WO1999050925A1 - Procede de recharge d'un accumulateur electrochimique - Google Patents

Procede de recharge d'un accumulateur electrochimique Download PDF

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Publication number
WO1999050925A1
WO1999050925A1 PCT/CA1999/000269 CA9900269W WO9950925A1 WO 1999050925 A1 WO1999050925 A1 WO 1999050925A1 CA 9900269 W CA9900269 W CA 9900269W WO 9950925 A1 WO9950925 A1 WO 9950925A1
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WO
WIPO (PCT)
Prior art keywords
cell
charge
voltage
charging
positive electrode
Prior art date
Application number
PCT/CA1999/000269
Other languages
English (en)
Inventor
Lynn S. Marcoux
Original Assignee
Bluestar Advanced Technology Corp.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Bluestar Advanced Technology Corp. filed Critical Bluestar Advanced Technology Corp.
Publication of WO1999050925A1 publication Critical patent/WO1999050925A1/fr

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • 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
    • 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
    • H02J7/00714—Regulation of charging or discharging current or voltage the cycle being controlled or terminated in response to electric parameters in response to battery charging or discharging current
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • This invention relates to battery charging systems and, in particular, to battery charging systems for lithium ion batteries.
  • Electrochemical storage batteries are well known in commerce.
  • the term battery is used to refer to a device comprising one or more electrochemical cells.
  • These electrochemical cells comprise two active electrodes and an ionically conductive electrolyte interposed between the electrodes.
  • Such cells are designed to convert the energy stored within the cell, in the form of reactable chemical materials, into an electric current.
  • the reactable chemicals one of which is capable of oxidizing the other, are kept separate from one another, typically within the structure of the two electrodes, to prevent the direct reaction of these chemicals.
  • the driving force for the spontaneous reaction of these chemicals appears as a voltage at the interface between each electrode and the electrolyte, and through electrical connections within the electrodes, to the external terminals of the cell.
  • the reaction of the chemical materials takes place spontaneously when an external circuit connecting the two electrodes is closed, permitting current to flow from one electrode to the other, and the oxidation of one material by the other.
  • Electrochemical cells and batteries fall into two distinct categories. In some batteries the reactions taking place within the cells during discharge produce products which, due to their chemical or physical nature, cannot be reconverted into the original reactable chemical materials . Such batteries are called primary or non-rechargeable batteries.
  • the common alkaline battery is an example of a primary battery. When the chemical energy stored originally within such primary cells is consumed, the cells are of no further use.
  • the chemical and physical nature of the products of cell discharge are such that , by forcing a current through the discharged cell in a direction opposite to that produced by the cell during discharge, the products can be reconverted into the original reactable chemical materials.
  • the cell is then capable of a further discharge.
  • Such cells and batteries are called secondary or rechargeable batteries.
  • the common lead-acid battery is an example of a secondary battery.
  • the terminal voltage decreases only slightly during discharge and then decreases abruptly, as shown in FIG. 1, as the reactable chemical materials are completely consumed.
  • the capacity of the cell is defined as the charge withdrawn from the cell, expressed in coulombs or amp hours, before a predefined cutoff voltage is reached.
  • the cutoff voltage may be selected based upon the requirements of the device being powered, but is typically chosen, in the case of a cell which behaves as shown in FIG. 1, as a voltage in the near vertical region of the discharge curve. Note that the measured capacity would not differ significantly whether voltage A or voltage B were chosen as the cutoff voltage.
  • measured capacity for a cell will vary depending upon the rate of discharge (the current being drawn from the cell) and the temperature of the cell. This is due in part to voltage drops across resistive components within the cell, such as the terminals, the tabs connecting the terminals to the electrodes, the electrode structures and the electrolyte. At a high discharge current, a greater fraction of the voltage being generated at the two electrodes will not be seen at the cell terminals due to IR drop across resistive components. The IR drop across the electrolyte may become particularly significant at lower temperatures.
  • the rates of the electrochemical reactions at the two electrodes can also limit the capacity.
  • the current being demanded by the external circuit exceeds the capability of one or both electrodes, the voltage at the electrode/electrolyte interface decreases and thus the terminal voltage decreases. Because the reaction rates at the electrodes decrease with temperature, capacity generally decreases at lower temperatures.
  • a driving voltage must be supplied to the terminals of the cell in order to force current backward through the cell and to carry out the reconversion of the discharge products.
  • This charging voltage will be the sum of voltages at the two electrode/electrolyte interfaces, driving the electrochemical charging reactions, and the IR drops across the various resistive components of the cell. In an ideal secondary cell, the voltage necessary to force a significant charging current through a cell will rise rapidly, as shown in FIG. 2, when the reconversion - 4
  • the present invention is directed to providing a method and a device for substantially completely charging lithium ion batteries, under a variety of operating conditions, without causing measurable damage due to overcharge. In this way, discharge capacity remains substantially unchanged over hundreds, and perhaps thousands, of cycles.
  • a further advantage of the present method is that the charging times necessary to achieve full recharge are surprisingly short .
  • the application of this method significantly increases the capacity available from such lithium ion cells and batteries when operated at low temperatures. While the present method was developed specifically for the lithium ion battery, it is also applicable to other similar secondary battery systems.
  • Lewyn U.S. Patent No. 5,670,862 A conventional, prior art technique for recharging secondary batteries is disclosed in Lewyn U.S. Patent No. 5,670,862.
  • Lewyn' s technique attempts to reduce charging times by compensating for the expected IR drop across the tabs connecting the electrodes to the terminals.
  • Lewyn however, a specific resistor, representing that tab resistance, is wired into the charging circuit .
  • Lewyn does not teach or suggest the importance of measuring the electrolyte resistance and its variation with temperature, nor does Lewyn teach or suggest the variation of resistance within the cell with age.
  • the voltage which the charging device must supply to force this current into the cell is significantly less that the voltage at which concern of over charge damage arises.
  • the voltage needed to force more current into the cell increases and eventually reaches the predetermined cutoff voltage.
  • the charging device will continue to supply whatever current the cell can accept at the constant cutoff voltage.
  • Such a process gives rise to charging current and voltage curves, such as those shown in FIGs . 3A and 3B. Note that the charging current in the constant voltage region decreases approximately exponentially with time.
  • the effective charging voltage will continue to be less by the electrolyte IR drop in the low temperature case, so that the charging current will also continue to be less than in the room temperature case.
  • the low temperature cell receives less charge than a room temperature cell and thus will have reduced capacity in the subsequent discharge ._
  • the constant current phase of the charging process is increased in time at low temperature, as shown schematically in FIG. 7B and approaches that at room temperature, while the effective charging voltage at the electrode surfaces does not exceed the specified limit.
  • the voltage during the now nearly constant phase of the charging process varies slightly as the current decreases and the IR drop across the internal resistance decreases.
  • the measurement of the internal resistance and varying of the cutoff voltage also recognizes the effect of increased internal resistance with age found in some batteries, particularly those with reactive negative electrodes, such as lithium, and improve capacity retention.
  • FIG. 1 is a plot of cell terminal voltage as a function of time, showing that, in an ideal battery, the terminal voltage decreases only slightly during discharge and then decreases abruptly as the reactable chemical materials are completely consumed.
  • FIG. 2 is a plot of cell terminal voltage as a function of time, showing that in an ideal secondary cell, the voltage necessary to force a significant charging current through a cell will rise rapidly when the reconversion process is completed and - 10
  • FIGs . 3A and 3B are companion plots of cell terminal voltage as a function of time and cell current as a function of time, respectively, showing that the charging current in the constant voltage region of secondary cells decreases approximately exponentially with time.
  • FIG. 4 is a plot of cell capacity (in amp hours) as a function of the number of cycles, showing the observed discharge capacity decreases with cycle number up to cycle 210.
  • FIG. 5 is a plot of total charging time (in hours) as a function of the number of cycles, showing that the additional time required to achieve substantially complete recharging of a lithium ion secondary cell is not great, and though it increases with time, the increase is not great.
  • FIG. 6 is a schematic diagram of a secondary cell, showing that, when a current is forced through a lithium ion secondary cell, a portion of the terminal voltage applied to the terminal will appear as an IR drop across the various resistive components in the cell.
  • FIGs. 7A and 7B are companion plots of cell terminal voltage as a function of time and cell current as a function of time, respectively, showing the effects of IR compensation.
  • the curves labeled "a" are identical to those in FIG. 3 and show the conventional, prior art approach.
  • FIG. 8 is a plot of cell capacity (in amp hours) as a function of the number of cycles for a secondary cell in which the positive electrode material was a 11 -
  • lithiated manganese dioxide LiMn 2 0 4
  • lithiated cobalt oxide LiCo0 2
  • FIG. 9 is a composite plot of cell capacity (in amp hours) as a function of the number of cycles, showing that a significant improvement in cell capacity was achieved when the voltage limits included compensation for cell internal resistance.
  • the present method substantially completely charges lithium ion batteries, under a variety of operating conditions, without causing measurable damage due to overcharge, as shown in the following examples.
  • the examples show that the discharge capacity of lithium ion secondary cells remains substantially unchanged over numerous cycles.
  • the examples also show that the charging times necessary to achieve full recharge of lithium ion secondary cells are surprisingly short.
  • the examples further show that the present method significantly increases the capacity available from lithium ion secondary cells and batteries when operated at low temperatures .
  • a 40-Ah fully-welded electrochemical cell was assembled and activated and subjected to cycle life testing.
  • the positive electrode for this cell was prepared by coating a 0.001 inch (0.00254 cm) Al foil on both sides with a mixture of lithiated cobalt oxide (LiCo0 2 ) , conductive carbon and an organic binder. Following coating, this material was further densified, slit to width and fitted with metal tabs for connection to the internal terminals of the cell. 12 -
  • the negative electrode for this cell was prepared by coating a 0.0004 inch (.00116 cm) Cu foil on both sides with a mixture of synthetic graphite, conductive carbon and an organic binder. Following coating, this material was also further densified, slit to width and fitted with metal tabs for connection to the internal terminals of the cell. The electrodes were then combined with alternating layers of microporous polyolefin separator and concentrically wound to form a cylindrical element. This cylindrical element was placed within a closed- end stainless steel tube with a length of 7.00 inch (17.78 cm) and a diameter of 2.48 inch (6.2992 cm).
  • a circular cell cap was prepared by welding two glass insulated electrical connectors, a 175-psi (1.21 MP (1.21*10 6 N/m 2 ) ) rupture disk and stainless steel fill tube into a pre-punched stainless steel cap.
  • the tabs from the positive electrode of the cylindrical cell element were welded to one of the insulated electrical connectors and the tabs from the negative electrode of the cylindrical cell element were welded to the remaining connector.
  • the cap was then fitted into the cylindrical cell container and welded in place.
  • An organic electrolyte solution containing ethylene carbonate, diethyl carbonate and lithium hexafluorophosphate was then introduced under vacuum through the fill tube. The fill tube was then welded closed completing the assembly process.
  • the cycling regime was maintained from cycle 11 to cycle 216 and, as may be seen in FIG. 4, during this time the discharge capacity continuously declined from a value of 38 Ah to a value of 32 Ah. After cycle 216, the discharge regime was allowed to remain the same and the charging methodology was modified.
  • the modified charging program consisted of an initial constant current charge to 4.1 V followed by constant voltage charging at 4.1 also identical to that of the initial cycles. The change effected involved the criterion for charge termination. Rather than terminating the charging process after a fixed time interval, a coulombic criterion for charge termination was employed.
  • a cell with a diameter of 1.31 inch (3.3274 cm) and a length of 4.38 inch (11.1252 cm) was assembled using techniques similar to those described in Example 1.
  • the positive electrode material was a lithiated manganese dioxide (LiMn 2 0 4 ) rather than LiCo0 2 and the coulombic charge termination was employed for all cycles following the formation cycles.
  • This cell was discharged at a rate of 1.0 A to a voltage of 3.00 V and then charged at this current until a voltage of 4.1 V was achieved at which point the voltage was held constant at this value and charging was allowed to continue with decreasing current until and amount of charge had been returned equivalent to that extracted during the discharge segment of the cycle. Cycling was continued until a total of 75 cycles had been accumulated and then terminated for convenience. During this time cell capacity remained constant at 4.75 Ah, as shown in FIG. 8, and the total charging time increased from 5 hours to 10 hours.
  • the value of voltage limit compensation for achieving good low temperature performance is demonstrated using 6 -Ah cells with a LiCo0 2 positive electrode.
  • the cell had a diameter of 1.31 inch (3.3274 cm), a length of 4.38 inch (11.1252 cm), and was assembled with components and processes similar to those described in Example 1.
  • the tests were performed at -30 °C with a single 3- cell pack with the cells connected in a parallel configuration. Results were reported as single cell capacities (that is, the pack capacity was divided by 3) for comparison purposes. In one test, the cell pack was cycled at the C/5 rate (1.2A/cell) between 15 -
  • the standard voltage range of 3.0 to 4.1 V was employed and in the other case a range of 2.92 to 4.18 V was employed.
  • the latter range included compensation for the internal resistance of the cell at this temperature.
  • the cells were discharged to the lower voltage limit at the C/5 rate and the current was then reversed and the cells were charged at this rate until the upper voltage cutoff value was achieved. Charging was then continued in the constant voltage mode for a period of 2.5 hours.
  • This test sequence was also repeated at the C/2 rate (2.0 A) in which case the voltage limits were 2.79 V and 4.31 V. Cells were cycled for at least 4 cycles at each set of charge/discharge conditions. The results for these tests are shown in FIG. 9.

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  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

L'invention concerne un procédé d'utilisation d'un accumulateur électrochimique, comprenant les opérations suivantes: (a) on mesure la quantité de charge produite par l'accumulateur durant la décharge, (b) on recharge l'accumulateur en faisant passer un courant de charge sensiblement constant à travers l'accumulateur jusqu'à ce que la tension de l'accumulateur atteigne un point de coupure prédéterminé, et (c) on continue à charger l'accumulateur en maintenant le niveau de tension de coupure prédéterminé jusqu'à ce que la totalité de la charge retournée à l'accumulateur soit égale à la charge produite par l'accumulateur pendant la décharge précédente. Ce procédé permet de charger quasi intégralement des accumulateurs à ions lithium et d'autres accumulateurs du même type dans des conditions d'utilisation diverses, sans provoquer de dégâts mesurables dus à la surcharge. Avec ce procédé, la capacité de décharge reste sensiblement inchangée pendant un grand nombre de cycles. Les durées nécessaire à une recharge complète sont également plus brèves qu'avec les procédés conventionnels existant à ce jour. Ce procédé accroît en outre la capacité obtenue avec des accumulateurs fonctionnant à de basses températures. Il est avantageux de procéder séparément à un réglage de la tension de coupure afin de compenser une résistance interne mesurée et de charger jusqu'à un point de coupure coulombien, la combinaison des deux opérations permettant d'améliorer la rétention de la charge et de réduire le temps de charge tout en protégeant l'accumulateur contre des réactions indésirables de décharge excessive.
PCT/CA1999/000269 1998-03-27 1999-03-26 Procede de recharge d'un accumulateur electrochimique WO1999050925A1 (fr)

Applications Claiming Priority (2)

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US7974898P 1998-03-27 1998-03-27
US60/079,748 1998-03-27

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WO1999050925A1 true WO1999050925A1 (fr) 1999-10-07

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Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2003044880A1 (fr) * 2001-11-19 2003-05-30 Quallion Llc Accumulateur rechargeable au lithium prevu pour supporter la decharge a zero volt
FR2872633A1 (fr) * 2004-07-02 2006-01-06 Commissariat Energie Atomique Procede de charge d'un accumulateur lithium-ion a electrode negative
US7177691B2 (en) 1999-07-30 2007-02-13 Advanced Bionics Corporation Implantable pulse generators using rechargeable zero-volt technology lithium-ion batteries
EP1850446A1 (fr) * 2006-04-26 2007-10-31 Sagem Defense Securite Procédé de charge de batterie avec compensation de resistance interne, chargeur et batterie pour la mise en oeuvre de ce procédé
CN107039681A (zh) * 2016-08-22 2017-08-11 杜文龙 一种旧动力锂电池提高内阻一致性的充电方法
CN113948783A (zh) * 2021-10-12 2022-01-18 远景动力技术(江苏)有限公司 锂离子电池及其预循环活化方法

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH01294374A (ja) * 1988-05-20 1989-11-28 Japan Storage Battery Co Ltd 非水リチウム二次電池の充電方法
DE3832839A1 (de) * 1988-09-28 1990-03-29 Ind Automation Mikroelektronik Geraet zur ueberwachung von wiederaufladbaren batterien
EP0709906A1 (fr) * 1994-10-26 1996-05-01 Sony Corporation Batterie secondaire au lithium à électrolyte non-aqueux
EP0795946A2 (fr) * 1996-03-12 1997-09-17 SILICONIX Incorporated Technique de chargement rapide pour batteries à ions de lithium
US5691620A (en) * 1993-09-17 1997-11-25 Sony Corporation Battery charging method

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH01294374A (ja) * 1988-05-20 1989-11-28 Japan Storage Battery Co Ltd 非水リチウム二次電池の充電方法
DE3832839A1 (de) * 1988-09-28 1990-03-29 Ind Automation Mikroelektronik Geraet zur ueberwachung von wiederaufladbaren batterien
US5691620A (en) * 1993-09-17 1997-11-25 Sony Corporation Battery charging method
EP0709906A1 (fr) * 1994-10-26 1996-05-01 Sony Corporation Batterie secondaire au lithium à électrolyte non-aqueux
EP0795946A2 (fr) * 1996-03-12 1997-09-17 SILICONIX Incorporated Technique de chargement rapide pour batteries à ions de lithium

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
PATENT ABSTRACTS OF JAPAN vol. 014, no. 082 (E - 0889) 15 February 1990 (1990-02-15) *

Cited By (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7818068B2 (en) 1999-07-30 2010-10-19 Boston Scientific Neuromodulation Corporation Implantable pulse generators using rechargeable zero-volt technology lithium-ion batteries
US7248929B2 (en) 1999-07-30 2007-07-24 Advanced Bionics Corporation Implantable devices using rechargeable zero-volt technology lithium-ion batteries
US7177691B2 (en) 1999-07-30 2007-02-13 Advanced Bionics Corporation Implantable pulse generators using rechargeable zero-volt technology lithium-ion batteries
US7184836B1 (en) 1999-07-30 2007-02-27 Advanced Bionics Corporation Implantable devices using rechargeable zero-volt technology lithium-ion batteries
WO2003044880A1 (fr) * 2001-11-19 2003-05-30 Quallion Llc Accumulateur rechargeable au lithium prevu pour supporter la decharge a zero volt
US7671568B2 (en) 2004-07-02 2010-03-02 Commissariat A L'energie Atomique Method of charging a lithium-ion battery comprising a negative electrode
FR2872633A1 (fr) * 2004-07-02 2006-01-06 Commissariat Energie Atomique Procede de charge d'un accumulateur lithium-ion a electrode negative
WO2006097586A1 (fr) * 2004-07-02 2006-09-21 Commissariat A L'energie Atomique Procede de charge d’un accumulateur lithium-ion a electrode negative
EP1850446A1 (fr) * 2006-04-26 2007-10-31 Sagem Defense Securite Procédé de charge de batterie avec compensation de resistance interne, chargeur et batterie pour la mise en oeuvre de ce procédé
US8212531B2 (en) 2006-04-26 2012-07-03 Sagem Defense Securite Method of charging a battery, and a corresponding charger and battery
FR2900503A1 (fr) * 2006-04-26 2007-11-02 Sagem Defense Securite Procede de charge de batterie avec compensation de resistance interne, chargeur de batterie pour la mise en oeuvre de ce procede
CN107039681A (zh) * 2016-08-22 2017-08-11 杜文龙 一种旧动力锂电池提高内阻一致性的充电方法
CN113948783A (zh) * 2021-10-12 2022-01-18 远景动力技术(江苏)有限公司 锂离子电池及其预循环活化方法
CN113948783B (zh) * 2021-10-12 2023-12-01 远景动力技术(江苏)有限公司 锂离子电池及其预循环活化方法

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