WO2022198584A1 - Procédé de charge, appareil de charge et dispositif de charge - Google Patents

Procédé de charge, appareil de charge et dispositif de charge Download PDF

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Publication number
WO2022198584A1
WO2022198584A1 PCT/CN2021/083056 CN2021083056W WO2022198584A1 WO 2022198584 A1 WO2022198584 A1 WO 2022198584A1 CN 2021083056 W CN2021083056 W CN 2021083056W WO 2022198584 A1 WO2022198584 A1 WO 2022198584A1
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Prior art keywords
charging
current
negative
constant current
constant
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PCT/CN2021/083056
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English (en)
Chinese (zh)
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魏红梅
陈茂华
胡乔舒
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宁德新能源科技有限公司
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Priority to PCT/CN2021/083056 priority Critical patent/WO2022198584A1/fr
Priority to CN202180004986.8A priority patent/CN114531928B/zh
Publication of WO2022198584A1 publication Critical patent/WO2022198584A1/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
    • H01M10/446—Initial charging measures
    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02J—CIRCUIT ARRANGEMENTS OR SYSTEMS FOR SUPPLYING OR DISTRIBUTING ELECTRIC POWER; SYSTEMS FOR STORING ELECTRIC ENERGY
    • H02J7/00—Circuit arrangements for charging or depolarising batteries or for supplying loads from batteries
    • H02J7/0047—Circuit arrangements for charging or depolarising batteries or for supplying loads from batteries with monitoring or indicating devices or circuits
    • H02J7/0048—Detection of remaining charge capacity or state of charge [SOC]
    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02J—CIRCUIT ARRANGEMENTS OR SYSTEMS FOR SUPPLYING OR DISTRIBUTING ELECTRIC POWER; SYSTEMS FOR STORING ELECTRIC ENERGY
    • H02J7/00—Circuit arrangements for charging or depolarising batteries or for supplying loads from batteries
    • H02J7/007—Regulation of charging or discharging current or voltage
    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02J—CIRCUIT ARRANGEMENTS OR SYSTEMS FOR SUPPLYING OR DISTRIBUTING ELECTRIC POWER; SYSTEMS FOR STORING ELECTRIC ENERGY
    • H02J7/00—Circuit arrangements for charging or depolarising batteries or for supplying loads from batteries
    • H02J7/007—Regulation of charging or discharging current or voltage
    • H02J7/00712—Regulation of charging or discharging current or voltage the cycle being controlled or terminated in response to electric parameters
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present application relates to the field of energy storage, and in particular, to a charging method, a charging device and a charging device.
  • Lithium metal is the metal with the smallest relative atomic mass (6.94) and the lowest standard electrode potential (-3.045V) among all metal elements, and its theoretical gram capacity can reach 3860mAh/g. Therefore, using lithium metal as the negative electrode of the battery, with some high energy density positive electrode materials, can greatly improve the energy density of the battery and the working voltage of the battery.
  • lithium metal as a negative electrode material is truly commercialized, there are some problems that must be solved: 1) Li metal itself is highly reactive, especially the freshly formed lithium metal, which is very easy to electrolyze with existing small organic molecules.
  • the thickness of the negative electrode plate With the charging-discharging of the lithium metal negative electrode, the thickness of the negative electrode plate will undergo a violent expansion-shrinkage.
  • the thickness of the expansion and contraction is related to the amount of active material per unit area of the cathode and the gram capacity of the active material, and is also related to the deposition of lithium.
  • the density and the volume of the side reaction products are related.
  • the thickness change of the single-sided lithium metal anode from full charge to full discharge will reach 8 ⁇ m to 100 ⁇ m. This will cause the interface between the negative pole piece and the less flexible inorganic protective coating to peel off and lose the protective effect.
  • the charging rate is low.
  • the purpose of this application is to improve the cycle performance of lithium metal batteries by over-optimizing the charging process.
  • the present application provides a charging method, a charging device and a charging apparatus for a rechargeable device.
  • the present application provides a charging method for a rechargeable device, the charging method including a constant current charging stage and a constant voltage charging stage, wherein in the constant current charging stage, the constant current charging is carried out to 10% to 90% Perform at least one rest and/or at least one negative charge at the SOC, wherein the time for each rest is T 1 , T 1 ⁇ 30s, and the time for each negative charge is T 2 , T 2 ⁇ 10s.
  • the charging method includes the following steps:
  • the rechargeable device is charged with a first constant current until 10% to 90% SOC;
  • the anode of the rechargeable device contains lithium metal or an alloy of lithium metal.
  • 1min ⁇ T1 ⁇ 4min and 30s ⁇ T2 ⁇ 4min .
  • the number of times of standing is 1 to 10 times
  • the number of times of negative charging is 1 to 5 times.
  • the charging capacity of the current I + of the constant current charging is Q +
  • the charging capacity of the current I - of the negative charging is Q ⁇ , where Q + >Q ⁇ .
  • each negative charge capacity Q- satisfies : 1%Q ⁇ Q- ⁇ 10%Q, preferably 2%Q ⁇ Q- ⁇ 5%Q, where Q is the sum of Q + and Q- Difference.
  • the negative charging current I ⁇ and the constant current charging current I + satisfy: 3 ⁇ I ⁇ /I + ⁇ 20, preferably 3 ⁇ I ⁇ /I + ⁇ 6.
  • the current I + of the constant current charging satisfies: 0.1C ⁇ I + ⁇ 0.5C.
  • the negative charging has any one of the following characteristics A) to C): A) the current I- of the negative charging remains unchanged; B) the current I- of the negative charging is The first change slope increases, and then decreases with the second change slope; C) the negative charging current I- increases with the first change slope, maintains for a period of time, and then decreases with the second change slope.
  • the first change slope k1 satisfies: 0.0167C/s ⁇ k1 ⁇ 0.2C/s.
  • the second change slope k2 satisfies: 0.0167C/s ⁇ k2 ⁇ 0.2C/s.
  • a first variable current charging is further included between steps (1) and (2).
  • the first forward current I 1 decreases with a third change slope.
  • the third change slope k3 satisfies: 0.0167C/s ⁇ k3 ⁇ 0.2C/s.
  • a second variable current charging is further included between steps (2) and (3).
  • the second forward current I 2 increases at a fourth change slope.
  • the fourth change slope k4 satisfies: 0.0167C/s ⁇ k4 ⁇ 0.2C/s.
  • the present application provides a charging device, the charging device comprising: a constant current charging module; a stationary module and/or a negative charging module for performing constant current charging to 10% to 90% SOC At least one standstill and/or at least one negative charge, wherein the time for each stand is T 1 , T 1 ⁇ 30s, and the time for each negative charge is T 2 , T 2 ⁇ 10s; constant voltage charging module , used for constant voltage charging of rechargeable devices after constant current charging.
  • the present application provides a charging device comprising a memory and a processor, where the memory is used for storing executable program codes, and the processor is used for reading the executable program codes stored in the memory to execute the charging method described in the first aspect of the present application.
  • FIG. 1 is a current trend change diagram of a conventional charging method in the prior art.
  • FIG. 2 is a schematic diagram of current trend changes of charging methods according to some embodiments of the present application.
  • FIG. 3 is a schematic diagram of current trend changes of charging methods according to some embodiments of the present application.
  • FIG. 4 is a schematic diagram of current trend changes of charging methods according to some embodiments of the present application.
  • FIG. 5 is a schematic diagram of current trend changes of charging methods according to some embodiments of the present application.
  • FIG. 6 is a schematic diagram of current trend changes of charging methods according to some embodiments of the present application.
  • FIG. 7 is a schematic diagram of current trend changes of charging methods according to some embodiments of the present application.
  • FIG. 8 is a schematic diagram of current trend changes of charging methods according to some embodiments of the present application.
  • the present application provides a charging method for a rechargeable device, the charging method including a constant current charging stage and a constant voltage charging stage, wherein in the constant current charging stage, the constant current charging is carried out to 10% to 90%
  • the SOC performs at least one rest and/or at least one negative charge, wherein the time for each rest is T 1 , T 1 ⁇ 30s, and the time for each negative charge is T 2 , and T 2 ⁇ 10s.
  • the static process is to eliminate the electrochemical and concentration polarization process of the cell.
  • the negative charging process has two effects: one is to eliminate lithium dendrites with an instantaneous negative current; the other is to eliminate the polarization process.
  • SOC charge capacity/theoretical capacity
  • C represents the current rate
  • C current/capacity
  • the standing time T 1 satisfies 1 min ⁇ T 1 ⁇ 4min. In some embodiments, T 1 is 1 min, 1.5 min, 2 min, 2.5 min, 3 min, or 3.5 min.
  • the negative charging time T 2 satisfies 10s ⁇ T 2 ⁇ 4min. In some embodiments, 30s ⁇ T2 ⁇ 4min . In some embodiments, 1 min ⁇ T2 ⁇ 4min. In some embodiments, T 2 is 1 min, 1.5 min, 2 min, 2.5 min, 3 min, or 3.5 min.
  • the rechargeable device may be a lithium metal battery.
  • the anode of the rechargeable device contains lithium metal or an alloy of lithium metal.
  • the lithium metal alloy is Li x M, wherein M is selected from one or more of Al, Mg, In, Sn, and B.
  • constant current charging to 10% to 90% SOC, eg 10% SOC, 15% SOC, 20% SOC, 25% SOC, 40% SOC, 50% SOC, 60 %SOC, 70% SOC or 80% SOC for first negative charge or rest. In some embodiments, constant current charging to 10% to 40% SOC for negative charging or resting.
  • the frequency of negative charging may be one time in a single circle, or one time in multiple circles, and the multiple circles may be every 5 circles or every 10 circles or every 20 circles or every 50 circles, preferably a single circle Circle once.
  • the charging method includes the following steps: (1) performing a first constant current charging on the rechargeable device until 10% to 90% SOC; (2) charging the rechargeable device after the first constant current charging The charging device performs static and/or negative charging; (3) the rechargeable device after static and/or negative charging is subjected to second constant current charging; (4) after the second constant current charging The rechargeable device is charged with constant voltage.
  • the number of times of standing is n, and 1 ⁇ n ⁇ 10.
  • the number of times of negative charging is m, where 1 ⁇ m ⁇ 5.
  • standing can be used multiple times, and the interval time can be of equal length, or consistent with the anodic polarization overpotential, or other variation laws.
  • the negative current may be used multiple times, and the interval time may be equal, or consistent with the anodic polarization overpotential, or may be other variation laws.
  • the charging capacity of the constant current charging is Q +
  • the charging capacity of the negative charging is Q ⁇
  • the charging capacity of the constant current charging is greater than the charging capacity of the negative charging, that is, Q + > Q - .
  • each negative charge capacity Q ⁇ satisfies: 1%Q ⁇ Q ⁇ 10%Q, where Q is the difference between Q + and Q ⁇ (the charge capacity of constant current charging and the negative charge difference in charging capacity).
  • Q is the difference between Q + and Q ⁇ (the charge capacity of constant current charging and the negative charge difference in charging capacity).
  • 2%Q ⁇ Q- ⁇ 5%Q is the charge capacity of constant current charging and the negative charge difference in charging capacity.
  • the negative charging current I ⁇ and the constant current charging current I + satisfy: 3 ⁇ I ⁇ /I + ⁇ 20, preferably 3 ⁇ I ⁇ /I + ⁇ 6.
  • the current I + of the constant current charging satisfies: 0.1C ⁇ I + ⁇ 0.5C.
  • the negative current needs to eliminate lithium dendrites. Under the condition of high current, it has a stronger tip effect, eliminates lithium dendrites more thoroughly, improves the anode interface, and prolongs the cycle life.
  • the negative charging has any one of the following characteristics A) to C): A) the current I- of the negative charging remains unchanged; B) the current I- of the negative charging is The first change slope increases, and then decreases with the second change slope; C) the negative charging current I- increases with the first change slope, maintains for a period of time, and then decreases with the second change slope.
  • the first method is to change the forward current stepwise to the negative current.
  • the charging current suddenly changes from 1C to the negative maximum negative current -Cmax.
  • the direction pulse is a negative current (as shown in Figure 2), and its ladder means that the positive current changes directly to the negative current, during which the current does not gradually change continuously.
  • 1C suddenly changes to 0C, at this time, the negative pulse is that the negative current gradually increases continuously from 0 to the maximum negative current -Cmax (as shown in Figure 4);
  • the third method is that the positive current gradually decreases to 0, and the negative current It gradually decreases from 0 to the maximum negative current Cmax with the same change slope (as shown in Figure 5).
  • the negative charging process uses the negative current I ⁇ to satisfy: 0.2C ⁇ I ⁇ ⁇ 2C, such as 0.5C, 0.8C, 1.0C, 1.5C, and the like.
  • the first change slope k1 satisfies: 0.0167C/s ⁇ k1 ⁇ 0.2C/s.
  • the second change slope k2 satisfies: 0.0167C/s ⁇ k2 ⁇ 0.2C/s.
  • a first variable current charging is further included between steps (1) and (2).
  • a second variable current charging is further included between steps (2) and (3).
  • in the first variable current charging the first forward current I 1 decreases with a third slope of change
  • the second forward current I 2 decreases with the third 4. The slope of change increases.
  • the third change slope k3 satisfies: 0.0167C/s ⁇ k3 ⁇ 0.2C/s.
  • the fourth change slope k4 satisfies: 0.0167C/s ⁇ k4 ⁇ 0.2C/s.
  • the present application provides a charging device, the charging device comprising: a constant current charging module; a stationary module and/or a negative charging module for performing constant current charging to 10% to 90% SOC At least one standstill and/or at least one negative charge, wherein the time for each stand is T 1 , T 1 ⁇ 30s, and the time for each negative charge is T 2 , T 2 ⁇ 10s; constant voltage charging module , used for constant voltage charging of rechargeable devices after constant current charging.
  • the charging device is configured to execute the charging method described in the first aspect of the present application.
  • the present application provides a charging device comprising a memory and a processor, where the memory is used for storing executable program codes, and the processor is used for reading the executable program codes stored in the memory to execute the charging method described in the first aspect of the present application.
  • the aforementioned storage medium includes: U disk, mobile hard disk, read-only memory (Read-Only Memory, ROM), random access memory (Random Access Memory, RAM), magnetic disk or optical disk and other media that can store program codes.
  • Positive electrode The positive electrode is composed of a mixture of 96.7% LiCoO 2 +1.7% PVDF (binder) + 1.6% SP (conducting agent), which is coated on the surface of the positive current collector aluminum foil. After cold pressing, the length and width are 42.5mm. The 49.5mm square piece is ready for use;
  • Negative electrode Punch the ready-made lithium-coated copper foil into square pieces with a length and width of 44mm and 51mm, respectively;
  • EC ethylene carbonate
  • EMC ethyl methyl carbonate
  • DEC diethyl carbonate
  • Isolation film use polyethylene (PE) with a thickness of 15um and cut it into rolls with a width of 47.2mm for use;
  • the conventional CC-CV charging method is used to charge the lithium metal battery, as shown in Figure 1, which includes the following steps:
  • Constant current charging stage charge with 0.2C constant current until the cut-off voltage is 4.45V;
  • Constant voltage charging stage charge at a constant voltage of 4.45V to a cut-off current of 0.05C.
  • charging a lithium metal battery includes the following steps:
  • the first constant current charging stage charge at 0.2C constant current to 20% SOC;
  • Negative charging stage then charge with a single step negative current of 1C for 2min (3.3%Q);
  • the second constant current charging stage continue to charge with 0.2C constant current until the cut-off voltage is 4.45V;
  • Constant voltage charging stage After reaching the cut-off voltage of 4.45V, constant-voltage charging is performed until the cut-off current is 0.05C.
  • Example 1 The only difference from Example 1 is that the state of charge at the start of negative charging is different, where Example 2 is 40% SOC, Example 3 is 60% SOC, and Example 4 is 80% SOC.
  • Embodiments 5 to 7 differ from Embodiment 1 only in that the parameters of the negative charging phase in step (2) are adjusted, wherein:
  • Example 5 is to use a single step negative current 2C to charge, and the time is 1min (3.3%Q);
  • Example 6 is to use a single step negative current 1C to charge, and the time is 3min (4.95%Q);
  • Example 7 uses a single step negative current 2C to charge for 3min (9.9%Q).
  • charging a lithium metal battery includes the following steps:
  • the first constant current charging stage charge at 0.2C constant current to 20% SOC;
  • the first negative charging stage then use a single step negative current 1C to charge for 2min (3.3%Q);
  • the second constant current charging stage continue to charge at 0.2C constant current to 80% SOC;
  • the second negative charging stage then use a single step negative current 1C to charge, and the charging time is 2min (3.3% SOC);
  • the third constant-direction charging stage continue to charge at a constant current of 0.2C to a cut-off voltage of 4.45V;
  • Constant voltage charging stage After reaching the cut-off voltage, constant-voltage charging to cut-off current of 0.05C.
  • each cycle of charging is carried out according to the above steps.
  • charging a lithium metal battery includes the following steps:
  • the first constant current charging stage charge at 0.2C constant current to 40% SOC;
  • the first negative charging stage then use a single step negative current 1C to charge for 2 minutes (3.3% SOC);
  • the second constant current charging stage continue to charge at 0.2C constant current to 60% SOC;
  • the second negative charging stage then use a single step negative current 1C to charge, and the charging time is 2min (3.3% SOC);
  • the third constant-direction charging stage continue to charge at a constant current of 0.2C to a cut-off voltage of 4.45V;
  • Constant voltage charging stage After reaching the cut-off voltage, constant-voltage charging to cut-off current of 0.05C.
  • each cycle of charging is carried out according to the above steps.
  • the charging method is basically the same as in Example 1, except that in the cycle test, the first cycle is exactly the same as in Example 1, and the second to fifth cycles are charged according to conventional CC-CV (ie, there is no negative charging stage), and The 6th lap continues to follow the charging method of the 1st lap, that is, repeats every 5 laps, as shown in Figure 8.
  • the charging method is basically the same as in Example 1, except that in the cycle test, the first cycle is exactly the same as in Example 1, and the 2-9 cycles are charged according to conventional CC-CV (ie, there is no negative charging stage), and The 11th lap continues to follow the charging method of the 1st lap, which is repeated every 10 laps.
  • the charging method is basically the same as that of Example 8, the difference is that during the cycle test, the first cycle is carried out according to Example 8, and the second to fifth cycles are charged according to the conventional CC-CV charging method of Comparative Example 1, that is, every 5 cycles is repeated. .
  • charging the lithium metal battery includes the following steps:
  • the first constant current charging stage charge at 0.2C constant current to 20% SOC;
  • Negative charging stage use a single negative current charging, in which the negative current gradually changes from 0 to the maximum negative current 1C at a rate of change of 0.033C/s, and is charged with a negative current of 1C for a certain period of time, and then The negative current gradually changes from 1C to 0 at a rate of change of 0.033C/s, and the negative charging stage lasts for 2min (3.3%Q);
  • the second constant current charging stage continue to charge with 0.2C constant current until the cut-off voltage is 4.45V;
  • each cycle of charging is carried out according to the above steps.
  • the lithium metal battery is charged, as shown in Figure 5, which includes the following steps:
  • the first constant current charging stage charge at 0.2C constant current to 20% SOC;
  • the first variable current charging stage the current gradually decreases from 0.2C to 0 at a rate of change of 0.0367C/s;
  • Negative charging stage charge with a single negative current, in which the negative current gradually changes from 0 to the maximum negative current of 1C at a rate of change of 0.0367C/s, and then the negative current is charged at a rate of 0.0367C/s. The rate of change gradually changed from 1C to 0, and the negative charging stage lasted for 2min (3.3%Q);
  • the second variable current charging stage the current gradually increases from 0 to 0.2C at a rate of change of 0.0367C/s;
  • the second constant current charging stage continue to charge with 0.2C constant current until the cut-off voltage is 4.45V;
  • Constant voltage charging stage After reaching the cut-off voltage, the 4.45V constant voltage is charged to the cut-off current of 0.05C.
  • each cycle of charging is carried out according to the above steps.
  • charging a lithium metal battery includes the following steps:
  • the first constant current charging stage charge at 0.2C constant current to 20% SOC;
  • the second constant current charging stage continue to charge with 0.2C constant current until the cut-off voltage is 4.45V;
  • Constant voltage charging stage after reaching the cut-off voltage, constant-voltage charging to cut-off current 0.05C.
  • charging the lithium metal battery includes the following steps:
  • the first constant current charging stage charge at 0.2C constant current to 20% SOC;
  • the second constant current charging stage continue to charge at 0.2C constant current to 80% SOC;
  • the second constant current charging stage continue to charge with 0.2C constant current until the cut-off voltage is 4.45V;
  • Constant voltage charging stage After reaching the cut-off voltage, constant-voltage charging to cut-off current of 0.05C.
  • Comparing Examples 1 to 4 it can be seen that when the initial SOC of negative charging is lower than 50% SOC, preferably 10% to 40% SOC, it is helpful to further improve the cycle performance of lithium metal batteries. Comparing Example 1 and Example 5, it can be seen that when 3 ⁇ I ⁇ /I + ⁇ 9, the cycle performance of the lithium metal battery can be further improved. Comparing Examples 1, 6 and 7, it can be seen that when 2%Q ⁇ Q- ⁇ 5%Q, the cycle performance of the lithium metal battery can be further improved.
  • the aforementioned program can be stored in a computer-readable storage medium.
  • the steps including the above method embodiments are executed; and the aforementioned storage medium includes: ROM, RAM, magnetic disk or optical disk and other media that can store program codes.

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  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Secondary Cells (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Charge And Discharge Circuits For Batteries Or The Like (AREA)

Abstract

La présente invention concerne un procédé de charge pour un appareil rechargeable, un appareil de charge, et un dispositif de charge. Le procédé de charge comporte une phase de charge à courant constant et une phase de charge à tension constante. Lors de la phase de charge à courant constant, une attente et/ou une charge négative est effectuée au moins une fois lorsque la charge à courant constant atteint 10% à 90% de SOC, la période pour chaque instance d'attente étant T1, T1≥30s, et la période pour chaque instance de charge négative étant T2, T2≥10s. Le procédé de charge de la présente invention peut améliorer les performances cycliques d'une batterie lithium-métal.
PCT/CN2021/083056 2021-03-25 2021-03-25 Procédé de charge, appareil de charge et dispositif de charge WO2022198584A1 (fr)

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PCT/CN2021/083056 WO2022198584A1 (fr) 2021-03-25 2021-03-25 Procédé de charge, appareil de charge et dispositif de charge
CN202180004986.8A CN114531928B (zh) 2021-03-25 2021-03-25 充电方法、充电装置和充电设备

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