to determine the deterioration state every day and update the optimum battery usage method every day accordingly.
  • Patent Document 2 it is necessary to detect the positive electrode capacity and the negative electrode capacity
  • Patent Document 3 it is necessary to detect the negative electrode capacity.
  • a hybrid vehicle frequently accelerates and decelerates, frequently switches between input and output of the storage battery, and uses a large current value. Larger currents are required in railway vehicles and electric vehicles. For this reason, there has been a problem that it is difficult to obtain several open-circuit potentials for a specific capacity in a relaxed state after a lapse of time since the energization of the secondary battery is cut off during traveling.
  • the object of the present invention is to measure deterioration of a secondary battery by a simple method.
  • a lithium ion secondary battery system for diagnosing a deterioration state of a lithium ion secondary battery wherein the lithium ion secondary battery includes a positive electrode, a negative electrode, and a reference electrode, and the lithium ion secondary battery system includes a positive electrode and a reference electrode
  • a positive / negative potential detection unit that detects a positive electrode potential that is a potential difference between the negative electrode and a negative electrode potential that is a potential difference between the negative electrode and a reference electrode
  • a battery deterioration diagnosis unit that diagnoses a deterioration state of the lithium ion secondary battery
  • the battery deterioration diagnosis unit is a lithium ion secondary battery based on the correspondence relationship between the positive electrode potential and the negative electrode potential detected by the positive and negative electrode potential detection unit and the correspondence relationship between the positive electrode potential and the negative electrode potential in the initial state.
  • Lithium ion secondary battery system for diagnosing the deterioration state of batteries wherein the lithium ion secondary battery includes a positive electrode, a negative
  • the deterioration of the secondary battery can be measured by a simple method. Problems, configurations, and effects other than those described above will be clarified by the following description of embodiments.
  • FIG. 1 is an overall configuration diagram of a battery system according to an embodiment of the present invention. It is a block diagram of the battery module which concerns on one Embodiment of this invention. It is a figure which shows the circuit structure of the single battery cell controller which concerns on one Embodiment of this invention. It is a half sectional schematic diagram of the wound type lithium ion secondary battery applied according to an embodiment of the present invention. It is a figure which shows the circuit structure of the module controller which concerns on one Embodiment of this invention. It is a figure for demonstrating the positive electrode potential and negative electrode potential which concern on one Embodiment of this invention. It is a figure which shows the correspondence of the positive electrode potential and negative electrode potential which concern on one Embodiment of this invention.
  • Embodiments of the present invention will be described with reference to the drawings.
  • a case where the present invention is applied to a power storage device constituting a power source of a plug-in hybrid vehicle (PHEV) will be described as an example.
  • the configuration of the embodiment described below is also applied to a secondary battery control circuit of a secondary battery device that constitutes a power source for an industrial vehicle such as a passenger car such as a hybrid vehicle (HEV) or an electric vehicle (EV) or a hybrid railway vehicle. it can.
  • a case where a lithium ion battery is applied to a battery constituting the power storage unit will be described as an example.
  • FIG. 1 shows an example of the overall configuration of a battery system of a secondary battery device for a plug-in hybrid vehicle in the present embodiment.
  • the battery 1000 includes a battery module 1200 (battery module 1200a-1, battery module 1200a-2, battery module 1200b-1, battery module 1200b-2, battery, and the like, which includes a plurality of unit cells 1210 of FIG. 2 connected in series.
  • a voltage detection unit 1300 (voltage detection unit 1300a, voltage detection unit 1300b, voltage detection unit 1300c) for detecting the battery module and a battery module controller 1400 (battery module controller 1400a, A battery module controller 1400b, a battery module controller 1400c), a battery module 1200, and a database unit 1700 for storing information related to battery characteristics of the single battery 1210.
  • the module controller 1400 is transmitted from the voltage detection unit 1300, the battery voltage and temperature of the unit cell 1210 transmitted from the unit cell controller 1220 shown in FIG.
  • the total voltage value of the battery module 1200 is input, and the state of the battery module 1200 is detected based on the input information.
  • the result of the processing performed by the module controller 1400 is transmitted to the unit cell controller 1220 and the system controller 1500.
  • the system controller 1500 controls an inverter and a charger connected to the battery 1000 via the relay 1600 based on information of the module controller 1400.
  • Fig. 2 shows a configuration example of the battery module.
  • the battery module 1200 of FIG. 1 is configured by electrically connecting a plurality of unit cells 1210 (lithium ion batteries or cells) capable of storing and releasing electrical energy (charging and discharging DC power) in series.
  • the battery module 1200 includes a plurality of unit cells 1210 and a unit cell controller 1220 that monitors the state of the unit cells 1210.
  • One unit cell 1210 will be described by taking as an example a case where the output voltage is 3.0 to 4.2 V (average output voltage: 3.6 V), but other voltage specifications may be used. .
  • the unit cells 1210 constituting the battery module 1200 are grouped into a predetermined number of units when managing and controlling the state.
  • the grouped unit cells 1210 are electrically connected in series.
  • the predetermined number of units may be equal divisions such as 1, 4, 6, etc., or may be combined divisions such as combining 4 and 6 units. is there.
  • the unit cell controller 1220 that monitors the state of the unit cell 1210 that constitutes the cell module 1200 of FIG. 2 includes a plurality of unit cell controllers such as the unit cell controllers 1220-1 and 1220-2.
  • a single battery controller 1220-1 is assigned to the single battery groups 1230-1 and 1230-2 grouped into groups.
  • the unit cell controller 1220-1 operates by receiving power from the allocated unit cell group 1230-1, and monitors and controls the states of the unit cells 1210-1 and 1210-2 constituting the unit cell group 1230-1. .
  • FIG. 3 is a diagram showing a circuit configuration of the cell controller.
  • the cell controller 1220 includes a voltage detection unit 1221, a control circuit 1223, a signal input / output circuit 1224, a temperature detection unit 1222, and a positive / negative potential detection unit (positive / negative potential detection unit) 1225.
  • the voltage detection unit 1221 measures the voltage between the terminals of each single battery 1210.
  • the temperature detection unit 1222 measures the temperature of the cell group 1230.
  • the positive electrode / negative electrode potential detector 1225 measures a positive electrode potential that is an actual measurement value of a potential difference between the positive electrode and the reference electrode, and measures a negative electrode potential that is an actual measurement value of the potential difference between the negative electrode and the reference electrode.
  • the control circuit 1223 receives the measurement results from the voltage detection unit 1221 and the temperature detection unit 1222 and transmits them to the module controller 1200 via the signal input / output circuit 1224. Note that a circuit configuration that is generally mounted on the unit cell controller 1220 and that equalizes voltage variations between the unit cells 1210 caused by self-discharge and variation in consumption current is described as being known. Was omitted.
  • the temperature detector 1222 provided in the cell controller 1220 in FIG. 3 has a function of measuring the temperature of the cell group 1230.
  • the temperature detection unit 1222 measures one temperature as the whole cell group 1230 and treats the temperature as a temperature representative value of the cell 1210 constituting the cell group 1230.
  • the temperature measured by the temperature detector 1222 is used for various calculations for detecting the state of the unit cell 1210, unit cell group 1230, or the battery module 1200. Since FIG. 3 is based on this assumption, the single battery controller 1220 is provided with one temperature detection unit 1222.
  • a temperature detector 1222 is provided for each unit cell 1210 to measure the temperature for each unit cell 1210, and various calculations can be executed based on the temperature for each unit cell 1210.
  • the configuration of the unit cell controller 1220 is simplified when the unit 1222 is provided.
  • the temperature detection unit 1222 is simply shown. Actually, a temperature sensor is installed in the temperature measurement target, the installed temperature sensor outputs temperature information as a voltage, and the measurement result is transmitted to the signal input / output circuit 1224 via the control circuit 1223, and the signal input / output circuit 1224 is output. Outputs the measurement result to the outside of the unit cell controller 1220.
  • a function for realizing this series of flows is mounted on the single battery controller 1220 as a temperature detection unit 1222, and the voltage detection unit 1221 can be used for measuring temperature information (voltage).
  • the positive / negative electrode potential detection unit 1225 provided in the single battery controller 1220 has a function of measuring the positive and negative electrode potentials of the single battery group 1230.
  • the positive electrode / negative electrode potential detection unit 1225 measures one positive electrode and negative electrode potential as a whole cell group 1230 and treats the potential as a positive / negative representative value of the cell 1210 constituting the cell group 1230.
  • the potential measured by the positive / negative electrode potential detection unit 1225 is used for various calculations for detecting the state of the unit cell 1210, unit cell group 1230, or the battery module 1200. Since FIG. 3 is based on this assumption, the single battery controller 1220 is provided with one positive / negative potential detection unit 1225.
  • a positive / negative electrode potential detector 1225 is provided for each unit cell 1210 to measure the potential for each unit cell 1210, and various calculations can be performed based on the unit cell 1210 potential.
  • the configuration of the unit cell controller 1220 becomes simpler when the two positive / negative electrode potential detectors 1225 are provided.
  • the positive / negative electrode potential detector 1225 is simply shown. Actually, a reference electrode is installed in the potential measurement target, and the installed reference electrode outputs potential information, and the measurement result is transmitted to the signal input / output circuit 1224 via the control circuit 1223, and the signal input / output circuit 1224 is simply connected. The measurement result is output outside the battery controller 1220. A function for realizing this series of flows is mounted on the single battery controller 1220 as a positive / negative electrode potential detection unit 1225, and the voltage detection unit 1221 can be used for measuring potential information.
  • FIG. 4 shows an embodiment of a lithium ion secondary battery to which the present invention is applied, and shows a schematic cross-sectional side view of a wound lithium ion secondary battery 2000.
  • the lithium ion secondary battery 2000 uses lithium as an electrode reactant.
  • the lithium ion secondary battery 2000 is a so-called cylindrical type, and a pair of strip-shaped positive electrodes 2003, a strip-shaped negative electrode 2006, and a separator 2007 are wound inside a substantially hollow cylindrical negative electrode battery can 2013.
  • the positive electrode 2003 and the negative electrode 2006 are disposed to face each other with a separator 2007 interposed therebetween, and an electrolyte solution 2017 is injected therein.
  • a reference electrode 2015 is disposed in the negative electrode battery can 2013.
  • the negative electrode battery can 2013 is made of, for example, iron (Fe) plated with nickel (Ni), and has one end closed and the other end open. Inside the negative electrode battery can 2013, a pair of positive electrode insulating material 2010 and negative electrode insulating material 2011 are arranged perpendicular to the wound peripheral surface so as to sandwich the wound electrode group.
  • a positive electrode battery lid 2012 is attached to the open end of the negative electrode battery can 2013 by caulking through a gasket 2014, and the inside of the negative electrode battery can 2013 is sealed.
  • the positive battery lid 2012 is made of the same material as the negative battery can 2013, for example.
  • a positive electrode lead 2008 made of, for example, aluminum (Al) or the like is connected to the positive electrode 2003 of the wound electrode group, and a negative electrode lead 2009 made of, for example, nickel (Ni) or the like is connected to the negative electrode 2006.
  • the positive electrode lead 2008 is electrically connected to the positive electrode battery lid 2012, and the negative electrode lead 2009 is welded and electrically connected to the negative electrode battery can 2013.
  • the shape of the electrode winding group in the present invention is not necessarily a true cylindrical shape, and may be a long cylindrical shape having an elliptic winding group cross section or a prism-like shape having a rectangular winding cross section.
  • a cylindrical battery can with a bottom is filled with an electrode winding group and an electrolytic solution, and a tab for taking out current from the electrode plate is sealed in a state welded to the lid and the battery can.
  • the form is preferable, it is not particularly limited to this form.
  • the shape of the battery includes a wound cylindrical shape, a flat oval shape, a wound square shape, and a laminated shape, and any shape may be selected.
  • the present invention may also be applied to a stacked lithium ion secondary battery in which a plurality of positive electrodes 2003 and a plurality of negative electrodes 2006 are alternately stacked with separators 2007 interposed therebetween.
  • the positive electrode 2003, the negative electrode 2006, the electrolyte solution 2017, the separator 2007, and the reference electrode 2015 will be described.
  • the positive electrode 2003 is formed by applying a positive electrode mixture layer 2002 composed of a positive electrode active material and a binder resin onto an aluminum foil that is a positive electrode current collector 2001. Further, a conductive agent may be further added to the positive electrode mixture layer 2002 in order to reduce electronic resistance.
  • the positive electrode 2003 can be obtained by applying a positive electrode paste containing a positive electrode active material, a conductive material, a binder, and the like to the surface of the positive electrode current collector 2001.
  • a positive electrode material paste is prepared using a positive electrode active material, a conductive material, graphite, and a binder in consideration of the solid weight during drying and using a solvent.
  • the positive electrode material paste is applied to the aluminum foil used as the positive electrode current collector 2001, dried at 80 ° C., pressed with a pressure roller, and dried at 120 ° C. to form the positive electrode mixture layer 2002 as the positive electrode current collector. Formed in 2001.
  • LiM x PO 4 Fe or Mn, 0.01 ⁇ x ⁇ 0.4
  • LiMn 1-x M x PO 4 M: divalent cation other than Mn, 0.01 ⁇ It may be an orthorhombic phosphate compound having symmetry of the space group Pnma where x ⁇ 0.4).
  • the binder resin may be any material that allows the material constituting the positive electrode mixture layer 2002 and the positive electrode current collector 2001 to be in close contact.
  • a homopolymer or copolymer such as vinylidene fluoride, tetrafluoroethylene, acrylonitrile, or ethylene oxide may be used. Examples thereof include merging and styrene-butadiene rubber.
  • the conductive agent is, for example, a carbon material such as carbon black, graphite, carbon fiber, and metal carbide, and each may be used alone or in combination.
  • the negative electrode 2006 is formed by applying a negative electrode mixture layer 2005 composed of a negative electrode active material and a binder resin on the negative electrode current collector 2004.
  • amorphous carbon material natural graphite, composite carbonaceous material in which a film is formed on natural graphite by dry CVD (Chemical Vapor Deposition) method or wet spray method, resin material such as epoxy and phenol
  • resin material such as epoxy and phenol
  • artificial graphite produced by firing using a pitch-based material obtained from petroleum or coal, silicon (Si), graphite mixed with silicon, or the like can be used.
  • a conductive agent may be further added to the negative electrode mixture layer 2005 in order to reduce electronic resistance.
  • the conductive agent is, for example, a carbon material such as carbon black, graphite, carbon fiber, and metal carbide, and each may be used alone or in combination.
  • the binder resin may be any material as long as the material constituting the negative electrode mixture layer 2005 and the negative electrode current collector 2004 are in close contact with each other.
  • a homopolymer or copolymer such as tetrafluoroethylene, acrylonitrile, ethylene oxide, styrene -Butadiene rubber can be mentioned.
  • Water can be used as a solvent constituting the binder resin solution. These solvents may be used alone or in combination.
  • a metal foil or metal mesh of stainless steel copper, nickel, titanium, or the like can be used.
  • copper is preferable, and zirconia and zinc-containing copper having high heat resistance are also preferable.
  • the electrolytic solution mainly includes a solvent, an additive, and an electrolyte.
  • the electrolytic solution 2017 of a lithium ion secondary battery that can be operated in a wide voltage range is required to have a withstand voltage characteristic, and an organic electrolytic solution using an organic compound as a solvent is used.
  • An electrolyte having a lithium salt as an electrolyte and carbonate as a solvent can be made highly conductive, and is widely used as an electrolyte for a lithium ion secondary battery 2000 in that it has a wide potential window.
  • an electrolytic solution 2017 composed of a lithium salt and a carbonate solvent reacts on the negative electrode surface of the lithium ion secondary battery 2000.
  • an additive having a reduction reaction potential higher than that of the solvent is often added to the electrolytic solution 2017.
  • These additives themselves undergo reductive decomposition to form an inactive film on the electrode surface. And the film formed on the electrode surface suppresses the continued electrode reaction.
  • the lithium salt used for the electrolyte solution 2017 is not particularly limited, but for inorganic lithium salts, LiPF 6 , LiBF 4 , LiClO 4 , LiI, LiCl, LiBr, etc., and for organic lithium salts, LiB [OCOCF 3 ] 4.
  • LiB [OCOCF 2 CF 3 ] 4 LiPF 4 (CF 3 ) 2 , LiN (SO 2 CF 3 ) 2 , LiN (SO 2 CF 2 CF 3 ) 2 or the like can be used.
  • VC vinylene carbonate
  • FEC fluoroethylene carbonate
  • a solvent ethylene carbonate (EC), dimethyl carbonate (DMC), propylene carbonate, butylene carbonate (BC), dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), diethyl carbonate (DEC), methyl propyl carbonate (MPC)
  • An aprotic organic solvent such as ethylpropyl carbonate (EPC), or a solvent of two or more of these mixed organic compounds is used.
  • EPC ethylpropyl carbonate
  • the lithium ion secondary battery 2000 has good discharge characteristics during the charge / discharge cycle, low temperature and high current discharge characteristics, and long-term storage or long-term high-temperature storage characteristics.
  • an organic electrolytic solution 2017 that satisfies these requirements is required.
  • ion-conducting polymers such as polyethylene oxide, polyacrylonitrile, polyvinylidene fluoride, polymethyl methacrylate, polyhexafluoropropylene, and polyethylene oxide are used as the electrolyte.
  • polyethylene oxide polyacrylonitrile
  • polyvinylidene fluoride polymethyl methacrylate
  • polyhexafluoropropylene polyethylene oxide
  • the separator 2007 related to the lithium ion secondary battery 2000 a separator used in a known lithium ion secondary battery 2000 can be used.
  • the separator 2007 includes a microporous film made of polyolefin such as polyethylene and polypropylene, a nonwoven fabric, and the like.
  • the positive electrode potential and the negative electrode potential are measured with the reference electrode 2015.
  • the reference electrode 2015 is provided via a separator 2007.
  • the reference electrode 2015 is formed by coating a metal substrate such as nickel as a surface electrode with a metal such as lithium, tin, silver, platinum, or lithium titanate, which is a metal different from the metal substrate.
  • a metal substrate such as nickel as a surface electrode
  • LiFePO 4, LiMnPO 4, metal oxides such as, such as a reference electrode consisting of Li metal can be used.
  • a reference electrode tab 2016 is connected to the reference electrode 2015, and the reference electrode tab 2016 is led out to the outside.
  • the lithium ion secondary battery which is one embodiment of the present invention can provide a lithium ion secondary battery with reduced internal resistance of the battery, the power source of the hybrid vehicle requiring high output and the electric control of the vehicle It can be widely used as a system power source and a backup power source, and is also suitable as a power source for industrial equipment such as railways, power tools and forklifts.
  • FIG. 5 is a diagram showing the configuration of the module controller.
  • the module controller 1400 includes a positive / negative electrode state detection unit 1410 and a battery deterioration diagnosis unit 1420.
  • FIG. 6 is a diagram schematically showing a method of measuring the positive electrode potential and the negative electrode potential using the reference electrode 2015.
  • a battery voltage Vcell that is a voltage between the positive electrode 2003 and the negative electrode 2006, a positive electrode potential Vp that is an actual measurement value between the reference electrode 2015 and the positive electrode 2003, and a negative electrode potential Vn that is an actual measurement value between the reference electrode 2015 and the negative electrode 2006 are obtained. taking measurement.
  • the position of the reference electrode 2015 of the lithium ion secondary battery in FIG. 4 is positioned at the center of the wound electrode group, but it may be installed between the battery can 2013 and the electrode wound group via the separator 2007. As long as the positive electrode potential Vp and the negative electrode potential Vn can be measured stably, it is not particularly limited to this form.
  • the positive electrode / negative electrode state detection unit 1410 in FIG. 5 is between the positive electrode potential Vp and the reference electrode 2015 and the negative electrode 2006 which are actually measured values between the reference electrode 2015 and the positive electrode 2003 detected by the positive electrode / negative electrode battery detection unit 1225.
  • the corresponding relationship of the negative electrode potential Vn, which is an actually measured value, is calculated.
  • the correspondence between the positive electrode potential Vp and the negative electrode potential Vn detected by the positive electrode / negative electrode state detection unit 1410 is stored in the database unit 1700 in advance in the initial state positive electrode potential Vp and negative electrode potential Vn. And the corresponding relationship.
  • the database unit 1700 includes a positive electrode potential Vp that is an actual measurement value between the reference electrode 2015 and the positive electrode 2003 in an initial state, a negative electrode potential Vn that is an actual measurement value between the reference electrode 2015 and the negative electrode 2006, and a battery deterioration state (SOH: It is stored as a data table that describes the correspondence with (State of health).
  • the deterioration state SOH of the lithium ion secondary battery is calculated from the information on the positive electrode potential Vp and the negative electrode potential Vn detected by the positive electrode / negative electrode battery detection unit 1225.
  • the calculated battery deterioration state SOH is reflected in the control parameter, the permissible current and upper / lower limit voltage of the detected battery state are calculated, and the battery module 1200 is charged / discharged according to the input / output command based on this.
  • the initial state refers to a new state in which metallic lithium is hardly deposited in the lithium ion secondary battery 2000.
  • an intermediate state between when the lithium ion secondary battery 2000 is new and when the lithium ion secondary battery 2000 is most deteriorated may be set as the initial state in addition to when the lithium ion secondary battery 2000 is new.
  • the initial state is assumed to be new.
  • FIG. 7 shows the correspondence between the positive electrode potential and the negative electrode potential.
  • the positive electrode active material is LiMn 1/3 Ni 1/3 Co 1/3 O 2 .
  • the negative electrode active material is graphite. In FIG. 7, it can be seen that the correspondence between the positive electrode potential Vp and the negative electrode potential Vn changes as the number of charge / discharge cycles increases.
  • FIG. 8 schematically shows a change in monopolar potential due to a decrease in monopolar capacity.
  • FIG. 8A shows the characteristics of the positive electrode 2003 and
  • FIG. 8B shows the characteristics of the negative electrode 2006.
  • Q_1p of the positive electrode capacity axis is the single electrode capacity of the positive electrode 2003 in the initial state of the lithium ion secondary battery 2000.
  • Q_2p on the axis of the positive electrode capacity is a single electrode capacity of the positive electrode 2003 after the lithium ion secondary battery 2000 is deteriorated.
  • Q_1n of the axis of the negative electrode capacity is the single electrode capacity of the negative electrode 2006 in the initial state of the lithium ion secondary battery 2000.
  • Q_2n of the axis of the negative electrode capacity is a single electrode capacity of the negative electrode 2006 after the lithium ion secondary battery 2000 is deteriorated.
  • the positive electrode capacity changes from Q_1p to Q_2p.
  • the negative electrode 2006 the negative electrode capacity changes from Q_1n to Q_2n when the lithium receiving ability decreases.
  • the capacity change of the positive electrode 2003 and the negative electrode 2006 and the amount of change in relative position with respect to the capacity axis between the positive electrode 2003 and the negative electrode 2006 are related. For this reason, it takes a long time to measure the parameter values corresponding to these, and therefore, it takes a long time to detect the battery deterioration state of the lithium ion secondary battery 2000.
  • the battery deterioration state can be detected based on the correspondence relationship between the positive electrode potential Vp and the negative electrode potential Vn, and the positive electrode potential Vp corresponding to the negative electrode potential Vn and the battery deterioration state corresponding to them can be detected in advance. By acquiring, the battery deterioration state at a certain time can be estimated.
  • the positive / negative electrode potential detection unit 1225 detects the positive / negative potential during charging / discharging, which is the positive / negative potential of the lithium ion secondary battery 2000 when charging / discharging of the lithium ion secondary battery 2000 is stopped.
  • the database unit 1700 stores the charging / discharging pause positive / negative potential, and the battery deterioration diagnosis unit 1420 is mounted in the database unit 1700 in advance with the charging / discharging halting positive / negative potential stored in the database unit 1700.
  • Diagnosing the deterioration state of the lithium ion secondary battery 2000 based on the correspondence relationship between the positive electrode potential and the negative electrode potential at the time of a new article can more accurately grasp the battery deterioration state.
  • a current flows through the lithium ion secondary battery 2000 or immediately after the current is cut off, there is a difference in lithium concentration in the active material or in the electrolyte solution. It is difficult to obtain the positive electrode potential Vp.
  • Table 1 shows the correspondence between positive electrode potential, negative electrode potential, and battery capacity.
  • the correspondence relationship between the positive electrode potential Vp and the battery capacity with respect to the negative electrode potential Vn is shown.
  • the database is based on the correspondence between the positive electrode potential Vp and the negative electrode potential Vn measured at a certain time.
  • the battery capacity can be estimated at a certain point in time from the battery deterioration state stored in the unit 1700.
  • Table 2 shows the correspondence between the positive electrode potential, the negative electrode potential, and the battery internal resistance.
  • the correspondence relationship between the positive electrode potential Vp and the battery internal resistance with respect to the negative electrode potential Vn is shown.
  • the battery internal resistance changes with the change of the positive electrode potential Vp, and the battery internal resistance at a certain time can be estimated.
  • the battery internal resistance can be estimated at a certain point in time from the battery deterioration state stored in the database unit 1700.
  • the negative electrode potential Vn is set to 0.6 V.
  • any potential can be used as long as the correspondence relationship between the negative electrode potential Vn and the positive electrode potential Vp can be stably obtained, and the present invention is not limited to this potential.
  • FIG. 9 is a system flow diagram of a secondary battery system according to an embodiment of the present invention.
  • Step 101 a signal related to charging / discharging of the lithium ion secondary battery 2000 is transmitted from the system controller 1500 to the battery module 1200 to be charged / discharged, and charging / discharging of the lithium ion secondary battery 2000 is started.
  • the voltage detector 1221 in the battery module 1200 that has received the signal measures the voltage across the terminals of each unit cell 1210.
  • the temperature detection unit 1222 measures the temperature of the cell group 1230.
  • the positive electrode / negative electrode potential detector 1225 measures the positive electrode potential and the negative electrode potential.
  • the control circuit 1223 receives the measurement results from the voltage detection unit 1221 and the temperature detection unit 1222 and transmits them to the module controller 1400 via the signal input / output circuit 1224.
  • the positive electrode potential Vp which is an actual measurement value between the reference electrode 2015 and the positive electrode 2003 detected by the positive electrode / negative electrode battery detection unit 1225, the reference electrode 2015, and the negative electrode 2006.
  • the correspondence relationship of the negative electrode potential Vn which is an actually measured value, is calculated.
  • the correspondence between the positive electrode potential Vp and the negative electrode potential Vn detected by the positive electrode / negative electrode state detection unit 1410 is stored in the database unit 1700 in advance in the initial state positive electrode potential Vp and negative electrode potential Vn. And the corresponding relationship.
  • the database unit 1700 includes a positive electrode potential Vp that is an actual measurement value between the reference electrode 2015 and the positive electrode 2003 in an initial state, a negative electrode potential Vn that is an actual measurement value between the reference electrode 2015 and the negative electrode 2006, and a battery deterioration state (SOH: A data table describing the correspondence with (State of health) is stored.
  • a battery deterioration state is calculated from information on the positive electrode potential Vp and the negative electrode potential Vn detected by the positive electrode / negative electrode battery detection unit 1410.
  • the calculation result of the battery deterioration state of the module controller 1400 is transmitted to the single battery controller 1220 and the system controller 1500.
  • the system controller 1500 manages and controls the charge / discharge state based on the information of the module controller 1400.
  • the battery 1000 includes the system controller 1500 and the battery module 1200, and is detected by the positive electrode / negative electrode battery detection unit 1225 in the positive electrode / negative electrode state detection unit 1410 of the module controller 1400.
  • the battery deterioration diagnosis unit 1420 calculates the correspondence between the positive electrode potential Vp, which is an actual measurement value between the reference electrode 2015 and the positive electrode 2003, and the negative electrode potential Vn, which is an actual measurement value between the reference electrode 2015 and the negative electrode 2006.
  • the correspondence relationship between the positive electrode potential Vp and the negative electrode potential Vn detected by the positive electrode / negative electrode state detection unit 1410 is compared with the correspondence relationship between the positive electrode potential Vp and the negative electrode potential Vn in the initial state stored in the database unit 1700 in advance.
  • Secondary battery system capable of estimating the deterioration state of the battery by a simple method It is possible to provide.
  • Embodiment 2 of the present invention will be described with reference to FIGS. 4 and 9 to 12.
  • a lithium ion secondary battery 2000 was used for the effect verification test of Embodiment 2 of the present invention.
  • a wound type lithium ion secondary battery 2000 as shown in FIG. 4 was produced.
  • a cylindrical battery (hereinafter referred to as a 18650 type battery) having a battery size diameter of 18 mm and a length of 65 mm was used for the verification test.
  • the positive electrode active material is LiMn 1/3 Ni 1/3 Co 1/3 O 2 .
  • the negative electrode active material is an amorphous carbon material. The description of the same components as those in the first embodiment is omitted.
  • FIG. 10 shows the correspondence between the positive electrode potential Vp and the negative electrode potential Vn in the charge / discharge cycle. It can be seen that the correspondence between the positive electrode potential Vp and the negative electrode potential Vn changes as the number of charge / discharge cycles increases.
  • Table 3 shows the correspondence between positive electrode potential, negative electrode potential, and battery capacity.
  • the correspondence relationship between the positive electrode potential Vp and the battery capacity with respect to the negative electrode potential Vn is shown.
  • the database is based on the correspondence between the positive electrode potential Vp and the negative electrode potential Vn measured at a certain time.
  • the battery capacity can be estimated at a certain point in time from the battery deterioration state stored in the unit 1700.
  • Table 4 shows the correspondence between positive electrode potential, negative electrode potential, and battery internal resistance.
  • the correspondence relationship between the positive electrode potential Vp and the battery internal resistance with respect to the negative electrode potential Vn is shown.
  • the battery internal resistance changes with the change of the positive electrode potential Vp, and the battery internal resistance at a certain time can be estimated.
  • the battery internal resistance can be estimated at a certain point in time from the battery deterioration state stored in the database unit 1700.
  • the negative electrode potential Vp is set to 0.6 V.
  • the potential is not limited to this potential as long as the correspondence between the negative electrode potential Vn and the positive electrode potential Vp can be acquired stably.
  • Embodiment 3 of the present invention will be described with reference to FIGS. 4 and 11 to 13.
  • the charge / discharge current is limited without limiting the upper / lower limit voltage.
  • the positive / negative battery detection unit detects the positive electrode potential with respect to the preset negative electrode potential, and when the absolute value of the positive electrode potential corresponding to the negative electrode potential is larger than the predetermined potential threshold value Vp2, the lithium ion being charged / discharged The charge / discharge current value of the secondary battery is limited.
  • FIG. 11 is a diagram showing a circuit configuration of a module controller according to an embodiment of the present invention.
  • the module controller 1400 includes a positive / negative electrode state detection unit 1410, a battery deterioration diagnosis unit 1420, and a current limit value calculation unit 1430.
  • the lithium ion secondary battery 2000 was used for the effect verification test of Embodiment 3 of the present invention.
  • a wound lithium ion secondary battery 2000 as shown in FIG. 4 was produced.
  • the positive electrode active material is LiMn 1/3 Ni 1/3 Co 1/3 O 2 .
  • the negative electrode active material is graphite. The description of the same components as those in the first and second embodiments is omitted.
  • FIG. 12 is a system flow diagram of the secondary battery system according to one embodiment of the present invention.
  • Step 201> In the system flow diagram of the secondary battery system in FIG. 12, first, a signal related to charging / discharging of the lithium ion secondary battery 2000 is transmitted from the system controller 1500 to the battery module 1200 and charging / discharging of the lithium ion secondary battery 2000 is started. To do.
  • the voltage detector 1221 in the battery module 1200 that has received the signal measures the voltage across the terminals of each unit cell 1210.
  • the temperature detection unit 1222 measures the temperature of the cell group 1230.
  • the positive electrode / negative electrode potential detector 1225 measures the positive electrode potential and the negative electrode potential.
  • the current detection unit 1100 measures the current flowing through the cell group 1230.
  • the control circuit 1223 receives the measurement results from the voltage detection unit 1221 and the temperature detection unit 1222 and transmits them to the module controller 1400 via the signal input / output circuit 1224.
  • the positive electrode potential Vp which is an actual measurement value between the reference electrode 2015 and the positive electrode 2003 detected by the positive electrode / negative electrode battery detection unit 1225, the reference electrode 2015, and the negative electrode 2006.
  • the correspondence relationship of the negative electrode potential Vn which is an actually measured value, is calculated.
  • the correspondence between the positive electrode potential Vp and the negative electrode potential Vn detected by the positive electrode / negative electrode state detection unit 1410 is stored in the database unit 1700 in advance in the initial state positive electrode potential Vp and negative electrode potential Vn. And the corresponding relationship.
  • the database unit 1700 includes a positive electrode potential Vp that is an actual measurement value between the reference electrode 2015 and the positive electrode 2003 in an initial state, a negative electrode potential Vn that is an actual measurement value between the reference electrode 2015 and the negative electrode 2006, and a battery deterioration state (SOH: A data table describing the correspondence with (State of health) is stored.
  • a battery deterioration state is calculated from information on the positive electrode potential Vp and the negative electrode potential Vn detected by the positive electrode / negative electrode battery detection unit 1225.
  • the battery deterioration diagnosis unit 1420 of the module controller 1200 limits the charge / discharge current when the absolute value of the positive electrode potential Vp1 with respect to the negative electrode potential Vn1 is larger than a predetermined potential threshold value Vp2.
  • the process returns to step 201.
  • FIG. 13 shows a schematic diagram of the correspondence between the positive electrode potential Vp and the negative electrode potential Vn according to an embodiment of the present invention.
  • Vp1 on the axis of the positive electrode potential is a positive electrode potential with respect to the negative electrode potential Vn1 in the initial state of the lithium ion secondary battery 2000.
  • Vp2 on the axis of the positive electrode potential is a positive electrode potential with respect to the negative electrode potential Vn1 after deterioration of the lithium ion secondary battery 2000.
  • Predetermined potential threshold value Vp2 is determined from the correspondence relationship between positive electrode potential Vp after deterioration, negative electrode potential Vn, and battery deterioration state (SOH: State of health).
  • SOH State of health
  • the current limit value calculation unit 1430 calculates the internal resistance R from the battery voltage V, current I, temperature T, and time t.
  • the tendency of the increase rate of the internal resistance with respect to the charge / discharge cycle varies greatly depending on the environmental temperature. Therefore, it is preferable to appropriately set a limit value that is a threshold value of the internal resistance in accordance with a temperature change.
  • Step 207> The charge / discharge current value Imax1 is calculated using the battery voltage V and the temperature T from the internal resistance R calculated by the current limit calculation unit 1430. If the battery has not deteriorated, the process returns to step 202, and the current I, time t, temperature T, battery voltage V, positive electrode potential Vp, and negative electrode potential Vn are measured.
  • the charge / discharge current value of the lithium ion secondary battery 2000 during charge / discharge is limited.
  • the charge / discharge current value of the lithium ion secondary battery 2000 being charged / discharged is set to a predetermined current value or less.
  • the current limit value calculation unit 1430 determines the charge / discharge current Imax1.
  • the result of the charge / discharge current limit value of the current limit value calculation unit 1430 of the module controller 1400 is transmitted to the cell controller 1220 and the system controller 1500. Based on the information of the module controller 1400, the system controller 1500 makes it smaller than the charge / discharge current value before exceeding the potential threshold value Vp2.
  • the potential threshold corresponding to the correspondence relationship between the positive electrode potential Vp and the negative electrode potential Vn after deterioration and the battery deterioration state (SOH: State of health) is set in advance and becomes a potential higher than that potential
  • SOH State of health
  • Embodiment 4 of the present invention will be described with reference to FIGS. 4 and 14 to 15.
  • the current value is not limited and the upper and lower limit voltages are limited.
  • the battery state detection unit detects the end-of-charge voltage and the end-of-discharge voltage of the secondary battery
  • the positive / negative battery detection unit detects the positive electrode potential with respect to the preset negative electrode potential, and the positive electrode corresponding to the negative electrode potential.
  • the absolute value of the potential is larger than a predetermined potential threshold value Vp2
  • the charge end voltage and the discharge end voltage of the lithium ion secondary battery being charged / discharged are limited.
  • FIG. 14 is a diagram showing a circuit configuration of the module controller. It includes a positive / negative electrode state detection unit 1410, a battery deterioration diagnosis unit 1420, and a voltage limit value calculation unit 1440.
  • FIG. 15 is a system flow diagram of a lithium ion secondary battery system according to an embodiment of the present invention.
  • Step 301> In the system flow of the lithium ion secondary battery system in FIG. 15, first, a signal related to charging / discharging of the lithium ion secondary battery 2000 is transmitted from the system controller 1500 to the battery module 1200, and charging / discharging of the lithium ion secondary battery 2000 is performed. Start.
  • the voltage detector 1221 in the battery module 1200 that has received the signal measures the voltage across the terminals of each unit cell 1210.
  • the temperature detection unit 1222 measures the temperature of the cell group 1230.
  • the positive electrode / negative electrode potential detector 1225 measures the positive electrode potential and the negative electrode potential.
  • the control circuit 1223 receives the measurement results from the voltage detection unit 1221 and the temperature detection unit 1222 and transmits them to the module controller 1400 via the signal input / output circuit 1224.
  • the positive electrode potential Vp which is an actual measurement value between the reference electrode 2015 and the positive electrode 2003 detected by the positive electrode / negative electrode battery detection unit 1225, the reference electrode 2015, and the negative electrode 2006.
  • the correspondence relationship of the negative electrode potential Vn which is an actually measured value, is calculated.
  • the correspondence between the positive electrode potential Vp and the negative electrode potential Vn detected by the positive electrode / negative electrode state detection unit 1410 is stored in the database unit 1700 in advance in the initial state positive electrode potential Vp and negative electrode potential Vn. And the corresponding relationship.
  • the database unit 1700 includes a positive electrode potential Vp that is an actual measurement value between the reference electrode 2015 and the positive electrode 2003 in an initial state, a negative electrode potential Vn that is an actual measurement value between the reference electrode 2015 and the negative electrode 2006, and a battery deterioration state (SOH: A data table describing the correspondence with (State of health) is stored.
  • Step 305> A battery deterioration state is calculated from information on the positive electrode potential Vp and the negative electrode potential Vn detected by the positive electrode / negative electrode battery detection unit 1225. If the battery is not deteriorated, the process returns to step 302, and the current I, time t, temperature T, battery voltage V, positive electrode potential Vp, and negative electrode potential Vn are measured. When it is determined that the battery has deteriorated, that is, when the absolute value of the positive electrode potential corresponding to the negative electrode potential is larger than the predetermined potential threshold value Vp3, the process proceeds to step 306.
  • Step 306> When it is determined that the battery has deteriorated, the battery deterioration diagnosis unit 1420 of the module controller 1200 determines that the correspondence between the positive electrode potential Vp and the negative electrode potential Vn is greater than the potential threshold value Vp3 stored in the database unit 1700 in advance.
  • the upper and lower limit charge / discharge voltage values are limited.
  • Voltage limit value calculation unit 1440 measures upper limit voltage Vmax1 that is a charge end voltage and Vmin1 that is a discharge end voltage.
  • Voltage limit value calculation unit 1440 determines upper limit voltage value Vmax1 and lower limit voltage value Vmin1.
  • Step 307 The end-of-charge voltage and end-of-discharge voltage of the lithium ion secondary battery 2000 during charge / discharge are limited. In other words, the end-of-charge voltage and end-of-discharge voltage of the lithium ion secondary battery 2000 being charged / discharged are set within a predetermined voltage range.
  • the result of the upper and lower limit charge / discharge voltage values of the voltage limit value calculation unit 1440 of the module controller 1400 is transmitted to the cell controller 1220 and the system controller 1500.
  • the system controller 1500 controls the upper and lower limit voltage values based on the information of the module controller 1400.
  • the potential threshold corresponding to the correspondence relationship between the positive electrode potential Vp and the negative electrode potential Vn after deterioration and the battery deterioration state (SOH: State of health) is set in advance and becomes a potential higher than that potential
  • SOH State of health

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Abstract

La présente invention concerne la mesure de la détérioration d'une batterie secondaire au moyen d'un procédé simple. Le système pour batterie secondaire au lithium-ion permet de diagnostiquer l'état de détérioration d'une batterie secondaire au lithium-ion qui comporte une électrode positive, une électrode négative et une électrode de référence, le système pour batterie secondaire au lithium-ion comprenant une unité de détection de potentiels d'électrodes négatives et positives servant à détecter le potentiel de l'électrode positive, qui est la différence de potentiel entre l'électrode positive et l'électrode de référence, et le potentiel de l'électrode négative, qui est à la différence de potentiel entre l'électrode négative et l'électrode de référence, et une unité de diagnostic de détérioration de batterie servant à diagnostiquer l'état de détérioration de la batterie secondaire au lithium-ion, l'unité de diagnostic de détérioration de batterie diagnostiquant l'état de détérioration de la batterie secondaire au lithium-ion sur la base de la corrélation entre le potentiel de l'électrode positive et le potentiel de l'électrode négative qui sont détectés par l'unité de détection de potentiel d'électrodes négatives et positives, et de la corrélation entre les potentiels initiaux de l'électrode positive et de l'électrode négative.
PCT/JP2013/081226 2013-11-20 2013-11-20 Système et procédé pour batterie secondaire au lithium-ion permettant de diagnostiquer la détérioration d'une batterie secondaire au lithium-ion Ceased WO2015075785A1 (fr)

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Cited By (4)

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US20150276884A1 (en) * 2014-03-31 2015-10-01 Hitachi, Ltd. Lithium-ion secondary battery system and status diagnostic method of lithium-ion secondary battery
US20180038917A1 (en) * 2014-07-10 2018-02-08 Toyo Tire & Rubber Co., Ltd. Sealed secondary battery deterioration diagnosis method and deterioration diagnosis system
CN114839251A (zh) * 2022-03-18 2022-08-02 清华大学 缺陷识别方法、装置、电位传感器、电池、介质和产品
CN115079005A (zh) * 2021-03-12 2022-09-20 株式会社东芝 电池的诊断方法、电池的诊断装置、电池的诊断系统、电池搭载设备以及存储介质

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JP2011215083A (ja) * 2010-04-01 2011-10-27 Toyota Motor Corp 二次電池の正負電位関係取得装置、二次電池の制御装置、車両、二次電池の正負電位関係取得方法、及び、二次電池の制御方法
WO2013105139A1 (fr) * 2012-01-13 2013-07-18 トヨタ自動車株式会社 Procédé et dispositif de commande de batterie rechargeable

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Publication number Priority date Publication date Assignee Title
JP2011215083A (ja) * 2010-04-01 2011-10-27 Toyota Motor Corp 二次電池の正負電位関係取得装置、二次電池の制御装置、車両、二次電池の正負電位関係取得方法、及び、二次電池の制御方法
WO2013105139A1 (fr) * 2012-01-13 2013-07-18 トヨタ自動車株式会社 Procédé et dispositif de commande de batterie rechargeable

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20150276884A1 (en) * 2014-03-31 2015-10-01 Hitachi, Ltd. Lithium-ion secondary battery system and status diagnostic method of lithium-ion secondary battery
US20180038917A1 (en) * 2014-07-10 2018-02-08 Toyo Tire & Rubber Co., Ltd. Sealed secondary battery deterioration diagnosis method and deterioration diagnosis system
CN115079005A (zh) * 2021-03-12 2022-09-20 株式会社东芝 电池的诊断方法、电池的诊断装置、电池的诊断系统、电池搭载设备以及存储介质
CN114839251A (zh) * 2022-03-18 2022-08-02 清华大学 缺陷识别方法、装置、电位传感器、电池、介质和产品

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