WO2021184376A1 - Procédé pour améliorer les performances de cycle de batterie et dispositif électronique - Google Patents

Procédé pour améliorer les performances de cycle de batterie et dispositif électronique Download PDF

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WO2021184376A1
WO2021184376A1 PCT/CN2020/080489 CN2020080489W WO2021184376A1 WO 2021184376 A1 WO2021184376 A1 WO 2021184376A1 CN 2020080489 W CN2020080489 W CN 2020080489W WO 2021184376 A1 WO2021184376 A1 WO 2021184376A1
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Prior art keywords
charging
battery
stage
current
voltage
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PCT/CN2020/080489
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English (en)
Chinese (zh)
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刘奥
高潮
方占召
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宁德新能源科技有限公司
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Priority to PCT/CN2020/080489 priority Critical patent/WO2021184376A1/fr
Priority to CN202080008681.XA priority patent/CN113632290B/zh
Publication of WO2021184376A1 publication Critical patent/WO2021184376A1/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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/44—Methods for charging or discharging
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • 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

  • This application relates to the field of battery technology, and in particular to a method and electronic device for improving battery cycle performance.
  • the current charging method is usually a constant current and constant voltage charging method, that is, the battery is first charged to the charging limit voltage with a constant current, and then constant voltage charging is performed at the charging limit voltage.
  • the constant current and constant voltage charging method is used because of the polarization of the battery during the charging process. The greater the current, the more obvious the polarization.
  • the constant current is charged to the charging limit voltage, since there is a phenomenon that the polarized cell is not fully charged, it is necessary to continue constant voltage charging.
  • the voltage of the battery remains constant, and the current is gradually reduced to a very small cut-off current, thus completing the full charge.
  • the cathode potential is the highest at the end of the constant voltage charging process, and the maintenance time is very long, so it damages the battery cathode material and affects the thermal stability, and worsens the battery during the cycle.
  • the low-temperature discharge performance is the highest at the end of the constant voltage charging process, and the maintenance time is very long, so it damages the battery cathode material and affects the thermal stability, and worsens the battery during the cycle. The low-temperature discharge performance.
  • An embodiment of the present application provides a method for improving the cycle performance of a battery, which is applied to a battery, the battery includes a positive electrode film, the positive electrode film includes a positive electrode active material capable of inserting and extracting lithium ions, and the positive electrode
  • the active material includes lithium cobalt oxide primary particles and lithium cobalt oxide secondary particles composed of the lithium cobalt oxide primary particles, the average particle size of the lithium cobalt oxide primary particles is 0.1 ⁇ m-5 ⁇ m, and the lithium cobalt oxide secondary particles
  • the average particle size of the particles is 10 ⁇ m-25 ⁇ m
  • the method includes: in the first stage, charging the battery to the first stage voltage with the first stage current; in the second stage, charging the battery with the second stage current Charge to the second stage voltage, the second stage voltage is greater than the first stage voltage, and the second stage current is less than the first stage current.
  • the chemical formulas of the lithium cobalt oxide primary particles and the lithium cobalt oxide secondary particles are Li a Co 1-b M b O 2-b , wherein M is selected from Na, Mg, Al At least one of, Ti, Zr, Y, Ha, Ni, Mn, V, Cr, La and Ce, 0.99 ⁇ a ⁇ 1.01, 0 ⁇ b ⁇ 0.05.
  • the surfaces of the lithium cobalt oxide primary particles and the lithium cobalt oxide secondary particles are both provided with a coating layer, and the chemical formula of the coating layer is LiNO d , wherein N is selected from Al, At least one of Ti, Cr and Y, 2 ⁇ d ⁇ 3.
  • the weight ratio of the lithium cobalt oxide primary particles and the lithium cobalt oxide secondary particles is 5:95-50:50.
  • the second stage adopts a first charging method or a second charging method to charge the battery to the second stage voltage
  • the average value of the charging current of the jth charging substage is less than the charging current of the first phase, and the average value of the charging current of the j+1th charging substage is less than or equal to the jth charging current.
  • the charging current of the electronic phase is less than the charging current of the first phase.
  • the first stage adopts a third charging method to charge the battery to the first stage voltage
  • the third charging method adopts the first charging method or the second charging method
  • the number of charging sub-stages K between the two is the same; or when the third charging method adopts the second charging method In the charging mode, the number of charging sub-stages D between the two is the same.
  • the first stage voltage is equal to the charge limit voltage of the battery, and the second stage voltage is less than the oxidative decomposition voltage of the electrolyte in the battery.
  • the second stage voltage is less than or equal to the first stage voltage plus 500 millivolts.
  • the method further includes: in the third stage, performing constant voltage charging on the battery with the second stage voltage.
  • An embodiment of the present application also provides an electronic device, including a battery and a battery management module.
  • the battery includes a positive electrode film, the positive electrode film includes a positive electrode active material capable of inserting and extracting lithium ions, and the positive electrode active material Including lithium cobalt oxide primary particles and lithium cobalt oxide secondary particles composed of the lithium cobalt oxide primary particles, the average particle size of the lithium cobalt oxide primary particles is 0.1 ⁇ m-5 ⁇ m, and the lithium cobalt oxide secondary particles The average particle size is 10 ⁇ m-25 ⁇ m, and the battery management module is used to perform any of the methods described above.
  • the embodiment of the present application adjusts the weight ratio of lithium cobalt oxide primary particles and lithium cobalt oxide secondary particles in the positive electrode active material of the battery, and increases the charge limit voltage of the battery (that is, increases from the first stage voltage to the second stage voltage). ), etc., which can significantly reduce polarization and reduce the temperature rise of the battery cell. It can also shorten the time that the cathode of the battery is under high voltage, reduce the occurrence of side reactions, and further improve the cycle performance of the battery, and can significantly Improve low-temperature discharge performance during battery cycling.
  • Fig. 1 is a schematic diagram of an electronic device according to an embodiment of the present application.
  • Fig. 2 is a flowchart of a method for improving battery cycle performance according to an embodiment of the present application.
  • FIG. 3 is a first specific embodiment of the method for improving the cycle performance of the battery shown in FIG. 2.
  • FIG. 4 is a schematic diagram of the current and voltage changes with time during the charging process of the battery according to the first embodiment of the present application.
  • FIG. 5 is a schematic diagram of the current and voltage changes with time during the charging process of the battery according to the second embodiment of the present application.
  • Fig. 6 is a schematic diagram of the power and voltage changes with time in the first stage and the current and voltage changes with time in the second stage according to an embodiment of the present application.
  • FIG. 7 is a schematic diagram of the current and voltage changes with time during the charging process of the battery according to the third embodiment of the present application.
  • FIG. 8 is a schematic diagram of the current and voltage changes with time during the charging process of the battery according to the fourth embodiment of the present application.
  • FIG. 9 is a second specific embodiment of the method for improving the cycle performance of the battery shown in FIG. 2.
  • FIG. 10 is a third specific embodiment of the method for improving the cycle performance of the battery shown in FIG. 2.
  • FIG. 11 is a fourth specific embodiment of the method for improving the cycle performance of the battery shown in FIG. 2.
  • FIG. 1 is a schematic diagram of an electronic device according to an embodiment of the application.
  • the electronic device 1 includes a battery 10, a control unit 11 and a battery management module 12.
  • the battery 10, the control unit 11 and the battery management module 12 may be connected via a bus or directly.
  • the battery 10 includes at least one battery cell, and the battery 10 can be repeatedly charged in a rechargeable manner.
  • the battery 10 is mainly composed of a positive electrode film, a negative electrode film, a separator, an electrolyte, and a packaging bag.
  • the control unit 11 may control the battery management module 12 to execute the method for improving battery cycle performance.
  • the control unit 11 can be a microcontroller (Microcontroller, MCU), a processor (Processor), or an application-specific integrated circuit (ASIC), etc., and can control the battery management module 12 to execute The method for improving the cycle performance of the battery.
  • MCU microcontroller
  • processor processor
  • ASIC application-specific integrated circuit
  • FIG. 1 is only an example of the electronic device 1.
  • the electronic device 1 may also include more or fewer elements, or have different element configurations.
  • the electronic device 1 may be an electric motorcycle, an electric bicycle, an electric car, a mobile phone, a tablet computer, a digital assistant, a personal computer, or any other suitable rechargeable equipment.
  • the electronic device 1 may also include other components such as a wireless fidelity (Wireless Fidelity, WiFi) unit, a Bluetooth unit, a speaker, etc., which will not be repeated here.
  • a wireless fidelity (Wireless Fidelity, WiFi) unit Wireless Fidelity, WiFi
  • a Bluetooth unit Bluetooth unit
  • speaker etc., which will not be repeated here.
  • FIG. 2 is a flowchart of a method for improving battery cycle performance according to an embodiment of the present application.
  • the method for improving the cycle performance of a battery applied to a battery includes the following steps:
  • Step S21 In the first stage, the battery is charged to the first stage voltage with the first stage current.
  • Step S22 In the second stage, the battery is charged to the second stage voltage with the second stage current, the second stage voltage is greater than the first stage voltage, and the second stage current is smaller than the first stage voltage Current.
  • the positive electrode membrane of the battery includes a positive electrode active material capable of inserting and extracting lithium ions, and the positive electrode active material includes lithium cobalt oxide primary particles and lithium cobalt oxide secondary particles.
  • the average particle size of the lithium cobalt oxide primary particles is 0.1 ⁇ m-5 ⁇ m (small particles), and the average particle size of the lithium cobalt oxide secondary particles is 10 ⁇ m-25 ⁇ m (large particles).
  • the average particle size of the lithium cobalt oxide primary particles is 1 ⁇ m to 3 ⁇ m; the average particle size of the lithium cobalt oxide secondary particles is 15 ⁇ m to 20 ⁇ m.
  • the weight ratio of lithium cobalt oxide primary particles and lithium cobalt oxide secondary particles is 5:95 to 50:50. In another embodiment, the weight ratio is 15:85 to 35:65.
  • the chemical formula of the lithium cobalt oxide primary particles and the lithium cobalt oxide secondary particles is Li a Co 1-b M b O 2-b , wherein M is selected from Na, Mg, Al, Ti At least one of, Zr, Y, Ha, Ni, Mn, V, Cr, La and Ce, 0.99 ⁇ a ⁇ 1.01, 0 ⁇ b ⁇ 0.05.
  • both the lithium cobalt oxide primary particles and the lithium cobalt oxide secondary particles are provided with a coating layer, and the chemical formula of the coating layer is LiNO d , wherein N is selected from Al, Ti, At least one of Cr and Y, 2 ⁇ d ⁇ 3.
  • FIG. 3 is a first specific embodiment of the method for improving the cycle performance of the battery shown in FIG. 2.
  • Step S31 In the first stage, the battery is charged to the first stage voltage with the first stage current.
  • the current in the first stage is a constant current, that is, a constant charging current is used when charging is started in the prior art.
  • the current in the first stage may also be a current of varying magnitude.
  • the battery is charged with a constant voltage, and the charging current corresponding to the constant voltage (that is, the first The size of the phase current) will vary, as long as the battery can be charged to the first phase voltage through the first phase current.
  • the first stage voltage is equal to the charging limit voltage of the battery (which can be understood as a well-known charging limit voltage).
  • Step S32 In the second stage, the battery is charged to the second stage voltage with the second stage current, the second stage voltage is greater than the first stage voltage, and the second stage current is smaller than the first stage voltage Current; the second stage adopts the first charging method or the second charging method to charge the battery to the second stage voltage.
  • the battery includes a positive electrode film, the positive electrode film includes a positive electrode active material capable of inserting and extracting lithium ions, and the positive electrode active material includes lithium cobalt oxide primary particles and cobalt composed of the lithium cobalt oxide primary particles. Lithium oxide secondary particles, the average particle size of the lithium cobalt oxide primary particles is 0.1 ⁇ m-5 ⁇ m, and the average particle size of the lithium cobalt oxide secondary particles is 10 ⁇ m-25 ⁇ m.
  • the average particle size of the lithium cobalt oxide primary particles is 1 ⁇ m-3 ⁇ m; the average particle size of the lithium cobalt oxide secondary particles is 15 ⁇ m-20 ⁇ m.
  • the positive active material includes lithium cobalt oxide primary particles and lithium cobalt oxide secondary particles.
  • the weight ratio of lithium cobalt oxide primary particles and lithium cobalt oxide secondary particles is 5:95 to 50:50. In another embodiment, the weight ratio is 15:85 to 35:65.
  • the charging current in the (i+1)th charging sub-phase is less than or equal to the charging current in the i-th charging sub-phase.
  • the (i+1)th voltage is greater than or equal to the (i)th voltage.
  • the (i+1)th power is less than or equal to the (i)th power.
  • the average value of the charging current of the j+1th charging substage is less than or equal to the charging current of the jth charging substage, and when the third charging method adopts the second charging method, The average value of the charging current in the jth charging substage is smaller than the charging current in the first charging mode or the second charging mode.
  • the first stage voltage is equal to the charging limit voltage of the battery.
  • Lithium evolution potential can be obtained by testing in the following way.
  • the battery in this embodiment another three-electrode battery with the same specifications is produced.
  • the three-electrode battery has one more electrode, that is, it contains three electrodes, which are anodes. , Cathode and reference electrode.
  • the material of the reference electrode is lithium, and the three-electrode battery is used for testing to obtain the lithium evolution potential of the anode of the battery of this embodiment.
  • the specific test method for the lithium evolution potential of the anode is as follows: make a plurality of three-electrode batteries, and charge and discharge the three-electrode battery with charging currents of different magnifications (for example, 1C, 2C, 3C), and cycle multiple times ( For example, 10 times), and detect the potential difference between the anode and the reference electrode during the charge and discharge process. Then, the three-electrode battery was fully charged and disassembled, and the anodes of the three-electrode batteries charged with different rates were observed whether lithium evolution occurred (that is, whether lithium metal was deposited on the surface of the anode).
  • magnifications for example, 1C, 2C, 3C
  • cycle multiple times For example, 10 times
  • the minimum potential difference between the anode and the reference electrode during the charge and discharge process at the rate is used as the anode lithium evolution potential.
  • the charging current of lithium batteries is generally referred to by the rate C, which is the value corresponding to the capacity of the lithium battery.
  • Lithium battery capacity is generally expressed in Ah and mAh. For example, when the battery capacity is 1200mAh, the corresponding 1C is 1200mA, and 0.2C is equal to 240mA.
  • the anode does not undergo lithium evolution when using 1C and 2C charging and discharging, and the anode occurs when using 3C charging and discharging.
  • the minimum value of the potential difference between the anode and the reference electrode at the 2C rate is the anode lithium evolution potential.
  • the lithium evolution potential of the cathode can also be tested in a similar manner, which will not be repeated here.
  • the anode potential and the cathode potential of the battery can be further understood through the above anode lithium evolution potential test process as follows: the anode potential is the potential difference between the anode and the reference electrode, that is, the anode versus lithium potential, and the cathode potential is the cathode and the reference electrode. The potential difference than the electrode, that is, the potential of the cathode to lithium.
  • the second stage voltage is less than the oxidative decomposition voltage of the electrolyte in the battery.
  • the oxidative decomposition voltage of the electrolyte in the battery can be understood as follows: when the potential of the battery exceeds a certain potential threshold, the solvent molecules, additive molecules, and even impurity molecules in the electrolyte will irreversibly reduce at the interface between the electrode and the electrolyte. Or oxidative decomposition reaction, this phenomenon is called electrolyte decomposition.
  • the potential threshold is the reduction decomposition voltage and the oxidation decomposition voltage of the electrolyte in the battery.
  • the second stage voltage is also less than or equal to the first stage voltage plus 500 millivolts.
  • the cut-off condition for charging the battery may be A cut-off voltage, a cut-off current, or a cut-off capacity. More specifically, in the K-th charging sub-phase or the D-th charging sub-phase, when the charging current of the battery is equal to the cut-off current, the reached charging voltage (that is, the voltage difference between the positive electrode and the negative electrode) is equal to that of the battery. When the cut-off voltage or the electric capacity of the battery is equal to the cut-off capacity, the battery is stopped charging, that is, the charging is cut off.
  • the cut-off current, the cut-off voltage, and the cut-off capacity can be obtained by using the aforementioned three-electrode battery test method and observing that the cathode of the three-electrode battery does not undergo excessive delithiation.
  • the electric capacity of the battery is equivalent to that of the conventional charging method in the prior art, and to ensure that the cathode of the battery does not undergo excessive delithiation.
  • the first stage current, the first stage voltage, the i-th current of the i-th charging substage of the first stage, the One of the i-th voltage, and the i-th power, one of the i-th current, the i-th voltage, and the i-th power in the i-th charging substage of the second stage The value of the second stage voltage and the cut-off condition may be stored in the battery management module in advance.
  • the battery In the first stage, from time 0 to t1, the battery is charged to voltage U1 with a constant current I1; from time t1 to t2, the battery is charged to voltage U2 with a constant current I2; from time t(i-2) to During t(i-1), charge with constant current I(i-1) to voltage U(i-1); during time ti-1 to ti, charge with constant current Ii to voltage Ui; at time t(K -1) Between tK, charge with constant current Icl to voltage Ucl. Between time t2 and t(i-2), and between time ti and t(K-1), similar charging is performed, but it is omitted in the figure and not shown.
  • the battery is charged with a constant current I1' to the voltage U1'; from time t2' to t3', the battery is charged with a constant voltage U1', the corresponding charging current for this period of time Decrease from I1' to current I2'; from time t3' to t4', charge the battery with a constant current I2' to voltage U2'; from time t4' to t5', charge the battery with a constant voltage U2'; Between time t(i-1)' and ti', charge the battery with a constant current Ii' to the voltage Ui'; between time ti' and t(i+1)', charge the battery with a constant voltage Ui', this period The charging current corresponding to time drops from I1' to the current I(i+1)'; between time t(K-2)' and t(K-1)', the charging current is charged to the voltage Um with a constant current Im; at
  • the tK and t1' are the same time.
  • the battery is charged with a constant charging current, and I1 ⁇ I2 ⁇ ... ⁇ Icl, U1 ⁇ U2 ⁇ ... ⁇ Ucl;
  • Each of the K charging sub-phases of the two stages charges the battery alternately with a constant charging current and a constant voltage, Icl ⁇ I1' ⁇ I2' ⁇ ... ⁇ Im', Ucl ⁇ U1' ⁇ U2' ⁇ ... ⁇ Um.
  • the battery In the first stage, between time 0 and t1, the battery is charged with a constant voltage U1 until the current is I1; between time t1 and t2, the battery is charged with a constant voltage U2 until the current is I2; at time t(i-1 From) to ti, charge with a constant voltage Ui until the current is Ii; from time t(K-1) to tK, charge with a constant voltage Ucl until the current is Icl. Similar charging is performed between time t2 and t(i-1) and between time ti and t(K-1), but is omitted in the figure and not shown.
  • the battery is charged with a constant current I1' to the voltage U1'; from time t2' to t3', the battery is charged with a constant voltage U1', the corresponding charging current for this period of time Decrease from I1' to current I2'; from time t3' to t4', charge the battery with a constant current I2' to voltage U2'; from time t4' to t5', charge the battery with a constant voltage U2'; Between time t(i-1)' and ti', charge the battery with a constant current Ii' to the voltage Ui'; between time ti' and t(i+1)', charge the battery with a constant voltage Ui', this period The charging current corresponding to time drops from Ii' to the current I(i+1)'; between time t(K-2)' and t(K-1)', the charging current is charged to the voltage Um with a constant current Im; at
  • the tK and t1' are the same time.
  • the battery In each of the K charging sub-phases of the first stage, the battery is charged with a constant charging voltage, and U1 ⁇ U2 ⁇ ... ⁇ Ucl, I1 ⁇ I2 ⁇ ... ⁇ Icl.
  • the battery In each of the K charging sub-stages of the second stage, the battery is charged alternately with a constant charging current and a constant charging voltage, and Ucl ⁇ U1' ⁇ U2' ⁇ ... ⁇ Um, Icl ⁇ I1' ⁇ I2' ⁇ ... ⁇ Im'.
  • the first charging method is used to charge the battery in the first stage, and the first charging method includes K charging sub-stages in sequence, and the K charging sub-stages are respectively defined as the i-th charger.
  • the battery In the first stage, between time 0 and t1, the battery is charged with constant power P1 until the voltage is U1; between time t1 and t2, the battery is charged with constant power P2 to voltage U2; at time t(i-2) To t(i-1), charge to voltage U(i-1) with constant power P(i-1); from time t(i-1) to ti, charge to voltage Ui with constant power Pi; Between time t(K-1) and tK, the battery is charged to the voltage Ucl with a constant power Pcl. Between time t2 and t(i-2), and between time ti and t(K-1), similar charging is performed, but it is omitted in the figure and not shown.
  • the battery is charged with a constant current I1' to the voltage U1'; from time t2' to t3', the battery is charged with a constant voltage U1', the corresponding charging current for this period of time Decrease from I1' to current I2'; from time t3' to t4', charge the battery with a constant current I2' to voltage U2'; from time t4' to t5', charge the battery with a constant voltage U2'; Between time t(i-1)' and ti', charge the battery with a constant current Ii' to the voltage Ui'; between time ti' and t(i+1)', charge the battery with a constant voltage Ui', this period The charging current corresponding to time drops from I1' to the current I(i+1)'; between time t(K-2)' and t(K-1)', the charging current is charged to the voltage Um with a constant current Im; at
  • the battery in each of the K charging sub-stages of the first stage, the battery is charged with a constant power, and P1 ⁇ P2 ⁇ ... ⁇ Pcl, U1 ⁇ U2 ⁇ ... ⁇ Ucl.
  • the battery is charged alternately with a constant charging current and a constant charging voltage, and Ucl ⁇ U1' ⁇ U2' ⁇ ... ⁇ Um, Icl ⁇ I1' ⁇ I2' ⁇ ... ⁇ Im'.
  • the battery is charged with a constant current I1 to the voltage U1; between time t1 and t2, the battery is charged with a constant voltage U1, and the corresponding charging current during this period is reduced from I1 To the current I2; from time t2 to t3, the battery is charged with a constant current I2 to the voltage U2; from time t3 to t4, the battery is charged with a constant voltage U2, the corresponding charging current for this period of time drops from I2 to the current I3; From time t(i-2) to t(i-1), charge the battery with a constant current Ii to the voltage Ui; from time t(i-1) to ti, charge the battery with a constant voltage Ui; at time t(K From -2) to t(K-1), charge the battery with a constant current Icl to the voltage Ucl; from time t(K-1) to tK, charge the battery with a constant voltage Ucl, the corresponding charging
  • the battery is charged with a constant current I1' to the voltage U1'; from time t2' to t3', the battery is charged with a constant voltage U1', the corresponding charging current for this period of time Decrease from I1' to current I2'; from time t3' to t4', charge the battery with a constant current I2' to voltage U2'; from time t4' to t5', charge the battery with a constant voltage U2'; Between time t(i-1)' and ti', charge the battery with a constant current Ii' to the voltage Ui'; between time ti' and t(i+1)', charge the battery with a constant voltage Ui', this period The charging current corresponding to time drops from I1' to the current I(i+1)'; between time t(K-2)' and t(K-1)', the charging current is charged to the voltage Um with a constant current Im; at
  • a constant charging current and a constant charging voltage alternately charge the battery
  • I1 ⁇ I2 ⁇ ... ⁇ Icl, U1 ⁇ U2 ⁇ ... ⁇ Ucl In each of the K charging sub-phases of the second stage, the battery is also charged alternately with a constant charging current and a constant charging voltage, and I1' ⁇ I2' ⁇ ... ⁇ Im', U1' ⁇ U2' ⁇ ... ⁇ Um, and Icl ⁇ I1', Ucl ⁇ U1'.
  • the battery In one of the j-th pre-charge sub-stage and the j-th post-charge sub-stage, the battery is not charged or is charged or discharged with a j-th pre-charger current for Tj1. In the other of the j-th pre-charging sub-stage and the j-th post-charging sub-stage, the battery is charged with a j-th post-charge sub-current for a duration of Tj2.
  • the absolute value of the j-th front charger current is smaller than the absolute value of the j-th rear charger current.
  • the battery is charged by pulse charging or pulse charging and discharging, and the average value of the charging current of the j+1 charging substage is less than or It is equal to the charging current of the j-th charging sub-stage, for example, (the first front charger current*T11+the first rear charger current*T12)/(T11+T12) is greater than or equal to (the second front charger current*T21+ The second rear charger current*T22)/(T21+T22), (the second front charger current*T21+the second rear charger current*T22)/(T21+T22) is greater than or equal to (the third front charger current *T31+3rd post-charger current*T32)/(T31+T32) and so on.
  • the sum of the duration of each Tj1 and the duration of Tj2 is the charging period or the charging and discharging period of the pulse charging or the pulse charging and discharging in the jth charging sub-phase.
  • the j-th pre-charger current is used to charge or discharge for Tj1 time
  • the j-th post-charger In the stage charging is performed with the j-th post-charger current for a duration of Tj2.
  • the charge or discharge current of the front charger is Tj1.
  • the charging sub-phase before the jth charge is not charged or is left to stand that is, the charging current is 0 at this time
  • the charging sub-phase after the jth charge After the jth sub-current is charged or discharged for Tj2 duration.
  • time t1 and t1000 that is, in each charging sub-stage from the first charging sub-stage to the 1000th charging sub-stage of the first stage, the current I2 is first applied to The battery is charged, and then the battery is charged with a current I3. Between time tx and t1000, similar charging is performed, but it is omitted and not shown in the figure.
  • the battery in the D charging sub-phases of the first phase, the battery is charged in three different pulse charging or pulse charging and discharging methods.
  • the charging period or the charging and discharging period of different pulse charging or pulse charging and discharging may also be different.
  • the battery is charged with a constant current I1' to the voltage U1'; from time t2' to t3', the battery is charged with a constant voltage U1', the corresponding charging current for this period of time Decrease from I1' to current I2'; from time t3' to t4', charge the battery with a constant current I2' to the voltage U2'; from time t4' to t5', charge the battery with a constant voltage U2'; Between time ti' and t(i+1)', charge with constant current Ii' to voltage Ui'; between time t(i+1)' and t(i+2)', use constant voltage Ui' to When charging the battery, the charging current corresponding to this period of time drops from I1' to the current I(i+1)'; during the time t(D-2)' to t(D-1)', the constant current Im is charged to the voltage Um; between time t(
  • the method for improving battery cycle performance adjusts the weight ratio of lithium cobalt oxide primary particles and lithium cobalt oxide secondary particles in the positive electrode active material of the battery, and increases the charge limit voltage of the battery (that is, from The combination of increasing the voltage in the first stage to the voltage in the second stage, etc., can significantly reduce the polarization and reduce the temperature rise of the battery cell. It can also shorten the time that the battery’s cathode is under high voltage and reduce the occurrence of side reactions. It can further improve the cycle performance of the battery, and can significantly improve the low-temperature discharge performance of the battery during the cycle.
  • the battery system used in the comparative examples and examples described below uses lithium cobalt oxide as the cathode, graphite as the anode, plus a diaphragm, electrolyte and packaging shell, through mixing, coating, assembling, forming and aging, etc. Craft made.
  • the cathode is composed of 96.7% LiCoO 2 (as the cathode active material) plus 1.7% polyvinylidene fluoride (PVDF, as the binder) and 1.6% conductive carbon black (SUPER-P, as the conductive agent).
  • the anode is composed of 98.
  • the comparative example and the embodiment used different new charging methods to charge the battery, and used lithium cobalt oxide positive active materials with different weight ratios to test the capacity retention rate, temperature rise, impedance growth rate and after cycling of the battery after cycling charge and discharge.
  • Low-temperature discharge performance, specific schemes and performance summary are shown in Table 1.
  • the existing charging methods in Comparative Example 1 and Comparative Example 3 are the constant current and constant voltage charging methods in the prior art.
  • the specific process of the existing charging method is:
  • the ambient temperature is 45°C:
  • Step 1 Charge the battery to 4.4V with 0.7C constant current
  • Step 2 Charge the battery to 0.05C with a constant voltage of 4.4V;
  • Step 3 Let the battery stand for 5 minutes
  • Step 4 Discharge the battery to 3.0V at a constant current of 0.5C;
  • Step 5 Let the battery stand for 5 minutes
  • Step 6 Cycle the above steps 1 to 5 500 times.
  • C is a value corresponding to the capacity of the lithium ion battery.
  • Lithium-ion battery capacity is generally expressed in Ah and mAh.
  • the corresponding 1C is 1200mA
  • 0.2C is equal to 240mA.
  • Comparative Example 2 and Examples 1-16 adopt the new charging method 1 in this application, and the specific process is as follows:
  • the ambient temperature is 45°C;
  • Step 1 Charge the battery to 4.4V with 0.7C constant current
  • Step 2 Charge the battery to 4.45V with a constant current of 0.5C;
  • Step 3 Charge the battery to 4.54V with 0.4C constant current
  • Step 4 Let the battery stand for 5 minutes
  • Step 5 Discharge the battery to 3.0V at a constant current of 0.5C;
  • Step 6 Let the battery stand for 5 minutes
  • Step 7 Cycle the above steps 1 to 6 for 500 times.
  • Embodiment 17 adopts the new charging method 2 in this application, and the specific process is as follows:
  • the ambient temperature is 45°C;
  • Step 1 Charge the battery to 4.4V with 0.7C constant current
  • Step 2 Charge the battery to 0.4C with a constant voltage of 4.35V;
  • Step 3 Charge the battery to 0.13C with a constant voltage of 4.45V;
  • Step 4 Let the battery stand for 5 minutes
  • Step 5 Discharge the battery to 3.0V at a constant current of 0.5C;
  • Step 6 Let the battery stand for 5 minutes
  • Step 7 Cycle the above steps 1 to 6 for 500 times.
  • Embodiment 18 adopts the new charging method 3 in this application, and the specific process is as follows: the ambient temperature is 45°C;
  • Step 1 Charge the battery to 4.4V with 0.7C (2.1A) constant current
  • Step 2 Charge the battery to 4.45V with a constant power of 7W;
  • Step 3 Charge the battery to 4.55V with a constant power of 5.5W;
  • Step 4 Let the battery stand for 5 minutes
  • Step 5 Discharge the battery to 3.0V at a constant current of 0.5C;
  • Step 6 Let the battery stand for 5 minutes
  • Step 7 Cycle the above steps 1 to 6 for 500 times.
  • Embodiment 19 adopts the new charging method 4 in this application, and the specific process is as follows:
  • the ambient temperature is 45°C;
  • Step 1 Charge the battery to 4.4V with 0.7C constant current
  • Step 2 Charge the battery to 0.5C with a constant voltage of 4.4V;
  • Step 3 Charge the battery to 4.45V at a constant current of 0.5C;
  • Step 4 Charge the battery to 0.3C with a constant voltage of 4.45V;
  • Step 5 Let the battery stand for 5 minutes
  • Step 6 Discharge the battery to 3.0V at a constant current of 0.5C;
  • Step 7 Let the battery stand for 5 minutes
  • Step 8 Circulate 500 times from step 1 to step 7 above.
  • Embodiment 20 adopts the new charging method 5 in this application, and the specific charging process is as follows:
  • the ambient temperature is 45°C;
  • Step 1 Charge the battery to 4.4V with 0.7C constant current
  • Step 2 Leave the battery for 2.9 seconds
  • Step 3 Charge the battery with a constant current of 0.7C for 7.1 seconds, and judge whether the battery voltage is greater than or equal to 4.45V. When the battery voltage is greater than or equal to 4.45V, skip to step five;
  • Step 4 Cycle Step 2 to Step 3 100000 times
  • Step 5 Discharge the battery for 1 second at a constant current of 0.05C;
  • Step 6 Charge the battery with a constant current of 0.41C for 9 seconds, and judge whether the battery voltage is greater than or equal to 4.54V. When the battery voltage is greater than or equal to 4.54V, skip to step 8;
  • Step 7 Let the battery stand for 5 minutes
  • Step 8 Discharge the battery to 3.0V at a constant current of 0.5C;
  • Step 9 Let the battery stand for 5 minutes
  • Step 10 Cycle the above steps 1 to 9 500 times.
  • the calculation method of the capacity retention rate after 500 cycles of charge and discharge at 45°C in Table 1 is: when the ambient temperature is 45°C, the batteries of the comparative example and the examples use the corresponding charging process cycle For 500 cycles, the discharge capacity after 500 cycles of the battery is divided by the discharge capacity at the first cycle.
  • the low-temperature discharge performance of the battery in Table 1 describes the low-temperature discharge capacity retention rate of the battery.
  • the low-temperature discharge capacity retention rate was measured by the following method: before the cycle test, the battery was discharged at a capacity of 0.2C to 3.0V under an environment of 25°C (comparative example and example) as the reference capacity; after the discharge was completed, the comparative example was used
  • the charging process corresponding to the embodiment has 500 cycles of charging and discharging. After 500 cycles, the battery is transferred to an environment of -10°C and discharged at 0.2C to 3.0V.
  • the discharge capacity at this step is divided by the reference capacity to obtain the low-temperature discharge capacity retention rate.
  • test methods please refer to the following test methods:
  • the ambient temperature is 25°C;
  • Step 1 Charge the battery to 4.4V with 0.2C constant current
  • Step 2 Charge the battery to 0.05C with a constant voltage of 4.4V;
  • Step 3 Discharge the battery to 3.0V at a constant current of 0.2C; (calculate the discharge capacity of this step, and use this step as the benchmark);
  • Step 4 Let the battery stand for 5 minutes
  • Step 5 Use the test procedure of the comparative example and the embodiment to complete 500 cycles and remove the battery cell, transfer to -10°C and let it stand for 10 minutes, and then install the cell into the battery;
  • Step 6 Charge the battery to 4.4V with 0.2C constant current
  • Step 7 Charge the battery to 0.05C with a constant voltage of 4.4V;
  • Step 8 Discharge the battery to 3.0V with a constant current of 0.2C; (calculate the discharge capacity of this step, and divide the discharge capacity of this step by the discharge capacity calculated in step 3 is the low-temperature discharge capacity retention rate);
  • Step 9 Let the battery stand for 5 minutes
  • the calculation method of the impedance growth rate after 500 cycles of charge-discharge cycles at 45°C in Table 1 is: before the cycle test, the Autolab electrochemical workstation is used, and the battery impedance test is carried out with a 10mV disturbance voltage in the range of 1MHz-0.1MHz to obtain the cycle test. After charging and discharging the battery for 500 cycles using the charging method in Comparative Example 1-3 and Example 1-20, the impedance of the battery after the 500-cycle cycle test was tested using the same test method, and then passed the following The formula calculates the impedance growth rate.
  • Impedance growth rate impedance before cycle test/impedance after 500 cycles test -1.
  • Examples 1-20 and Comparative Example 2 and Comparative Example 3 that by adjusting the weight ratio of lithium cobalt oxide primary particles and lithium cobalt oxide secondary particles in the positive electrode active material of the battery and using the charging method of the application (such as New charging method 1, new charging method 2, new charging method 3, etc.), can significantly reduce the battery impedance growth rate and the temperature rise of the battery cell, improve the battery cycle capacity retention rate and low-temperature discharge performance after cycling. Especially after 500 cycles of charge and discharge at 45°C, the low-temperature discharge performance of the battery is improved by about 20%.
  • the charging method of the application such as New charging method 1, new charging method 2, new charging method 3, etc.
  • the charging method of the present application can significantly shorten the time that the cathode is under high voltage, and by increasing the content of lithium cobalt oxide primary particles, the temperature rise caused by excessive charging speed can be reduced. Therefore, the damage to the cathode of the battery can be significantly reduced during the entire cycle, and the side reactions can be reduced at the same time, so that the low-temperature discharge performance of the battery after the cycle can be significantly improved.
  • this application adjusts the weight ratio of the lithium cobalt oxide primary particles and the lithium cobalt oxide secondary particles in the positive electrode active material of the battery, and increases the charge limit voltage of the battery (as in Example 1, the charging of Comparative Examples 1 and 3)
  • the combination of limiting the voltage from 4.4V to 4.45V, etc.) can significantly reduce polarization and reduce the temperature rise of the battery cell. It can also shorten the time that the battery’s cathode is under high voltage and reduce the occurrence of side reactions. Improve the cycle performance of the battery, and can significantly improve the low-temperature discharge performance of the battery during the cycle.
  • FIG. 9 is a second specific embodiment of the method for improving battery cycle performance shown in FIG. 2.
  • the second specific embodiment is similar to the first specific embodiment, and the second specific embodiment also includes step S91 and step S92.
  • step S91 which is specifically as follows:
  • Step S91 In the first stage, the battery is charged to the first stage voltage with the first stage current.
  • a third charging method is used to charge the battery to the first stage voltage, and the third charging method is the first charging method or the second charging method.
  • the first charging method and the second charging method are the same as the first charging method and the second charging method in the first specific embodiment, and will not be repeated here.
  • the number of charging sub-stages K between the two may be the same, that is, the charging sub-stages included in the first charging method adopted in the first stage
  • the number may be the same as the number of charging sub-stages included in the first charging method adopted in the second stage; or when the third charging method adopts the second charging method, the charging between the two
  • the number D of electronic stages may be the same, that is, the number of charging sub-stages included in the second charging method adopted in the first stage and the charging sub-stages included in the second charging method adopted in the second stage The number can be the same.
  • the number of charging sub-stages K between the two may be different, that is, the charging sub-stages included in the first charging method adopted in the first stage
  • the number may be different from the number of charging sub-stages included in the first charging method used in the second stage; or when the third charging method uses the second charging method, the charge between the two
  • the number D of electronic stages may be different, that is, the number of charging sub-stages included in the second charging method adopted in the first stage and the number of charging sub-stages included in the second charging method adopted in the second stage The number can be different.
  • FIG. 10 is a third specific embodiment of the method for improving the cycle performance of the battery shown in FIG. 2.
  • the third specific embodiment is similar to the first specific embodiment, and the third specific embodiment also includes step S101 and step S102.
  • the difference lies in step S101 and step S102, which are specifically as follows:
  • Step S101 In the first stage, the battery is charged to the first stage voltage with the first stage current.
  • a third charging method is used to charge the battery to the first stage voltage, and the third charging method is the first charging method or the second charging method.
  • the first charging method and the second charging method are the same as the first charging method and the second charging method in the first specific embodiment, and will not be repeated here.
  • Step S102 In the second stage, the battery is charged to the second stage voltage with the second stage current, the second stage voltage is greater than the first stage voltage, and the second stage current is smaller than the first stage voltage Current; the second stage adopts the first charging method or the second charging method to charge the battery to the second stage voltage;
  • the battery includes a positive electrode film
  • the positive electrode film includes a positive electrode active material capable of inserting and extracting lithium ions
  • the positive electrode active material includes lithium cobalt oxide primary particles and cobalt composed of the lithium cobalt oxide primary particles.
  • Lithium oxide secondary particles, the average particle size of the lithium cobalt oxide primary particles is 0.1 ⁇ m-5 ⁇ m, and the average particle size of the lithium cobalt oxide secondary particles is 10 ⁇ m-25 ⁇ m.
  • the second stage current is a constant current, that is, an existing charging current that uses constant current charging when charging is started.
  • the current in the second stage may also be a current of varying magnitude.
  • the battery is charged with a constant voltage, and the charging current corresponding to the constant voltage (that is, the second The size of the phase current) will vary, as long as the battery can be charged to the second phase voltage through the second phase current.
  • FIG. 11 is a fourth specific embodiment of the method for improving battery cycle performance shown in FIG. 2.
  • the fourth specific embodiment is similar to the first specific embodiment, and the fourth specific embodiment also includes step S111 and step S112. The difference is that the fourth specific embodiment further includes step S113, which is specifically as follows:
  • Step S113 In the third stage, charge the battery at a constant voltage with the second stage voltage.
  • the battery in the third stage, is charged at a constant voltage with the second stage voltage until the battery is fully charged.
  • the second specific embodiment can be improved with reference to the fourth embodiment, and step S113 is added: in the third stage, the battery is charged at a constant voltage with the second stage voltage.
  • the third specific embodiment can be improved with reference to the fourth embodiment, and step S113 is added: In the third stage, the battery is charged at a constant voltage with the second stage voltage.

Abstract

La présente demande concerne un procédé pour améliorer les performances d'un cycle de batterie, appliqué à une batterie. La batterie comprend une membrane d'électrode positive ; la membrane d'électrode positive comprend un matériau actif positif capable d'insérer et d'extraire des ions lithium ; le matériau actif positif comprend des particules primaires de cobaltate de lithium et des particules secondaires de cobaltate de lithium composées des particules primaires de cobaltate de lithium ; la taille moyenne de particule des particules primaires de cobaltate de lithium est de 0,1 à 5 µm, et la taille moyenne de particule des particules secondaires de cobaltate de lithium est de 10 à 25 µm. Le procédé comprend les étapes suivantes consistant à : dans un premier temps, charger la batterie avec un courant de première phase jusqu'à une tension de première phase ; et dans un second temps, charger la batterie avec un courant de seconde phase jusqu'à une tension de seconde phase, la tension de seconde phase étant supérieure à la tension de première phase, et le courant de seconde phase étant inférieur au courant de première phase. La présente demande concerne également un dispositif électronique. Selon le procédé, les performances de décharge à basse température dans le processus de cycle de batterie peuvent être remarquablement améliorées.
PCT/CN2020/080489 2020-03-20 2020-03-20 Procédé pour améliorer les performances de cycle de batterie et dispositif électronique WO2021184376A1 (fr)

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