WO2013187581A1 - 혼합 양극재를 포함하는 이차 전지의 충전 상태 추정 장치 및 방법 - Google Patents
혼합 양극재를 포함하는 이차 전지의 충전 상태 추정 장치 및 방법 Download PDFInfo
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- WO2013187581A1 WO2013187581A1 PCT/KR2013/002141 KR2013002141W WO2013187581A1 WO 2013187581 A1 WO2013187581 A1 WO 2013187581A1 KR 2013002141 W KR2013002141 W KR 2013002141W WO 2013187581 A1 WO2013187581 A1 WO 2013187581A1
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- charge
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- secondary battery
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- charging
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
- G01R31/00—Arrangements for testing electric properties; Arrangements for locating electric faults; Arrangements for electrical testing characterised by what is being tested not provided for elsewhere
- G01R31/36—Arrangements for testing, measuring or monitoring the electrical condition of accumulators or electric batteries, e.g. capacity or state of charge [SoC]
- G01R31/382—Arrangements for monitoring battery or accumulator variables, e.g. SoC
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
- G01R31/00—Arrangements for testing electric properties; Arrangements for locating electric faults; Arrangements for electrical testing characterised by what is being tested not provided for elsewhere
- G01R31/36—Arrangements for testing, measuring or monitoring the electrical condition of accumulators or electric batteries, e.g. capacity or state of charge [SoC]
- G01R31/367—Software therefor, e.g. for battery testing using modelling or look-up tables
-
- G—PHYSICS
- G01—MEASURING; TESTING
- G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
- G01R31/00—Arrangements for testing electric properties; Arrangements for locating electric faults; Arrangements for electrical testing characterised by what is being tested not provided for elsewhere
- G01R31/36—Arrangements for testing, measuring or monitoring the electrical condition of accumulators or electric batteries, e.g. capacity or state of charge [SoC]
- G01R31/382—Arrangements for monitoring battery or accumulator variables, e.g. SoC
- G01R31/3835—Arrangements for monitoring battery or accumulator variables, e.g. SoC involving only voltage measurements
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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
- H01M10/48—Accumulators combined with arrangements for measuring, testing or indicating the condition of cells, e.g. the level or density of the electrolyte
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/364—Composites as mixtures
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/50—Current conducting connections for cells or batteries
- H01M50/569—Constructional details of current conducting connections for detecting conditions inside cells or batteries, e.g. details of voltage sensing terminals
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
- G01R31/00—Arrangements for testing electric properties; Arrangements for locating electric faults; Arrangements for electrical testing characterised by what is being tested not provided for elsewhere
- G01R31/36—Arrangements for testing, measuring or monitoring the electrical condition of accumulators or electric batteries, e.g. capacity or state of charge [SoC]
- G01R31/382—Arrangements for monitoring battery or accumulator variables, e.g. SoC
- G01R31/3828—Arrangements for monitoring battery or accumulator variables, e.g. SoC using current integration
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
Definitions
- the present application relates to a method and an apparatus capable of estimating the state of charge of a secondary battery.
- a battery may be a device that can be carried in a human hand such as a mobile phone, a laptop computer, a digital camera, a video camera, a tablet computer, a power tool, or the like;
- Various electric drive power devices such as electric bicycles, electric motorcycles, electric vehicles, hybrid vehicles, electric boats, electric airplanes, and the like;
- a power storage device used to store power generated by renewable energy or surplus generated power;
- the field of use extends to an uninterruptible power supply for stably supplying power to various information communication devices including server computers and communication base stations.
- the cell comprises three basic components: an anode comprising a material that is oxidized while releasing electrons during discharge, and a cathode comprising a material that is reduced while receiving electrons during discharge. And an electrolyte that allows ion transport between the cathode and the anode.
- the battery may be classified into a primary battery that cannot be reused after being discharged, and a secondary battery capable of repetitive charging and discharging because the electrochemical reaction is at least partially reversible.
- secondary batteries examples include lead-acid batteries, nickel-cadmium batteries, nickel-zinc batteries, nickel-iron batteries, silver oxide batteries, nickel metal hydride batteries, zinc-manganese oxide batteries, zinc-bromide batteries, and metal- Air batteries, lithium secondary batteries and the like are known. Among them, lithium secondary batteries have attracted the greatest commercial interest because of their higher energy density, higher battery voltage, and longer shelf life than other secondary batteries.
- the material used as a positive electrode material has an important influence on the performance of a secondary battery. Therefore, various attempts have been made to provide a cathode material that is stable at high temperatures, can provide a high energy capacity, has a long lifetime, and has a low manufacturing cost.
- the present application provides a blended cathode material that can compensate for the disadvantages of each cathode material by branding two or more cathode materials, and provides an apparatus and method for estimating the state of charge of a secondary battery including the blended cathode material. .
- An apparatus for estimating the state of charge of a secondary battery includes a positive electrode including a mixed positive electrode material including a first positive electrode material and a second positive electrode material having different operating voltage ranges, a negative electrode including a negative electrode material, and the positive electrode;
- An apparatus for estimating the state of charge of a secondary battery comprising a separator for separating a negative electrode, comprising: a sensor for measuring a dynamic voltage of the secondary battery while the secondary battery is being charged; And identify the dynamic voltage profile of the secondary battery as a transition interval voltage pattern, calculate a parameter of the transition interval voltage pattern, and calculate the secondary battery from the calculated parameter using a predefined correlation between the parameter and the state of charge. It may include a control unit for estimating the state of charge of.
- the state of charge refers to the amount of electrical energy stored in the secondary battery, and is known in the art as a parameter called state of charge (SOC).
- SOC state of charge
- the state of charge can be quantitatively indicated by the parameters SOC and z, using the SOC parameter to indicate the state of charge as a percentage and the z parameter to indicate the state of charge to a value of 1 or less. do.
- the state of charge may be measured by an ampere counting method or the like as a non-limiting example.
- the transition period voltage pattern means a profile of a voltage including an inflection point and having a shape in which a curvature changes around the inflection point.
- the curvature changes from concave to convex, for example.
- the transition section voltage pattern is generated in a charged state section in which reaction kinetics of operating ions change while the secondary battery is charged.
- the transition section voltage pattern is generated in a charged state section in which the type of cathode material mainly reacting with the operating ions is changed.
- the charging state section in which the transition section voltage pattern occurs is defined as a transition section.
- the dynamic voltage means a voltage measured while the secondary battery is being charged or discharged. Therefore, even if the state of charge of the secondary battery is the same, the dynamic voltage is different from the open voltage measured when the secondary battery is in a no-load state. The difference is caused by the IR effect and the polarization effect generated when the secondary battery is charged or discharged.
- the dynamic voltage shows a change pattern similar to the open voltage as the state of charge changes. For example, if the curvature of the open voltage profile changes in a specific charging state section, the curvature of the dynamic voltage profile may change in the same charging state section.
- the working ions refer to ions which electrochemically react with the first and second cathode materials in the process of charging or discharging the secondary battery.
- the operating ions may vary depending on the type of secondary battery. For example, in the case of a lithium secondary battery, the operating ion may be lithium ion.
- the reaction refers to an electrochemical reaction including oxidation and reduction reactions of the first and second cathode materials involved in the charging or discharging of the secondary battery, and may vary according to an operation mechanism of the secondary battery.
- the electrochemical reaction may mean that operating ions are inserted into the first cathode material and / or the second cathode material or vice versa.
- the concentration of operating ions inserted into the first and / or second cathode material or vice versa may vary as the voltage of the secondary battery changes. For example, in one voltage band, operating ions may be preferentially inserted into the first cathode material over the second cathode material, and vice versa in another voltage band.
- operating ions may preferentially desorb from the second cathode material over the first cathode material, and vice versa in other voltage bands.
- the first positive electrode material and the second positive electrode material may have different operating voltage ranges from which they are activated.
- the activation of the first cathode material and the second cathode material means that the cathode material undergoes an electrochemical reaction with working ions.
- the first and second positive electrode material in order to satisfy the condition that the concentration of operating ions reacting with the first and second positive electrode material in accordance with the change in voltage, is at least one of the following conditions The above can be satisfied.
- the first and second positive electrode materials may show a difference in the position of the main peak and / or the intensity of the main peak when the dQ / dV distribution is measured.
- the dQ / dV distribution means the capacity characteristics of the operating ions for the cathode material by voltage.
- the position and / or intensity difference with respect to the main peak may vary depending on the type of the first and second cathode materials.
- the discharge resistance profile may have a convex pattern (so-called convex shape).
- the discharge resistance profile may have at least two inflection points before and after the peak of the Convex pattern.
- At least one voltage plateau may appear in an open voltage profile of a secondary battery including the first and second cathode materials.
- the voltage flat region refers to a region where the bending of the profile is changed while the inflection point is present and before and after the inflection point.
- At least one of the first and second cathode materials may have a voltage profile including a voltage flat region.
- the first cathode material the general formula A [A x M y ] O 2 + z
- A includes at least one element of Li, Na and K; M is Ni, Co, Mn, Ca, At least one element selected from Mg, Al, Ti, Si, Fe, Mo, V, Zr, Zn, Cu, Al, Mo, Sc, Zr, Ru, and Cr; x ⁇ 0, 1 ⁇ x + y ⁇ 2, -0.1 ⁇ z ⁇ 2; the stoichiometric coefficients of the components included in x, y, z, and M may be alkali metal compounds represented by).
- the first cathode material comprises at least one alkali metal compound xLiM 1 O 2- (1-x) Li 2 M 2 O 3 (M 1 has an average oxidation state of 3) disclosed in US 6,677,082, US 6,680,143 and the like.
- the second cathode material is a general formula Li a M 1 x Fe 1-x M 2 y P 1-y M 3 z O 4-z
- M 1 is Ti, Si, Mn, Co, Fe, At least one element selected from V, Cr, Mo, Ni, Nd, Al, Mg, and Al
- M 2 is Ti, Si, Mn, Co, Fe, V, Cr, Mo, Ni, Nd, Al, Mg
- M 3 includes a halogenated element optionally comprising F; 0 ⁇ a ⁇ 2, 0 ⁇ x ⁇ 1, 0 ⁇ y ⁇ 1, 0 ⁇ z ⁇ 1; the stoichiometric coefficients of the components included in a, x, y, z, M 1 , M 2 , and M 3 are selected so that the compound maintains electrical neutrality, or Li 3 Number of lithium metal phosphates represented by M 2 (PO 4 ) 3 [
- the second positive electrode material may be at least one selected from the group consisting of LiFePO 4 , LiMn x Fe y PO 4 (0 ⁇ x + y ⁇ 1), and Li 3 Fe 2 (PO 4 ) 3 .
- the first positive electrode material and / or the second positive electrode material may include a coating layer.
- the coating layer comprises a carbon layer, or in the group consisting of Ti, Si, Mn, Co, Fe, V, Cr, Mo, Ni, Nd, Al, Mg, Al, As, Sb, Si, Ge, V and S It may include an oxide layer or a fluoride layer containing at least one element selected.
- the mixing ratio of the first and second cathode materials may be appropriately adjusted in consideration of electrochemical design conditions considering the use of the secondary battery to be manufactured.
- the number of cathode materials that may be included in the mixed cathode material is not limited to two.
- the addition of other additives such as a conductive agent, a binder, etc. to the mixed cathode material is not particularly limited in order to improve physical properties of the mixed cathode material.
- control unit if the inflection point is present in the dynamic voltage profile, the dynamic voltage profile includes different bends, or if the first derivative of the dynamic voltage profile has a maximum value, the dynamic voltage profile Can be identified by the transition period voltage pattern.
- the calculated parameter may include a charge start voltage V initial at which an increase in voltage is started in the identified transition period voltage pattern, and a charge end voltage at which an increase in voltage in the identified transition period voltage pattern ends.
- V final the time it takes for the inflection point to appear on the basis of when the increase in voltage in the identified transition period voltage pattern is started, dV / dt at the inflection point, dV / at the inflection point dSOC (dSOC is obtained by calculating the capacity change per unit time using ampere counting method), the time taken for the dynamic voltage of the secondary battery to increase from the charge start voltage to the charge end voltage ( ⁇ T), the identified In the group consisting of the global integration value of the entire transition period voltage pattern and the local integration value integrating the transition period voltage pattern in a constant time range before and after the inflection point. It may include at least one selected.
- the predefined correlation may be a lookup table that defines a corresponding relationship between the parameter and the state of charge.
- the predefined correlation may be a lookup function using the parameter as an input variable and the state of charge as an output variable.
- the correlation may be predefined under the same charging condition that the dynamic voltage is measured.
- the apparatus for estimating charge state according to the present application may further include a storage unit in which the lookup table and / or the lookup function are stored.
- the estimated charging state may be a charging state before the charging is started or a charging state after the charging is completed.
- the senor measures the current of the secondary battery during the charging, and the control unit estimates the state of charge before the charge is started, and then accumulates the measured current to charge
- the state of charge change may be calculated and the state of charge after completion of the charge may be estimated by reflecting the state of charge change in the estimated state of charge.
- the charging may be pulse charging that is repeated at time intervals.
- the control unit may estimate the state of charge of the secondary battery whenever the pulse charging is repeated.
- the control unit may estimate the state of charge of the secondary battery whenever the dynamic voltage profile is identified by the transition period voltage pattern during each pulse charging.
- the apparatus for estimating charge state may further include a display unit configured to display the estimated charge state in a graphic interface, and the control unit may output the estimated charge state to the display unit.
- the apparatus for estimating state of charge according to the present application may further include a storage unit in which the estimated state of charge is stored, and the control unit may store the estimated state of charge in the storage unit.
- control unit may output the estimated state of charge to the outside.
- control unit calculates an inflection point identifier from the dynamic voltage measured by the sensor, and if the inflection point identifier satisfies an inflection point generation condition, determine a parameter corresponding to the transition period voltage pattern and The state of charge of the secondary battery may be estimated from the calculated parameter using a predefined correlation between the parameter and the state of charge of the secondary battery.
- the inflection point identifier may be updated each time a dynamic voltage is measured by the sensor.
- the inflection point identifier is used to determine whether the coin voltage measured by the sensor forms an inflection point over time.
- the inflection point identifier may be a first derivative value (dV / dt) of the dynamic voltage with respect to a measurement time of the dynamic voltage.
- the inflection point generation condition is a condition in which the first derivative value has a maximum value.
- the inflection point identifier may be a second derivative value (d 2 V / d 2 t) of the dynamic voltage with respect to the measurement time of the dynamic voltage.
- the inflection point generation condition is a condition that the second derivative value becomes zero.
- the inflection point identifier may be a first derivative value (dV / dSOC) of the dynamic voltage with respect to the state of charge of the secondary battery.
- the inflection point generation condition is a condition in which the first derivative value has a maximum value.
- the control unit is required until the inflection point generation condition is satisfied from the charge start voltage V initial , the charge end voltage V final , and the charge start time.
- control unit may estimate the state of charge of the secondary battery from the determined parameter using a lookup table that defines a corresponding relationship between the parameter and the state of charge.
- control unit may estimate the state of charge of the secondary battery from the determined parameter using a lookup function that uses the parameter and the state of charge as input variables and output variables, respectively. .
- An apparatus for estimating the state of charge of a secondary battery includes a positive electrode including a mixed positive electrode material including a first positive electrode material and a second positive electrode material having different operating voltage ranges, a negative electrode including a negative electrode material, and An apparatus for estimating a state of charge of a secondary battery mounted in an electric drive vehicle including a separator separating the positive electrode and the negative electrode and supporting a hybrid (HEV) mode, wherein in the hybrid mode, while the secondary battery is being charged, A sensor for measuring a dynamic voltage of the secondary battery; And identify the dynamic voltage profile of the secondary battery as a transition interval voltage pattern, calculate a parameter of the transition interval voltage pattern, and calculate the secondary battery from the calculated parameter using a predefined correlation between the parameter and the state of charge. It may include a control unit for estimating the state of charge of.
- control unit alternatively, calculates an inflection point identifier from the measured dynamic voltage, and if the inflection point identifier satisfies an inflection point generation condition, determines a parameter corresponding to the transition period voltage pattern and The state of charge of the secondary battery may be estimated from the calculated parameter using a predefined correlation between the parameter and the state of charge of the secondary battery.
- control unit may estimate the state of charge in each charge cycle.
- the charging may be charging in which pulse charging is repeated at time intervals.
- the control unit may estimate the state of charge of the secondary battery whenever the pulse charging is repeated.
- the control unit may estimate the state of charge of the secondary battery whenever the dynamic voltage profile is identified by the transition period voltage pattern during each pulse charging.
- An apparatus for estimating the state of charge of a secondary battery includes a cathode including a cathode material and a cathode material including a mixed cathode material including a first cathode material and a second cathode material having different operating voltage ranges. And a separator separating the positive electrode and the negative electrode and estimating a state of charge of a secondary battery mounted in an electric drive vehicle supporting an electric drive (EV) mode, wherein the secondary battery is charged in the electric drive mode.
- EV electric drive
- the sensor for measuring the dynamic voltage of the secondary battery While, the sensor for measuring the dynamic voltage of the secondary battery; And identify the dynamic voltage profile of the secondary battery as a transition interval voltage pattern, calculate a parameter of the transition interval voltage pattern, and calculate the secondary battery from the calculated parameter using a predefined correlation between the parameter and the state of charge. It may include a control unit for estimating the state of charge of.
- control unit alternatively, calculates an inflection point identifier from the measured dynamic voltage, and if the inflection point identifier satisfies an inflection point generation condition, determines a parameter corresponding to the transition period voltage pattern and The state of charge of the secondary battery may be estimated from the calculated parameter using a predefined correlation between the parameter and the state of charge of the secondary battery.
- a method of estimating a state of charge of a secondary battery includes: a cathode including a cathode material and a cathode material including a mixed cathode material including a first cathode material and a second cathode material having different operating voltage ranges; And a separator for separating the positive electrode and the negative electrode, the method comprising: (a) measuring a dynamic voltage of the secondary battery while the secondary battery is being charged; (b) identifying the dynamic voltage profile of the secondary battery as a transition period voltage pattern; (c) calculating a parameter of the identified transition period voltage pattern; And (d) estimating the state of charge of the secondary battery from the calculated parameter using a predefined correlation between the parameter and the state of charge.
- the steps (b) to (d) comprise: calculating an inflection point identifier from the measured dynamic voltage; Determining a parameter corresponding to a transition period voltage pattern if the inflection point identifier satisfies an inflection point occurrence condition; And estimating the state of charge of the secondary battery from the determined parameter using a predefined correlation between the parameter and state of charge.
- a method of estimating a state of charge of a secondary battery includes: a cathode including a cathode material and a cathode material including a mixed cathode material including a first cathode material and a second cathode material having different operating voltage ranges; And a separator for separating the positive electrode and the negative electrode and estimating a state of charge of a secondary battery mounted in an electric drive vehicle supporting hybrid (HEV) mode, wherein the charging of the secondary battery is performed in the hybrid mode.
- HEV electric drive vehicle supporting hybrid
- the steps (c) to (e) comprise: calculating an inflection point identifier from the measured dynamic voltage; Determining a parameter corresponding to a transition period voltage pattern if the inflection point identifier satisfies an inflection point occurrence condition; And estimating the state of charge of the secondary battery from the determined parameter using a predefined correlation between the parameter and state of charge.
- the charging state estimation method according to the present application may further include repeating the charging and discharging cycles of the secondary battery in the hybrid mode. In each of the charging cycles, the steps (b) to (e) are repeated. can do.
- the charging may be charging in which pulse charging is repeated at a time interval.
- steps (b) to (e) may be repeated whenever the pulse charging is repeated.
- steps (b) to (e) may be repeated when the dynamic voltage profile is identified by the transition period voltage pattern during each pulse charging.
- the method of estimating charge state according to the present application may include displaying the estimated charge state in a graphic interface, and / or storing the estimated charge state, and / or outputting the estimated charge state to the outside. It may include.
- Apparatus and method for estimating the state of charge of a secondary battery according to the present application are applicable to estimating the state of charge of a secondary battery mounted on various kinds of electric drive devices capable of operating with electrical energy.
- the electric drive device may be a mobile computer device such as a mobile phone, a laptop computer, a tablet computer, or a handheld multimedia device including a digital camera, a video camera, an audio / video playback device, and the like.
- a mobile computer device such as a mobile phone, a laptop computer, a tablet computer, or a handheld multimedia device including a digital camera, a video camera, an audio / video playback device, and the like.
- the electric drive device may be an electric power device capable of being moved by electricity, such as an electric car, a hybrid car, an electric bicycle, an electric motorcycle, an electric train, an electric boat, an electric plane, or an electric drill, an electric grinder, or the like. It can be a power tool with a motor as well.
- the electric drive device a large-capacity power storage device installed in the power grid to store renewable energy or surplus power generation, or various information including a server computer or mobile communication equipment in an emergency situation, such as a power outage It may be an uninterruptible power supply for supplying power to a communication device.
- the state of charge of the secondary battery may be reliably estimated. Therefore, as the electric driving vehicle equipped with the secondary battery operates in the hybrid mode, it is possible to solve the problem that the estimation error of the state of charge continues to increase even when the secondary battery repeats charging and discharging.
- the state of charge can be reliably estimated even in the state of charge in which the unusual voltage change behavior occurs
- branding of various combinations of cathode materials that could not be branded due to the unusual voltage change behavior is possible. Therefore, by selecting and branding two or more positive electrode materials in various combinations according to the purpose of using the secondary battery among various kinds of available positive electrode materials, it is possible to provide a mixed positive electrode material optimized for the purpose of using the secondary battery.
- FIG. 1 is a graph illustrating dQ / dV distribution of a lithium secondary battery including Li [Ni 1/3 Mn 1/3 Co 1/3 ] O 2 (NMC cathode material) and LiFePO 4 (LFP cathode material).
- FIG. 2 is a graph illustrating a discharge resistance profile of a lithium secondary battery including an NMC cathode material and an LFP cathode material.
- FIG 3 is a graph illustrating an open voltage profile of a lithium secondary battery including an NMC cathode material and an LFP cathode material.
- Figure 4 shows the half-cell using the NMC positive electrode and lithium metal as a positive electrode and a negative electrode, and a half-cell using the LFP positive electrode and lithium metal as a positive electrode and a negative electrode, respectively, the voltage change profile for each state of charge of each half cell It is a graph which measured and showed the result.
- FIG. 5 is a conceptual diagram illustrating a method in which the HEV mode is applied to an electric driving vehicle in which the HEV mode is supported.
- FIG. 6 is a graph illustrating a state of charge change of a secondary battery in the EV mode of FIG. 5.
- FIG. 7 is a graph illustrating a change in state of charge of a secondary battery in the HEV mode of FIG. 5.
- FIG. 8 shows an open voltage profile for four lithium secondary batteries containing a mixed cathode material in which the NMC cathode material and the LFP cathode material are branded at 7: 3 (weight ratio) and having different charge and discharge counts (ie, different aging degrees).
- This graph shows the state of charge and the state of charge applied to the EV mode and HEV mode on the horizontal axis.
- FIG. 9 is a graph showing how the dynamic voltage and state of charge of a battery change when pulsed charge is performed in a transition period of a lithium secondary battery including a mixed cathode material in which an NMC cathode material and an LFP cathode material are 7: 3 (weight ratio). to be.
- FIG. 10 is a block diagram schematically illustrating a configuration of an apparatus for estimating a state of charge of a secondary battery including a mixed cathode material according to an exemplary embodiment of the present application.
- FIG. 11 is a flowchart illustrating a method of estimating a state of charge of a secondary battery including a mixed cathode material according to an exemplary embodiment of the present application.
- the lithium secondary battery is a generic term for a secondary battery in which lithium ions act as operating ions during charging and discharging to induce an electrochemical reaction in the positive electrode and the negative electrode.
- the working ions refer to ions participating in the electrochemical oxidation and reduction reaction while the secondary battery is being charged or discharged, for example lithium. Therefore, even if the name of the secondary battery is changed according to the type of electrolyte or separator used in the lithium secondary battery, the type of packaging material used to package the secondary battery, or the internal or external structure of the lithium secondary battery, lithium ions are used as working ions. All secondary batteries should be interpreted as being included in the category of the lithium secondary battery.
- the present application can be applied to secondary batteries other than the lithium secondary battery. Therefore, even if the operating ion is not a lithium ion, any secondary battery to which the technical spirit of the present application can be applied should be interpreted as being included in the scope of the present application regardless of its type.
- secondary batteries are not limited by the number of elements which comprise it.
- secondary batteries may include a single cell based on a negative electrode, an electrolyte, and a positive electrode, an assembly of a single cell, a module in which a plurality of assemblies are connected in series and / or in parallel, a pack in which a plurality of modules are connected in series and / or in parallel, Should be interpreted to include battery systems connected in series and / or in parallel.
- the positive electrode of the secondary battery in which the state of charge is estimated contains a mixed positive electrode material.
- the mixed cathode material includes at least a first cathode material and a second cathode material, wherein the first and second cathode materials have different operating voltage ranges.
- the concentration of the operating ions reacting with the first positive electrode material and the concentration of the operating ions reacting with the second positive electrode material vary depending on the dynamic voltage change of the secondary battery while the secondary battery is being charged or discharged.
- the dynamic voltage means a voltage measured while the secondary battery is being charged or discharged.
- the working ions refer to ions which electrochemically react with the first and second cathode materials in the process of charging or discharging the secondary battery. When the secondary battery is a lithium secondary battery, lithium ions correspond to the operating ions.
- the reaction refers to an electrochemical reaction including oxidation and reduction reactions of the first and second cathode materials involved in the charging or discharging of the secondary battery, and may vary according to an operation mechanism of the secondary battery.
- the electrochemical reaction may mean that operating ions are inserted into the first cathode material and / or the second cathode material or vice versa from the inside.
- the concentration of operating ions inserted into the first and second cathode materials or the concentration of operating ions detached from the first and second cathode materials may vary as the dynamic voltage of the secondary battery changes.
- operating ions may be preferentially inserted into the first cathode material in a certain voltage band, and vice versa in another voltage band.
- operating ions may be preferentially desorbed from the second cathode material in one voltage band under the condition that the secondary battery is charged, and vice versa in another voltage band.
- the first and second cathode materials are subjected to the following conditions: At least one of them.
- the first and second positive electrode materials may show a difference in the position of the main peak and / or the intensity of the main peak when the dQ / dV distribution is measured.
- the dQ / dV distribution means the capacity characteristics of the operating ions for the cathode material by voltage.
- the position and / or intensity difference with respect to the main peak may vary depending on the type of the first and second cathode materials.
- NMC cathode material Li [Ni 1/3 Mn 1/3 Co 1/3 ] O 2
- LFP cathode material LiFePO 4
- the peak on the left corresponds to the main peak of the LFP cathode material
- the peak on the right corresponds to the main peak of the NMC cathode material.
- the LFP cathode material and the LFP cathode material correspond to the position of the main peak and / or the intensity of the main peak. Is different from each other.
- the profile displayed around the main peak of the LFP cathode material is the reaction between the LFP cathode material and the lithium ions
- the profile displayed around the main peak of the NMC cathode material is caused by the reaction of the NMC cathode material and the lithium ions.
- the LFP cathode material mainly reacts with lithium ions
- the NMC cathode material mainly reacts with lithium ions.
- the discharge resistance is measured for each secondary battery including the mixed positive electrode material by charging state.
- the resistance profile may have a Convex pattern (so-called convex shape), or the discharge resistance profile may have at least two inflection points before and after the apex of the Convex pattern.
- SOC state of charge
- the discharge resistance profile of the lithium secondary battery including the mixed cathode material has a convex pattern when the SOC is in a range of about 20 to 40%.
- an inflection point (a portion indicated by a dotted circle) occurs twice when the SOC is in the range of 20 to 30% and in the range of 30 to 40%. It has already been described with reference to FIG. 1 that the concentration of operating ions reacting with the NMC cathode material and the LFP cathode material depends on the dynamic voltage change of the secondary battery.
- the concentration of operating ions reacting with the first and second cathode materials varies depending on the dynamic voltage of the secondary battery
- at least one voltage flat region in the open voltage profile of the secondary battery including the mixed cathode material plateaus may occur.
- the voltage flat region refers to a region in which the bending of the voltage profile changes around the inflection point while the inflection point exists.
- FIG. 3 shows an open voltage for each SOC while discharging a lithium secondary battery including a mixed cathode material in which a NMC cathode material and an LFP cathode material are blended with a 7: 3 (weight ratio) in a cathode, and a carbon material in a cathode. It is an open-voltage profile showing the result of the measurement.
- the open voltage means a voltage measured when the secondary battery is in a no-load state for a predetermined time and stabilized, and the voltage of the secondary battery is stabilized, and a voltage having a different concept from a dynamic voltage measured when the secondary battery is charged or discharged to be.
- a voltage flat region occurs in the open voltage profile when the open voltage is about 3.2V. It has already been described with reference to FIG. 1 that the concentration of operating ions reacting with the NMC cathode material and the LFP cathode material depends on the dynamic voltage change of the secondary battery. Therefore, even when the open voltage profile of the lithium secondary battery including the first and second positive electrode materials has at least one voltage flat region, the concentration of operating ions reacting with the first and second positive electrode materials is dependent on the dynamic voltage change of the secondary battery. It will be appreciated that the operating voltage ranges of the first and second cathode materials will vary accordingly.
- the voltage flat region is generated in the open voltage profile illustrated in FIG. 3 because the type of the cathode material mainly reacting with the operating ions is changed in the charging state section corresponding to the voltage flat band.
- the mixed cathode material includes an NMC cathode material and an LFP cathode material
- the LFP cathode material reacts mainly with the working ions and the high voltage band (approximately 3.2V or more).
- NMC cathodes react mainly with working ions.
- NMC cathode material and LFP cathode material have different reaction kinetics (kinetics) from the working ions, the dominant reaction kinetics or change is changed when the type of cathode material mainly reacts with the working ions. Therefore, when the open voltage profile of the secondary battery including the mixed cathode material is analyzed, a voltage flat region including an inflection point is observed as shown in FIG. 3. On the other hand, if a voltage flat region occurs in the open voltage profile, a voltage flat region occurs in the dynamic voltage profile. Although the dynamic voltage differs from the open voltage due to the voltage component due to the IR effect or the polarization effect, the change pattern of the dynamic voltage is similar to the change pattern of the open voltage.
- the concentration of operating ions reacting with the first and second positive electrode materials is dependent on the dynamic voltage of the secondary battery. It may show a difference.
- Figure 4 shows the half-cell using the NMC positive electrode and lithium metal as a positive electrode and a negative electrode, and a half-cell using the LFP positive electrode and lithium metal as a positive electrode and a negative electrode, respectively, the voltage change profile for each state of charge of each half cell It is a graph which measured and showed the result.
- graph 1 is a voltage profile of a half cell containing an NMC cathode material
- graph 2 is a voltage profile of a half cell containing an LFP cathode material.
- the materials that can be used as the first and second cathode materials are not particularly limited in kind. Therefore, in addition to the NMC cathode material and the LFP cathode material, a combination of cathode materials satisfying at least one or more of the above-described conditions may be considered as the first and second cathode materials.
- the first cathode material the general formula A [A x M y ] O 2 + z
- A includes at least one element of Li, Na and K; M is Ni, Co, Mn, Ca, At least one element selected from Mg, Al, Ti, Si, Fe, Mo, V, Zr, Zn, Cu, Al, Mo, Sc, Zr, Ru, and Cr; x ⁇ 0, 1 ⁇ x + y ⁇ 2, -0.1 ⁇ z ⁇ 2; the stoichiometric coefficients of the components included in x, y, z, and M may be alkali metal compounds represented by).
- the first cathode material comprises at least one alkali metal compound xLiM 1 O 2- (1-x) Li 2 M 2 O 3 (M 1 has an average oxidation state of 3) disclosed in US 6,677,082, US 6,680,143 and the like.
- the second cathode material is a general formula Li a M 1 x Fe 1-x M 2 y P 1-y M 3 z O 4-z
- M 1 is Ti, Si, Mn, Co, Fe, At least one element selected from V, Cr, Mo, Ni, Nd, Al, Mg, and Al
- M 2 is Ti, Si, Mn, Co, Fe, V, Cr, Mo, Ni, Nd, Al, Mg
- M 3 includes a halogenated element optionally comprising F; 0 ⁇ a ⁇ 2, 0 ⁇ x ⁇ 1, 0 ⁇ y ⁇ 1, 0 ⁇ z ⁇ 1; the stoichiometric coefficients of the components included in a, x, y, z, M 1 , M 2 , and M 3 are selected so that the compound maintains electrical neutrality, or Li 3 Number of lithium metal phosphates represented by M 2 (PO 4 ) 3 [
- the second positive electrode material may be at least one selected from the group consisting of LiFePO 4 , LiMn x Fe y PO 4 (0 ⁇ x + y ⁇ 1), and Li 3 Fe 2 (PO 4 ) 3 .
- the first positive electrode material and / or the second positive electrode material may include a coating layer.
- the coating layer comprises a carbon layer, or in the group consisting of Ti, Si, Mn, Co, Fe, V, Cr, Mo, Ni, Nd, Al, Mg, Al, As, Sb, Si, Ge, V and S It may include an oxide layer or a fluoride layer containing at least one element selected.
- the mixing ratio of the first and second cathode materials may be appropriately adjusted in consideration of electrochemical design conditions considering the use of the secondary battery to be manufactured.
- a cathode material having a fast reaction rate with lithium ions may be selected as one of the first and second cathode materials, and the mixing ratio of the cathode material may be set as large as possible.
- Li [Ni 1/3 Mn 1/3 Co 1/3 ] O 2 and LiFePO 4 are selected as the first cathode material and the second cathode material, respectively, and the mixing ratio of the first cathode material and the second cathode material is Can be set to 9: 1.
- a cathode material having excellent high temperature safety may be selected as one of the first and second cathode materials, and the mixing ratio of the cathode material may be set as large as possible.
- Li [Ni 1/3 Mn 1/3 Co 1/3 ] O 2 and LiFePO 4 are selected as the first cathode material and the second cathode material, respectively, and the mixing ratio of the first cathode material and the second cathode material is Can be set to 2: 8.
- a cathode material having a low cost of materials may be selected as one of the first and second cathode materials, and the mixing ratio of the cathode material may be set as large as possible.
- Li [Ni 1/3 Mn 1/3 Co 1/3 ] O 2 and LiFePO 4 are selected as the first cathode material and the second cathode material, respectively, and the mixing ratio of the first cathode material and the second cathode material is Can be set to 1: 9.
- a positive electrode material having a high reaction rate with operating ions and a positive electrode material having high temperature safety are selected as the first and second positive electrode materials, respectively.
- the mixing ratio of the cathode materials may be set in consideration of the discharge output and the degree of balancing of the high temperature safety. For example, Li [Ni 1/3 Mn 1/3 Co 1/3 ] O 2 and LiFePO 4 are selected as the first cathode material and the second cathode material, respectively, and the mixing ratio of the first cathode material and the second cathode material is Can be set to 4: 6.
- a positive electrode material having a large capacity per weight may be selected as one of the first and second positive electrode materials and a large mixing ratio of the positive electrode material may be set.
- Li [Ni 0.5 Mn 0.3 Co 0.2 ] O 2 and LiFePO 4 may be selected as the first positive electrode material and the second positive electrode material, respectively, and the mixing ratio of the first positive electrode material and the second positive electrode material may be set to 9: 1. have.
- first and second cathode materials selection of the first and second cathode materials and the adjustment method of the mixing ratio are merely examples. Therefore, it will be apparent to those skilled in the art that the first and second cathode materials can be appropriately selected according to the design conditions of the secondary battery, and the mixing ratio of each cathode material can be appropriately set.
- the number of cathode materials that may be included in the mixed cathode material is not limited to two.
- other additives such as a conductive agent, a binder, and the like are not particularly limited.
- the secondary battery including the mixed cathode material may be mounted on various kinds of electric driving apparatuses capable of operating with electrical energy, and the electric driving apparatus is not particularly limited in its kind.
- the electric drive device may be a mobile computer device such as a mobile phone, a laptop computer, a tablet computer, or a handheld multimedia device including a digital camera, a video camera, an audio / video playback device, and the like.
- a mobile computer device such as a mobile phone, a laptop computer, a tablet computer, or a handheld multimedia device including a digital camera, a video camera, an audio / video playback device, and the like.
- the electric drive device may be an electric power device capable of being moved by electricity, such as an electric car, a hybrid car, an electric bicycle, an electric motorcycle, an electric train, an electric boat, an electric plane, or an electric drill, an electric grinder, or the like. It can be a power tool with a motor as well.
- the electric drive device a large-capacity power storage device installed in the power grid to store renewable energy or surplus power generation, or various information including a server computer or mobile communication equipment in an emergency situation, such as a power outage It may be an uninterruptible power supply for supplying power to a communication device.
- the open voltage profile of the secondary battery including the mixed cathode material includes an inflection point and a curvature is changed around the inflection point.
- the reason why the curvature is changed is that the type of cathode material mainly reacts with the working ions. Therefore, near the inflection point, the rate of change ( ⁇ SOC / ⁇ OCV) of the state of charge relative to the open voltage increases.
- the charging state section in which the bending of the open voltage profile is switched around the inflection point will be referred to as a transition section.
- the transition section may vary according to the type and branding ratio of the cathode material included in the blended cathode material, and in the open voltage profile illustrated in FIG. 3, the state of charge corresponding to the voltage flat region (the dotted box portion) is the transition section. May correspond to.
- the state of charge of a secondary battery can be estimated to be intrinsic by the open voltage.
- the open circuit voltage can be accurately measured when the secondary battery has been in a no-load state for a certain time.
- the open circuit voltage is estimated using the dynamic voltage of the secondary battery.
- the dynamic voltage has an error with the open voltage due to the IR effect and the polarization effect, and the error is further amplified in the transition region near the inflection point because the variation of the dynamic voltage increases with the change of the charging state.
- the dynamic voltage shows an error with the open voltage but shows a change pattern similar to the open voltage
- the dynamic voltage also increases in the amount of change in the dynamic voltage compared to the state of charge in the transition period. Therefore, when the charging state is calculated by estimating the open voltage from the dynamic voltage in the transition section, reliability is inevitably deteriorated.
- the secondary battery including the mixed cathode material has a large change rate of the dynamic voltage with respect to the state of charge in the transition section (particularly near the inflection point), so it is difficult to accurately estimate the state of charge in the transition section.
- the state of charge is a factor that determines the distance that can be driven forward. Therefore, failing to accurately estimate the state of charge does not provide the driver with the exact distance traveled, giving confidence in the car.
- the above-mentioned problem becomes more problematic in electric drive vehicles supporting hybrid mode.
- the hybrid mode is a mode in which driving using an engine and driving using a secondary battery are performed in parallel, and may be applied when the state of charge of the secondary battery is low, when continuous driving is possible at an economical speed, or by a driver's choice.
- FIG. 5 is a conceptual diagram illustrating a method of applying a hybrid mode in a low charging state section
- FIG. 6 is a graph illustrating a change in state of charge of a secondary battery in the EV mode of FIG. 5
- FIG. 7 is a secondary view in the HEV mode of FIG. 5.
- the electric driving vehicle supporting the hybrid mode is driven in the EV mode in a section in which the state of charge of the secondary battery is high (SOC min_EV to SOC max_EV ).
- SOC min_EV to SOC max_EV the state of charge of the secondary battery
- charging status of the secondary battery it is gradually reduced from SOC to the SOC max_EV min_EV as shown in FIG.
- SOC min_EV the state of charge of the secondary battery
- the HEV mode is applied from this point because only the secondary battery can achieve the desired output.
- the engine When the HEV mode is started, the engine is driven by an electric drive car. At this time, the secondary battery is charged by the generator coupled to the engine. Therefore, the state of charge of the secondary battery starts to increase.
- the secondary battery continues to be charged and the state of charge reaches SOC max_HEV , the secondary battery can be used again, so that the use of the engine is stopped and the secondary battery is discharged again. Then, the state of charge of the secondary battery starts to decrease again, and when the state of charge decreases to SOC min_HEV , the use of the secondary battery is stopped again and the use of the engine is started.
- the state of charge of the secondary battery changes periodically in the range of SOC min_HEV to SOC max_HEV as shown in FIG. 7.
- the state of charge indicated by hatching in FIG. 5 is a state of charge not used to prevent overcharge and overdischarge of the secondary battery.
- the state of charge to which the HEV mode is applied may unfortunately belong to the transition period of the mixed cathode material.
- the transition section is a section in which it is difficult to accurately estimate the state of charge of the secondary battery. Therefore, when the HEV mode is applied in the transition period and the charging state is estimated by using the dynamic voltage while the secondary battery is repeatedly charged and discharged, the error of the charged state accumulates over time, and the accuracy of the estimated state of charge decreases gradually. As a result, there arises a problem in that it is not possible to adequately control the use transition time of the engine and the secondary battery corresponding to the most important control elements of the HEV mode.
- FIG. 8 shows a mixed cathode material having a branded NMC cathode material and an LFP cathode material at 7: 3 (weight ratio) included in the cathode, and the carbon material included in the cathode, but the number of charge / discharge cycles (that is, the degree of aging) is different from each other. It is a graph showing the open voltage profile of the lithium secondary battery according to the state of charge and the state of charge in which the EV mode and the HEV mode are applied on the horizontal axis.
- FIG. 8 four open voltage profiles 1 to 4 are shown.
- the left side is an open voltage profile of a lithium secondary battery with a greater number of charge / discharge cycles, and the rightmost profile 1 is BOL (Beginning). Open voltage profile of a lithium secondary battery in a state of life.
- each open voltage profile has an area (dotted rectangle) in which curvature changes about an inflection point, and the charging state section of the area is an estimation of the state of charge. This is a difficult transition period.
- HEV1 and HEV2 sections In the horizontal axis of the graph shown in FIG. 8, two charge state sections HEV1 and HEV2 sections to which the HEV mode is applied are displayed.
- the HEV1 section is a HEV mode application section of the lithium secondary battery in the BOL state.
- the HEV2 section is a HEV mode application section of the lithium secondary battery having the open voltage profile 4.
- the reason why the HEV2 section is shifted to the left is that the capacity of the battery is reduced by the aging effect.
- the movement of the HEV2 section is proportional to the movement of the open voltage profile 4.
- the HEV1 and HEV2 sections may overlap the transition section, which is difficult to estimate the state of charge.
- the application section of the HEV mode should be moved to the intermediate charging state section.
- the energy efficiency is inferior, which means that the HEV mode is not used to drive an electric drive car.
- the charging state section to which the HEV mode is applied may overlap with the transition period.
- the inventor of the present application when the secondary battery is charged in the transition period of the secondary battery including the mixed positive electrode material, the dynamic voltage of the secondary battery shows a voltage change pattern including the inflection point, the shape of the voltage change pattern is in the state of charge It is confirmed that it depends. In addition, the inventors of the present application confirmed that a 1: 1 correspondence is established between a parameter capable of specifying the shape of the voltage change pattern and the state of charge.
- FIG. 9 illustrates a dynamic voltage of a battery when pulsed charging is performed in a transition period of a lithium secondary battery including a mixed cathode material in which a NMC cathode material and an LFP cathode material are 7: 3 (weight ratio) in a cathode, and a carbon material in a cathode.
- the graph shows how the state of charge changes.
- the state of charge increases linearly while pulse charging is performed.
- the profile of the dynamic voltage includes an inflection point, and the bend is changed from concave to convex shape around the inflection point. Therefore, at the inflection point, dV / dt becomes the maximum value, and before the inflection point, dV / dt tends to increase gradually. On the contrary, after the inflection point, dV / dt gradually decreases from the maximum value.
- the pattern of the dynamic voltage including the inflection point and the bending change around the inflection point will be referred to as a transition section voltage pattern.
- the shape of the transition period voltage pattern may be uniquely specified using at least one or more parameters. That is, the transition period voltage pattern may have an inflection point based on the charging start voltage V initial at which the increase of the voltage begins, the charge end voltage V final at which the increase of the voltage is finished, and the time at which the increase of the voltage is started.
- the transition period voltage pattern is defined in a time period ( ⁇ T) in which the dynamic voltage of the battery is changed from the charge start voltage to the charge end voltage, a broad integral value S1 of the entire transition period voltage pattern, and a constant time range before and after the inflection point. It may be specified by at least one parameter selected from the group consisting of integrated local integration values S2.
- the parameter depends on the state of charge of the secondary battery. Therefore, when the transition section voltage pattern is detected while the secondary battery is pulse-charged, the state of the secondary battery may be estimated by calculating the parameter for the detected transition section voltage pattern. As an example, the state of charge may be estimated by calculating the time ⁇ until the inflection point appears and the dV / dt value at the inflection point based on the time point at which the voltage increase is started from the transition period voltage pattern. In order to estimate the state of charge of the secondary battery using the parameter calculated from the transition period voltage pattern, a predefined correlation between the parameter and the state of charge is required.
- the predefined correlation may be a lookup table or a lookup function as a non-limiting example.
- the lookup table or the lookup function may be obtained through experiments. That is, an experimental condition capable of accurately measuring the state of charge of the secondary battery and enabling pulse charging is prepared. Then, the pulsed charge of the secondary battery to obtain an open voltage profile, and the transition period is identified by finding the state of charge section of the region where the bending is changed in the open voltage profile. Thereafter, the state of charge is gradually increased by pulse charging the secondary battery from the lower limit to the upper limit of the transition section. Pulse charging is performed under the same conditions as pulse charging applied in the HEV mode. That is, the current magnitude of the charging pulse and the application time of the charging pulse are made the same as those applied in the HEV mode.
- the transition section voltage pattern is measured and the state of charge before and after pulse charge is accurately measured. Then, at least one parameter is calculated for each transition period voltage pattern to collect data necessary to generate the lookup table or the lookup function.
- the collected data is then used to create a lookup table with a data structure that can reference the state of charge (state of charge before pulse charge or state of charge after pulse charge) from at least one or more parameters.
- a look-up function using one or more parameters as an input variable and a state of charge (a state of charge before pulse charging or a state of charge after pulse charging) as an output variable is derived through numerical analysis.
- the lookup table or the lookup function may be generated for each pulse charging current. This is because when the magnitude of the pulse charge current changes, the voltage pattern of the transition section also changes.
- the lookup table or the lookup function obtained through the above process may be used to accurately estimate the state of charge of the secondary battery including the mixed cathode material in the transition period. Therefore, hereinafter, an apparatus and method for estimating the state of charge of the secondary battery including the mixed cathode material using the lookup table or the lookup function will be described in more detail.
- FIG. 10 is a block diagram schematically illustrating a configuration of an apparatus for estimating a state of charge of a secondary battery including a mixed cathode material according to an exemplary embodiment of the present application.
- the apparatus 100 for estimating state of charge includes a sensor 120 and a control unit 130, and is electrically connected to a secondary battery 110 including a mixed cathode material. Estimate the state of charge in the transition period of
- the state of charge estimating apparatus 100 is electrically connected to the load 140.
- the load 140 is included in the above-described various electric driving apparatuses, and means an energy consuming apparatus included in the electric driving apparatus operated by electric energy supplied when the secondary battery 110 is discharged.
- the load may be a rotary power device such as a motor, a power converter such as an inverter, or the like as a non-limiting example, but the present application is not limited by the type of load.
- the state of charge estimating apparatus 100 may further optionally further include a storage unit 160.
- the storage unit 160 stores a lookup table or a lookup function obtained through experiments in advance. Since the lookup table or the lookup function have been described above, repetitive description thereof will be omitted.
- the lookup table or the lookup function may be stored in the storage unit 160 as part of binary data or program code.
- the storage unit 160 is not particularly limited as long as it is a storage medium capable of recording and erasing information.
- the storage unit 160 may be a RAM, a ROM, a register, a hard disk, an optical recording medium, or a magnetic recording medium.
- the storage unit 160 may also be connected with the control unit 130 via, for example, a data bus so as to be accessible by the control unit 130.
- the storage unit 160 also stores and / or updates and / or erases and / or programs containing various control logics performed by the control unit 130 and / or data generated when the control logic is executed. send.
- the storage unit 160 may be logically divided into two or more, and is not limited to being included in the control unit 130.
- the charging state estimating apparatus 100 may further optionally further include a display unit 150.
- the display unit 150 is not particularly limited as long as the display unit 150 can display the state of charge of the secondary battery 110 calculated by the control unit 130 using a graphic interface.
- the graphic interface refers to an interface that directly displays the state of charge of the secondary battery as a number or displays the state of charge at a relative level by using a graphic element such as a bar graph.
- the display unit 150 may be a liquid crystal display, an LED display, an OLED display, an E-INK display, a flexible display, or the like.
- the display unit 150 may be directly or indirectly connected to the control unit 130.
- the display unit 150 may be located in an area physically separated from the area in which the control unit 130 is located.
- a third control unit (not shown) is interposed between the display unit 150 and the control unit 130 so that the third control unit can express the display unit 150 from the control unit 130.
- the information may be provided and displayed on the display unit 150.
- the third control unit and the control unit 130 may be connected by a communication line.
- the sensor 120 repeatedly measures the dynamic voltage of the secondary battery 110 at intervals of time while the secondary battery 110 is being charged for a predetermined time and provides the measured dynamic voltage to the control unit 130.
- the predetermined time may be within several microseconds to several tens of seconds as an example.
- the charging may be pulse charging.
- pulse charging refers to charging in a manner in which a constant current is intermittently applied as a charging current.
- the charging may be charging performed in the HEV mode.
- the present application is not limited by the type of charging or the type of device to which the secondary battery 110 is applied.
- the sensor 120 optionally measures the current of the secondary battery 110 repeatedly at a time interval while the secondary battery 110 is being charged, and measures the current of the measured secondary battery 110 by a control unit ( 130, the control unit 130 may calculate the amount of change in the charging state using the ampere counting method while the charging is in progress.
- the control unit 130 executes at least one control logic necessary to estimate the state of charge of the secondary battery 110.
- the control logic may include logic for storing the dynamic voltage of the secondary battery 110 measured by the sensor 120 in the storage unit 160.
- the dynamic voltage is repeatedly measured at time intervals while the secondary battery 110 is being charged. Therefore, the plurality of voltage data stored in the storage unit 160 may constitute a dynamic voltage profile.
- the control logic may optionally include logic to store the current of the secondary battery 110 measured by the sensor 120 in the storage unit 160.
- the current of the secondary battery 110 may be repeatedly measured at time intervals while the secondary battery 110 is being charged. Therefore, the plurality of current data stored in the storage unit 160 constitutes a current profile.
- the control logic may also include logic to identify the dynamic voltage profile stored in the storage unit 160 as a transition period voltage pattern. The identification may be performed by determining whether an inflection point exists in the dynamic voltage profile, whether the dynamic voltage profile includes different bends, whether the first derivative of the dynamic voltage profile has a maximum value, or the like.
- the control logic also includes logic to calculate a parameter for the identified transition period voltage pattern.
- the parameter is a time required for the inflection point to appear on the basis of the charging start voltage V initial at which the increase of the voltage starts, the charge end voltage V final at which the increase of the voltage is finished, and the point at which the increase of the voltage is started. ( ⁇ ), dV / dt value at the inflection point, dV / dSOC at the inflection point (dSOC is obtained by calculating the capacity change per unit time using the ampere counting method), and the dynamic voltage of the secondary battery starts from the charge start voltage.
- a group consisting of a time ( ⁇ T) required to change to a voltage, a global integral value (S1) of the entire transition period voltage pattern, and a local integration value (S2) of integrating the transition period voltage pattern in a constant time range before and after the inflection point. It includes at least one selected from.
- the control logic also includes logic to estimate the state of charge of the secondary battery corresponding to the parameter calculated from the identified transition period voltage pattern using a lookup table or lookup function stored in the storage unit 160.
- the control logic may further include logic for selecting a lookup table or a lookup function to be used for estimating a charging state according to the magnitude of the charging current when the lookup table or the lookup function depends on the magnitude of the charging current. have.
- the selection logic may be omitted if the lookup table includes a data structure capable of mapping the state of charge using the magnitude of the charge current and the parameters simultaneously, or if the magnitude of the charge current is included as an input variable of the lookup function. Do.
- the control logic may include logic to estimate the state of charge by mapping a state of charge corresponding to the calculated parameter from a lookup table.
- the control logic may also include logic for estimating the state of charge by substituting the calculated parameter as an input value of a lookup function and obtaining the state of charge as an output value.
- the estimated charging state may be a charging state before charging is started or after charging is completed. If the estimated state of charge is a state of charge before charging is initiated, the control logic charge state by integrating the current profile stored in the storage unit 160 with an amp counting method while the secondary battery 110 is being charged. The method may include logic for estimating the state of charge after charging is completed by obtaining a change amount of.
- the control logic may further include logic for storing the estimated charge state in the storage unit 160 and / or logic for outputting the estimated charge state through the display unit 150 and / or the estimated charge state. It may further include logic to output to the other control device of the.
- the other control device may be a central computer device that electronically controls components mounted in a vehicle such as an engine when the secondary battery 110 is used in an electric drive vehicle.
- the control unit 130 may estimate the state of charge of the secondary battery 110 in each charge cycle by using the above-described control logic.
- the control unit 130 may estimate the state of charge of the secondary battery whenever the pulse charging is repeated using the above-described control logic.
- the control unit 130 may estimate the state of charge of the secondary battery only when the condition that the dynamic voltage profile is identified as the transition period voltage pattern is established during each pulse charging.
- the control unit 130 executes the above-described control logic when the dynamic voltage profile measured while the secondary battery is being charged is identified by the transition section voltage pattern regardless of the mode in which the electric driving vehicle is driven. The state of charge can be estimated.
- control unit 130 calculates the inflection point identifier from the dynamic voltage measured by the sensor 120, if the inflection point identifier satisfies the inflection point generation condition, the transition section voltage
- the parameter corresponding to the pattern may be determined, and the state of charge of the secondary battery may be estimated from the calculated parameter using a predefined correlation between the parameter and the state of charge of the secondary battery.
- the inflection point identifier may be updated each time a dynamic voltage is measured by the sensor 120.
- the inflection point identifier is used to determine in real time whether the coin voltage measured by the sensor 120 forms an inflection point over time.
- the inflection point identifier may be a first derivative value (dV / dt) of the dynamic voltage with respect to a measurement time of the dynamic voltage.
- the inflection point generation condition is a condition in which the first derivative value has a maximum value.
- the inflection point identifier may be a second derivative value (d 2 V / d 2 t) of the dynamic voltage with respect to the measurement time of the dynamic voltage.
- the inflection point generation condition is a condition that the second derivative value becomes zero.
- the inflection point identifier may be a first derivative value (dV / dSOC) of the dynamic voltage with respect to the state of charge of the secondary battery.
- the inflection point generation condition is a condition in which the first derivative value has a maximum value.
- the control unit 130 is configured to satisfy the inflection point generation condition from the charging start voltage V initial , the charging end voltage V final , and the charging start time.
- the time ( ⁇ T) required to change the dynamic voltage of the secondary battery from the charging start voltage to the charging end voltage, the voltage integration value from the charging start voltage to the charging end voltage, and the inflection point generation condition are satisfied.
- At least one selected from the group consisting of the integrated values of the measured dynamic voltages in a predetermined time range before and after the time point may be determined as a parameter corresponding to the transition period voltage pattern.
- control unit 130 may estimate the state of charge of the secondary battery from the determined parameter by using a lookup table that defines a corresponding relationship between the parameter and the state of charge.
- control unit 130 may estimate the state of charge of the secondary battery from the determined parameter using a lookup function that uses the parameter and the state of charge as input variables and output variables, respectively.
- control unit 130 estimates the state of charge of the secondary battery using the lookup table and the lookup function, the above description may be substantially the same.
- the control unit 130 selectively selects a processor, an application-specific integrated circuit (ASIC), another chipset, a logic circuit, a register, a communication modem, a data processing device, or the like, which are known in the art, to execute the various control logics described above. It may include.
- the control logic when the control logic is implemented in software, the control unit 130 may be implemented as a set of program modules.
- the program module may be stored in a memory and executed by a processor.
- the memory may be internal or external to the processor and may be coupled to the processor by a variety of known means.
- the memory may be included in the storage unit 160 of the present application.
- the memory refers to a device that stores information regardless of the type of device, and does not refer to a specific memory device.
- control unit 130 may be combined, and the combined control logics may be written in a computer readable code system and stored in a computer readable recording medium.
- the recording medium is not particularly limited as long as it is accessible by a processor included in the computer.
- the recording medium includes at least one selected from the group consisting of a ROM, a RAM, a register, a CD-ROM, a magnetic tape, a hard disk, a floppy disk, and an optical data recording device.
- the code system may be modulated into a carrier signal to be included in a communication carrier at a specific point in time, and may be distributed and stored and executed in a networked computer.
- functional programs, code and code segments for implementing the combined control logics can be easily inferred by programmers in the art to which this application belongs.
- FIG. 11 is a flowchart illustrating a method of estimating a state of charge of a secondary battery including a mixed cathode material according to an exemplary embodiment of the present application.
- control unit 130 measures the current of the secondary battery 110 using the sensor 120 at regular time intervals (S10).
- control unit 130 determines whether charging is started by referring to the current magnitude and the sign of the secondary battery 110 (S20). For reference, when the secondary battery 110 is being charged, the sign of the current becomes negative. On the contrary, when the secondary battery 110 is being discharged, the sign of the current is positive.
- control unit 130 When it is determined that charging is started, the control unit 130 initializes the time index to repeatedly measure the dynamic voltage of the secondary battery 110 and, optionally, the current (S30).
- control unit 130 measures the dynamic voltage and optionally the current of the secondary battery 110 using the sensor 120 and stores it in the storage unit 160 (S40).
- the control unit 130 determines whether the measurement period has elapsed (S50).
- the measurement period means a time period during which the dynamic voltage and optionally the current is repeatedly measured.
- control unit 130 measures the current of the secondary battery 110 through the sensor 120 to determine whether the charge is still maintained.
- control unit 130 updates the time index (S70). Then, the control unit 130 proceeds to the process S40 to control logic for measuring the dynamic voltage and optionally the current of the secondary battery 110 using the sensor 120 to store in the storage unit 160 Repeat again. Accordingly, the control unit 130 repeatedly measures the dynamic voltage and optionally the current of the secondary battery 110 by using the sensor 120 whenever the measurement period passes while the charging is maintained, thereby storing the storage unit 160. Repeat the control logic to save).
- control unit 130 executes control logic for estimating the state of charge of the secondary battery 110 using the dynamic voltage profile stored in the storage unit 160.
- control unit 130 reads the dynamic voltage profile stored in the storage unit 160 (S80). Then, the control unit 130 identifies whether the dynamic voltage profile corresponds to the transition period voltage pattern (S90).
- the identification may be performed by determining whether an inflection point exists in the dynamic voltage profile, whether the dynamic voltage profile includes different bends, whether the first derivative of the dynamic voltage profile has a maximum value, or the like.
- control unit 130 calculates a parameter for the identified transition period voltage pattern (S100).
- the parameter is a time required for the inflection point to appear on the basis of the charging start voltage V initial at which the increase of the voltage starts, the charge end voltage V final at which the increase of the voltage is finished, and the point at which the increase of the voltage is started.
- ( ⁇ ) dV / dt at the inflection point, dV / dSOC at the inflection point (dSOC is obtained by calculating the amount of change in capacity per unit time using the amperage counting method), and the dynamic voltage of the secondary battery is charged from the charge start voltage.
- control unit 130 estimates the state of charge of the secondary battery corresponding to the calculated parameter using a lookup table or a lookup function stored in the storage unit 160 (S110).
- control unit 130 When the lookup table or the lookup function depends on the magnitude of the charging current, the control unit 130 further executes logic to select a lookup table or a lookup function to use for estimation of the state of charge according to the magnitude of the charging current. Can be.
- the selection logic can be omitted if the lookup table includes a data structure that can be used to map the state of charge by using the magnitude of the charge current together with the parameters, or if the magnitude of the charge current is included as an input variable of the lookup function. Do.
- control unit 130 may estimate the state of charge by mapping the state of charge corresponding to the calculated parameter from the lookup table.
- control unit 130 calculates the time ⁇ until the inflection point appears from the identified transition period voltage pattern and the dV / dt value at the inflection point and
- the state of charge of the secondary battery 110 may be estimated by mapping the state of charge corresponding to two values calculated from the lookup table.
- control unit 130 may estimate the state of charge by substituting the calculated parameter as an input value of the lookup function to obtain a state of charge as an output value.
- control unit 130 calculates the time ⁇ until the inflection point appears from the identified transition period voltage pattern and the dV / dt value at the inflection point and
- the state of charge of the secondary battery 110 may be estimated by substituting the calculated two values into the lookup function as an input variable to obtain the state of charge as an output variable.
- the estimated state of charge is the state of charge before charge commences or after charge is complete.
- the control unit 130 accumulates the current profile stored in the storage unit 160 while the secondary battery 110 is being charged to calculate the change amount of the charge state.
- the charging state can be estimated after the completion of charging.
- control unit 130 outputs a logic for storing the estimated charge state in the storage unit 160 and / or the estimated charge state through the display unit 150 through a graphic interface.
- the logic and / or logic for outputting the estimated state of charge to another external control device may be further executed.
- control unit 130 when the method according to the present application is used for estimating the state of charge of the secondary battery mounted on the electric drive vehicle supporting the HEV mode, the control unit 130, the control logic for estimating the state of charge when the HEV mode is started You can run Of course, the control unit 130 may execute the above-described control logic regardless of whether the HEV mode is applied.
- the control unit 130 may receive information from the central computer device of the electric drive vehicle that the HEV mode has been started.
- the HEV mode may be automatically executed in a preset charging state range, automatically executed when the electric drive vehicle runs at an economically efficient engine speed, or may be forcibly executed by a driver in an electric drive vehicle. .
- the charging state estimation method may be preferably applied when the secondary battery is charged by pulse charging in the HEV mode. That is, when the secondary battery is pulse-charged for the first time after the HEV mode starts, the control unit 130 may estimate the state of charge of the secondary battery using the above-described control logic in the first pulse charge cycle. . It can also be run after the first pulse charge cycle. That is, each time the pulse charging is repeated, the execution of the above-described control logic is repeated to estimate the state of charge. The control unit The control unit 130 may update the most recently estimated state of charge of the secondary battery to the newly estimated state of charge. Obviously, the state of charge of the secondary battery most recently estimated is stored in the storage unit 160.
- control unit 130 may apply the following modified method in estimating the state of charge of the secondary battery.
- control unit 130 calculates an inflection point identifier whenever the dynamic voltage is measured by the sensor 120, and if the inflection point identifier satisfies the inflection point generation condition, the control unit 130 sets a parameter corresponding to the transition period voltage pattern. And a pre-defined correlation between the parameter and the state of charge of the secondary battery may be used to estimate the state of charge of the secondary battery from the calculated parameter.
- the charging state section in which the transition section voltage pattern is formed while the secondary battery is being charged that is, the transition section may be shifted to the left according to the capacity decay degree of the secondary battery.
- the capacity deterioration of the secondary battery may be defined as a relative ratio of the current capacity based on the capacity of the secondary battery in the BOL state, and the degree of capacity deterioration may be a method commonly used in the art to which the present application belongs.
- the degree of capacity degradation of the secondary battery is a non-limiting example, which is calculated by estimating the internal resistance of the secondary battery or quantitatively evaluating the degree to which the secondary battery's open voltage profile is shifted to the left based on the measured open voltage profile in the BOL state. Can be calculated.
- the scope of the present application is not limited by the manner of determining the capacity degradation of the secondary battery.
- the secondary battery may include a positive electrode including a mixed positive electrode material, a negative electrode including a negative electrode material, and a separator.
- the positive electrode may include a thin plate-shaped metal current collector made of a conductive material and a positive electrode material coating layer containing the mixed positive electrode material and coated on at least one surface of the metal current collector.
- the metal current collector is made of a material having high chemical stability and high conductivity.
- the metal current collector may be made of aluminum, stainless steel, nickel, titanium, calcined carbon, or the like.
- the metal current collector may be made of aluminum or stainless steel coated with carbon, nickel, titanium, silver, or the like on a surface thereof.
- the cathode material coating layer may further include additives such as a conductive agent and a binder in addition to the mixed cathode material.
- the conductive agent is not particularly limited as long as it is a material capable of improving the electrical conductivity of the mixed cathode material, but is not limited thereto. Carbon materials can be used.
- the binder is not particularly limited as long as it is a material which enables intimate physical bonding between the particles constituting the mixed cathode material and intimate interface bonding between the mixed cathode material and the metal current collector.
- vinylidene fluoride-hexafluoropropylene copolymer PVDF-co-HFP
- polyvinylidene fluoride polyvinylidenefluoride
- polyacrylonitrile polymethylmethacrylate
- Various kinds of polymers such as may be used as the binder.
- the negative electrode may include a thin plate-shaped metal current collector made of a conductive material, and a negative electrode material coating layer containing a negative electrode material and coated on at least one surface of the metal current collector.
- the metal current collector is made of a material having high chemical stability and high conductivity.
- the metal current collector may be made of copper, aluminum, stainless steel, nickel, titanium, calcined carbon, or the like.
- the metal current collector may be made of copper, stainless steel, or aluminum-cadmium alloy coated with carbon, nickel, titanium, silver, and the like on a surface thereof.
- the negative electrode material is not particularly limited as long as it has a different redox potential from the mixed positive electrode material, and the working ions are inserted in the charging process and desorb the working ions in the discharging process.
- a carbon material As a non-limiting example of the negative electrode material, a carbon material, a lithium metal, silicon, tin, or the like may be used, and metal oxides such as TiO 2 and SnO 2 having a potential of less than 2 V may be used.
- a carbon material may be used, and as the carbon material, both low crystalline carbon and high crystalline carbon may be used.
- Soft crystalline carbon and hard carbon are typical low crystalline carbon, and high crystalline carbon is natural graphite, artificial graphite, Kish graphite, pyrolytic carbon, liquid crystal pitch High temperature firing such as mesophase pitch based carbon fiber, meso-carbon microbeads, mesophase pitches, petroleum derived cokes, and tar pitch derived cokes Carbon is representative.
- the negative electrode material coating layer may further include additives such as a conductive agent and a binder in addition to the negative electrode material.
- additives such as a conductive agent and a binder in addition to the negative electrode material.
- a conductive agent and the binder a material which may be used as the conductive agent and the binder included in the cathode material coating layer may be used.
- the separator is not particularly limited as long as it has a pore structure for electrically separating the positive electrode and the negative electrode and mediating the movement of operating ions.
- the separator is a porous polymer film, for example, porous made of a polyolefin-based polymer such as ethylene homopolymer, propylene homopolymer, ethylene / butene copolymer, ethylene / hexene copolymer, ethylene / methacrylate copolymer, etc.
- the polymer films may be used alone or in combination of these.
- the separator may be a conventional porous nonwoven fabric, for example, a non-woven fabric made of high melting glass fibers, polyethylene terephthalate fibers, or the like.
- At least one surface of the separator may include a coating layer of inorganic particles. It is also possible that the separator itself consists of a coating layer of inorganic particles. Particles constituting the coating layer may have a structure combined with a binder such that an interstitial volume exists between adjacent particles. Such a structure is disclosed in PCT Publication WO / 2006/025662, which can be incorporated as part of the present specification.
- the inorganic particles may be made of an inorganic material having a dielectric constant of 5 or more.
- the inorganic particles may include Pb (Zr, Ti) O 3 (PZT), Pb 1-x La x Zr 1-y Ti y O 3 (PLZT), PB (Mg 3 Nb 2/3 ) O With 3 -PbTiO 3 (PMN-PT), BaTiO 3 , hafnia (HfO 2 ), SrTiO 3 , TiO 2 , Al 2 O 3 , ZrO 2 , SnO 2 , CeO 2 , MgO, CaO, ZnO and Y 2 O 3 It may include at least one material selected from the group consisting of.
- the secondary battery may further include an electrolyte containing operating ions.
- the electrolyte is not particularly limited as long as it can generate an electrochemical oxidation or reduction reaction at the anode and the cathode through the working ions, including the working ions.
- the electrolyte is A + B - It may be a salt having a structure such as.
- a + Li + , Na + , K + It includes ions consisting of alkali metal cations such as or a combination thereof.
- the electrolyte can also be used by dissolving in an organic solvent.
- organic solvent propylene carbonate (PC), ethylene carbonate (EC), diethyl carbonate (DEC), dimethyl carbonate (DMC), dipropyl carbonate (DPC) ), Dimethyl sulfoxide, acetonitrile, dimethoxyethane, diethoxyethane, tetrahydrofuran, N-methyl-2-pyrrolidone (N-methyl 2-pyrrolidone (NMP), ethyl methyl carbonate (EMC), gamma butyrolactone or mixtures thereof may be used.
- the secondary battery may further include a packaging material for sealing the positive electrode, the negative electrode and the separator.
- a packaging material for sealing the positive electrode, the negative electrode and the separator.
- the positive electrode and the negative electrode may be bonded to the positive electrode terminal and the negative electrode terminal, respectively, and the positive electrode terminal and the negative electrode terminal may be drawn out of the packing material.
- the packaging material functions as an electrode terminal
- any one of the positive electrode terminal and the negative electrode terminal may be replaced with the packaging material.
- the negative electrode is electrically connected to the inner surface of the packaging material, the outer surface of the packaging material may function as the negative electrode.
- the packaging material is not particularly limited as long as it is chemically safe, and as a non-limiting example, it may be made of a metal, a polymer, a flexible pouch film, or the like.
- the flexible pouch film may typically be an aluminum pouch film having a structure in which a heat seal layer, an aluminum layer, and an outer protective layer are stacked.
- the appearance of the secondary battery is determined by the structure of the packaging material.
- the structure of the packaging material can be adopted that used in the art, there is no particular limitation on the appearance according to the use of the battery.
- the outer shape of the packaging material may have a structure such as cylindrical, square, pouch type, coin type using a can.
- the secondary battery includes an electrode assembly in which a unit cell including at least a stack structure of a cathode, a separator, and a cathode is assembled.
- the unit cell may have various structures known in the art.
- the unit cell may have a bi-cell having the same polarity of the outermost electrode or a full cell structure in which the polarities of the outermost electrodes are opposite to each other.
- the bi-cell may have a structure of an anode, a separator, a cathode, a separator, and an anode.
- the full cell may have a structure of an anode, a separator, a cathode, a separator, an anode, a separator, and a cathode.
- the electrode assembly may have various structures known in the art.
- the electrode assembly may have a simple stack structure in which the unit cells and the separation film are repeatedly stacked while going from bottom to top.
- the electrode assembly may have a stack folding structure formed by arranging the unit cells at regular intervals on the separation film and then rolling the separation film together with the unit cells in a predetermined direction.
- the electrode assembly may have a jelly roll structure formed by placing a unit cell made in a sheet shape extending in one direction on a separation film and then rolling the unit cell and the separation film in a roll shape.
- components named 'units' should be understood as functionally distinct elements rather than physically distinct elements.
- each component may be selectively integrated with other components or each component may be divided into subcomponents for efficient execution of control logic (s).
- control logic control logic
- the integrated or divided components should also be interpreted as being within the scope of the present application, provided that the functional identity can be recognized even if the components are integrated or divided.
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Abstract
Description
Claims (59)
- 서로 다른 동작 전압 범위를 갖는 제1양극재 및 제2양극재를 포함하는 혼합 양극재가 포함되어 있는 양극, 음극재를 포함하는 음극 및 상기 양극과 음극을 분리시키는 분리막을 포함하는 이차 전지의 충전 상태를 추정하는 장치로서,상기 이차 전지가 충전되는 동안, 상기 이차 전지의 동적 전압을 측정하는 센서; 및상기 이차 전지의 동적 전압 프로파일을 전이구간 전압 패턴으로 식별하고, 상기 전이구간 전압 패턴의 파라미터를 계산하고, 상기 파라미터와 충전 상태 사이의 미리 정의된 상관 관계를 이용하여 상기 계산된 파라미터로부터 이차 전지의 충전 상태를 추정하는 제어 유닛을 포함하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항에 있어서,상기 제어 유닛은, 상기 동적 전압 프로파일에 변곡점이 존재하거나, 상기 동적 전압 프로파일이 서로 다른 굴곡을 포함하거나, 상기 동적 전압 프로파일의 일차 미분 값이 극대 값을 가지면, 상기 동적 전압 프로파일을 전이구간 전압 패턴으로 식별하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항에 있어서,상기 전이구간 전압 패턴은 적어도 하나의 변곡점을 포함하고,상기 계산된 파라미터는, 상기 식별된 전이구간 전압 패턴에서 전압의 증가가 시작되는 충전 개시 전압(Vinitial), 상기 식별된 전이구간 전압 패턴에서 전압의 증가가 마무리되는 충전 종료 전압(Vfinal), 상기 식별된 전이구간 전압 패턴에서 전압의 증가가 개시된 시점을 기준으로 상기 변곡점이 출현할 때까지 소요되는 시간(τ), 상기 변곡점에서의 dV/dt(V=동적 전압), 상기 변곡점에서의 dV/dSOC(V=동적 전압, SOC=충전 상태), 상기 이차 전지의 동적 전압이 상기 충전 개시 전압부터 상기 충전 종료 전압까지 변화하는데 소요된 시간(△T), 상기 식별된 전이구간 전압 패턴 전체의 광역 적분값 및 상기 변곡점 전후의 일정한 시간 범위에서 상기 전이구간 전압 패턴을 적분한 국소 적분값으로 이루어진 군에서 선택된 적어도 하나 이상을 포함하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항에 있어서,상기 미리 정의된 상관 관계는, 상기 파라미터와 상기 충전 상태 사이의 대응 관계를 정의한 룩업 테이블인 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항에 있어서,상기 미리 정의된 상관 관계는, 상기 파라미터를 입력 변수로 하고, 상기 충전 상태를 출력 변수로 하는 룩업 함수인 것인, 이차 전지의 충전 상태 추정 장치.
- 제4항에 있어서,상기 룩업 테이블이 저장된 저장 유닛을 더 포함하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제5항에 있어서,상기 룩업 함수가 저장된 저장 유닛을 더 포함하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항에 있어서,상기 상관관계는 상기 동적 전압이 측정된 충전 조건과 동일한 충전 조건 하에서 미리 정의된 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항 또는 제8항에 있어서,상기 추정된 충전 상태는, 상기 충전이 시작되기 전의 충전 상태 또는 상기 충전이 완료된 후의 충전 상태인 것인, 이차 전지의 충전 상태 추정 장치.
- 제9항에 있어서,상기 센서는, 상기 충전이 이루어지는 동안, 상기 이차 전지의 전류를 측정하고,상기 제어 유닛은, 상기 충전이 시작되기 전의 충전 상태를 추정한 다음, 상기 측정된 전류를 적산하여 충전 상태 변화량을 계산하고 상기 추정된 충전 상태에 상기 충전 상태 변화량을 반영하여 상기 충전이 완료된 후의 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항에 있어서,상기 충전은, 시간 간격을 두고 반복되는 펄스 충전인 것인, 이차 전지의 충전 상태 추정 장치.
- 제11항에 있어서,상기 제어 유닛은 상기 펄스 충전이 반복될 때마다 상기 이차 전지의 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제11항에 있어서,상기 제어 유닛은, 각 펄스 충전이 진행되는 동안, 상기 센서를 통해 측정된 상기 동적 전압 프로파일이 상기 전이구간 전압 패턴으로 식별되는 조건이 성립될 때, 상기 이차 전지의 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항에 있어서,상기 추정된 충전 상태를 그래픽 인터페이스로 표시하는 표시 유닛을 더 포함하고,상기 제어 유닛은, 추정된 충전 상태를 상기 표시 유닛으로 출력하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항에 있어서,상기 추정된 충전 상태가 저장되는 저장 유닛을 더 포함하고,상기 제어 유닛은 상기 추정된 충전 상태를 상기 저장 유닛에 저장하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항에 있어서,상기 제어 유닛은, 상기 추정된 충전 상태를 외부로 출력하는 것인, 이차 전지의 충전 상태 추정 장치.
- 서로 다른 동작 전압 범위를 갖는 제1양극재 및 제2양극재를 포함하는 혼합 양극재가 포함되어 있는 양극, 음극재를 포함하는 음극 및 상기 양극과 음극을 분리시키는 분리막을 포함하는 이차 전지의 충전 상태를 추정하는 장치로서,상기 이차 전지가 충전되는 동안, 상기 이차 전지의 동적 전압을 측정하는 센서; 및상기 측정된 동적 전압으로부터 변곡점 식별자를 계산하고, 상기 변곡점 식별자가 변곡점 발생 조건을 충족하면, 전이구간 전압 패턴에 대응되는 파라미터를 결정하고, 상기 파라미터와 상기 이차 전지의 충전 상태 사이의 미리 정의된 상관 관계를 이용하여 상기 계산된 파라미터로부터 이차 전지의 충전 상태를 추정하는 제어 유닛을 포함하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제17항에 있어서,상기 변곡점 식별자는, 시간에 대한 상기 동적 전압의 일차 미분 값이고,상기 변곡점 발생 조건은, 상기 일차 미분 값이 최대 값이 되는 조건임을 특징으로 하는, 이차 전지의 충전 상태 추정 장치.
- 제17항에 있어서,상기 변곡점 식별자는, 시간에 대한 상기 동적 전압의 이차 미분 값이고, 상기 변곡점 발생 조건은, 상기 이차 미분 값이 0이 되는 조건임을 특징으로 하는, 이차 전지의 충전 상태 추정 장치.
- 제17항에 있어서,상기 변곡점 식별자는, 상기 이차 전지의 충전 상태에 대한 상기 동적 전압의 일차 미분 값이고,상기 변곡점 발생 조건은, 상기 일차 미분 값이 최대 값이 되는 조건임을 특징으로 하는, 이차 전지의 충전 상태 추정 장치.
- 제17항에 있어서,상기 결정된 파라미터는, 충전 개시 전압(Vinitial), 충전 종료 전압(Vfinal), 충전 개시 시점부터 변곡점 발생 조건이 충족될 때까지 소요된 시간(τ), 상기 변곡점 발생 조건이 충족될 때의 dV/dt(V=동적 전압), 상기 변곡점 발생 조건이 충족될 때의 dV/dSOC(V=동적 전압, SOC=충전 상태), 상기 이차 전지의 동적 전압이 상기 충전 개시 전압부터 상기 충전 종료 전압까지 변화하는데 소요된 시간(△T), 상기 충전 개시 전압부터 상기 충전 종료 전압까지의 광역 적분값, 및 상기 변곡점 발생 조건이 충족되는 시점 전후의 일정한 시간 범위에서 상기 측정된 동적 전압의 국소 적분값으로 이루어진 군에서 선택된 적어도 하나 이상을 포함하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제17항에 있어서,상기 제어 유닛은, 상기 동적 전압이 측정될 때마다 상기 변곡점 식별자를 갱신하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제17항에 있어서,상기 미리 정의된 상관 관계는, 상기 파라미터와 상기 충전 상태 사이의 대응 관계를 정의한 룩업 테이블인 것인, 이차 전지의 충전 상태 추정 장치.
- 제17항에 있어서,상기 미리 정의된 상관 관계는, 상기 파라미터를 입력 변수로 하고, 상기 충전 상태를 출력 변수로 하는 룩업 함수인 것인, 이차 전지의 충전 상태 추정 장치.
- 서로 다른 동작 전압 범위를 갖는 제1양극재 및 제2양극재를 포함하는 혼합 양극재가 포함되어 있는 양극, 음극재를 포함하는 음극 및 상기 양극과 음극을 분리시키는 분리막을 포함하고 하이브리드(HEV) 모드가 지원되는 전기 구동 자동차에 탑재된 이차 전지의 충전 상태를 추정하는 장치로서,상기 하이브리드 모드에서, 상기 이차 전지가 충전되는 동안, 상기 이차 전지의 동적 전압을 측정하는 센서; 및상기 이차 전지의 동적 전압 프로파일을 전이구간 전압 패턴으로 식별하고, 상기 전이구간 전압 패턴의 파라미터를 계산하고, 상기 파라미터와 충전 상태 사이의 미리 정의된 상관 관계를 이용하여 상기 계산된 파라미터로부터 이차 전지의 충전 상태를 추정하는 제어 유닛을 포함하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제25항에 있어서,상기 제어 유닛은, 상기 동적 전압 프로파일에 변곡점이 존재하거나, 상기 동적 전압 프로파일이 서로 다른 굴곡을 포함하거나, 상기 동적 전압 프로파일의 일차 미분 값이 극대 값을 가지면, 상기 동적 전압 프로파일을 전이구간 전압 패턴으로 식별하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제25항에 있어서,상기 전이구간 전압 패턴은 적어도 하나의 변곡점을 포함하고,상기 계산된 파라미터는, 상기 식별된 전이구간 전압 패턴에서 전압의 증가가 시작되는 충전 개시 전압(Vinitial), 상기 식별된 전이구간 전압 패턴에서 전압의 증가가 마무리되는 충전 종료 전압(Vfinal), 상기 식별된 전이구간 전압 패턴에서 전압의 증가가 개시된 시점을 기준으로 상기 변곡점이 출현할 때까지 소요되는 시간(τ), 상기 변곡점에서의 dV/dt(V=동적 전압), 상기 변곡점에서의 dV/dSOC(V=동적 전압, SOC=충전 상태), 상기 이차 전지의 동적 전압이 상기 충전 개시 전압부터 상기 충전 종료 전압까지 변화하는데 소요된 시간(△T), 상기 식별된 전이구간 전압 패턴 전체의 광역 적분값 및 상기 변곡점 전후의 일정한 시간 범위에서 상기 전이구간 전압 패턴을 적분한 국소 적분값으로 이루어진 군에서 선택된 적어도 하나 이상을 포함하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제25항에 있어서,상기 제어 유닛은, 상기 하이브리드 모드에서, 상기 이차 전지의 충전과 방전 사이클이 반복될 때, 각 충전 사이클에서 상기 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제25항 또는 제28항에 있어서,상기 충전은 시간 간격을 두고 펄스 충전이 반복되는 충전인 것인, 이차 전지의 충전 상태 추정 장치.
- 제29항에 있어서,상기 제어 유닛은 상기 펄스 충전이 반복될 때마다 상기 이차 전지의 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제29항에 있어서,상기 제어 유닛은, 각 펄스 충전이 진행되는 동안, 상기 센서를 통해 측정된 상기 동적 전압 프로파일이 상기 전이구간 전압 패턴으로 식별되는 조건이 성립될 때, 상기 이차 전지의 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제25항에 있어서,상기 미리 정의된 상관 관계는, 상기 파라미터와 상기 충전 상태 사이의 대응 관계를 정의한 룩업 테이블인 것인, 이차 전지의 충전 상태 추정 장치.
- 제25항에 있어서,상기 미리 정의된 상관 관계는, 상기 파라미터를 입력 변수로 하고, 상기 충전 상태를 출력 변수로 하는 룩업 함수인 것인, 이차 전지의 충전 상태 추정 장치.
- 서로 다른 동작 전압 범위를 갖는 제1양극재 및 제2양극재를 포함하는 혼합 양극재가 포함되어 있는 양극, 음극재를 포함하는 음극 및 상기 양극과 음극을 분리시키는 분리막을 포함하고 하이브리드(HEV) 모드가 지원되는 전기 구동 자동차에 탑재된 이차 전지의 충전 상태를 추정하는 장치로서,상기 하이브리드 모드에서, 상기 이차 전지가 충전되는 동안, 상기 이차 전지의 동적 전압을 측정하는 센서; 및상기 측정된 동적 전압으로부터 변곡점 식별자를 계산하고, 상기 변곡점 식별자가 변곡점 발생 조건을 충족하면, 전이구간 전압 패턴에 대응되는 파라미터를 결정하고, 상기 파라미터와 상기 이차 전지의 충전 상태 사이의 미리 정의된 상관 관계를 이용하여 상기 계산된 파라미터로부터 이차 전지의 충전 상태를 추정하는 제어 유닛을 포함하는 것인, 이차 전지의 충전 상태 추정 장치.
- 제1항 내지 제34항 중 어느 한 항에 따른 이차 전지의 충전 상태 추정 장치를 포함하는 전기 구동 장치.
- 서로 다른 동작 전압 범위를 갖는 제1양극재 및 제2양극재를 포함하는 혼합 양극재가 포함되어 있는 양극, 음극재를 포함하는 음극 및 상기 양극과 음극을 분리시키는 분리막을 포함하는 이차 전지의 충전 상태를 추정하는 방법으로서,(a) 상기 이차 전지가 충전되는 동안, 상기 이차 전지의 동적 전압을 측정하는 단계;(b) 상기 이차 전지의 동적 전압 프로파일을 전이구간 전압 패턴으로 식별하는 단계;(c) 상기 식별된 전이구간 전압 패턴의 파라미터를 계산하는 단계; 및(d) 상기 파라미터와 충전 상태 사이의 미리 정의된 상관 관계를 이용하여 상기 계산된 파라미터로부터 이차 전지의 충전 상태를 추정하는 단계를 포함하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항에 있어서, 상기 (b) 단계에서,상기 동적 전압 프로파일에 변곡점이 존재하거나, 상기 동적 전압 프로파일이 서로 다른 굴곡을 포함하거나, 상기 동적 전압 프로파일의 일차 미분 값이 극대 값을 가지면, 상기 동적 전압 프로파일을 전이구간 전압 패턴으로 식별하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제37항에 있어서, 상기 (c) 단계에서,상기 계산된 파라미터는, 상기 식별된 전이구간 전압 패턴에서 전압의 증가가 시작되는 충전 개시 전압(Vinitial), 상기 식별된 전이구간 전압 패턴에서 전압의 증가가 마무리되는 충전 종료 전압(Vfinal), 상기 식별된 전이구간 전압 패턴에서 전압의 증가가 개시된 시점을 기준으로 상기 변곡점이 출현할 때까지 소요되는 시간(τ), 상기 변곡점에서의 dV/dt값(V=동적 전압), 상기 변곡점에서의 dV/dSOC(V=동적 전압, SOC=충전 상태), 상기 이차 전지의 동적 전압이 상기 충전 개시 전압부터 상기 충전 종료 전압까지 변화하는데 소요된 시간(△T), 상기 식별된 전이구간 전압 패턴 전체의 광역 적분값 및 상기 변곡점 전후의 일정한 시간 범위에서 상기 전이구간 전압 패턴을 적분한 국소 적분값으로 이루어진 군에서 선택된 적어도 하나 이상을 포함하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항에 있어서, 상기 (d) 단계에서,상기 파라미터와 상기 충전 상태 사이의 대응 관계를 미리 정의한 룩업 테이블을 사용하여 이차 전지의 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항에 있어서,상기 파라미터를 입력 변수로 하고, 상기 충전 상태를 출력 변수로 하는 룩업 함수를 사용하여 이차 전지의 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항에 있어서,상기 상관관계는 상기 동적 전압이 측정된 충전 조건과 동일한 충전 조건 하에서 미리 정의된 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항 또는 제41항에 있어서, 상기 (d) 단계에서,상기 충전이 시작되기 전의 충전 상태 또는 상기 충전이 완료된 후의 이차 전지에 대한 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제42항에 있어서,상기 충전이 이루어지는 동안, 상기 이차 전지의 전류를 측정하는 단계를 더 포함하고,상기 (d) 단계에서, 상기 충전이 시작되기 전의 충전 상태를 추정한 다음, 상기 측정된 전류를 적산하여 충전 상태 변화량을 계산하고 상기 추정된 충전 상태에 상기 충전 상태 변화량을 반영하여 상기 충전이 완료된 후의 충전 상태를 추정하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항에 있어서,상기 충전은, 시간 간격을 두고 반복되는 펄스 충전인 것인, 이차 전지의 충전 상태 추정 방법.
- 제44항에 있어서, 상기 (b) 단계 내지 상기 (d) 단계는,상기 펄스 충전이 반복될 때마다 반복되는 것인, 이차 전지의 충전 상태 추정 방법.
- 제44항에 있어서, 상기 (b) 단계 내지 상기 (d) 단계는,각 펄스 충전이 진행되는 동안, 상기 동적 전압 프로파일이 상기 전이구간 전압 패턴으로 식별되는 조건이 성립될 때, 반복되는 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항에 있어서,상기 추정된 충전 상태를 그래픽 인터페이스로 표시하는 단계를 더 포함하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항에 있어서,상기 추정된 충전 상태를 저장되는 단계를 더 포함하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항에 있어서,상기 추정된 충전 상태를 외부로 출력하는 단계를 더 포함하는 것인, 이차 전지의 충전 상태 추정 방법.
- 서로 다른 동작 전압 범위를 갖는 제1양극재 및 제2양극재를 포함하는 혼합 양극재가 포함되어 있는 양극, 음극재를 포함하는 음극 및 상기 양극과 음극을 분리시키는 분리막을 포함하고 하이브리드(HEV) 모드가 지원되는 전기 구동 자동차에 탑재된 이차 전지의 충전 상태를 추정하는 방법으로서,(a) 상기 하이브리드 모드에서 상기 이차 전지의 충전이 개시되는 단계;(b) 상기 충전이 진행되는 동안 상기 이차 전지의 동적 전압을 측정하는 단계;(c) 상기 이차 전지의 동적 전압 프로파일을 전이구간 전압 패턴으로 식별하는 단계;(d) 상기 식별된 전이구간 전압 패턴의 파라미터를 계산하는 단계; 및(e) 상기 파라미터와 충전 상태 사이의 미리 정의된 상관 관계를 이용하여 상기 계산된 파라미터로부터 이차 전지의 충전 상태를 추정하는 단계를 포함하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제50항에 있어서,상기 하이브리드 모드에서 상기 이차 전지의 충전과 방전 사이클이 반복되는 단계;를 더 포함하고,상기 각 충전 사이클에서, 상기 (b) 단계 내지 (e) 단계를 반복하는 것인 이차 전지의 충전 상태 추정 방법.
- 제50항 또는 제51항에 있어서,상기 충전은 시간 간격을 두고 펄스 충전이 반복되는 충전인 것인, 이차 전지의 충전 상태 추정 방법.
- 제52항에 있어서,상기 펄스 충전이 반복될 때마다 상기 (b) 단계 내지 (e) 단계를 반복하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제52항에 있어서, 상기 (b) 단계 내지 (e) 단계는,각 펄스 충전이 진행되는 동안, 상기 동적 전압 프로파일이 상기 전이구간 전압 패턴으로 식별되는 조건이 성립될 때, 반복되는 것인, 이차 전지의 충전 상태 추정 방법.
- 제50항에 있어서,상기 미리 정의된 상관 관계는, 상기 파라미터와 상기 충전 상태 사이의 대응 관계를 정의한 룩업 테이블인 것인, 이차 전지의 충전 상태 추정 방법.
- 제50항에 있어서,상기 미리 정의된 상관 관계는, 상기 파라미터를 입력 변수로 하고, 상기 충전 상태를 출력 변수로 하는 룩업 함수인 것인, 이차 전지의 충전 상태 추정 방법.
- 서로 다른 동작 전압 범위를 갖는 제1양극재 및 제2양극재를 포함하는 혼합 양극재가 포함되어 있는 양극, 음극재를 포함하는 음극 및 상기 양극과 음극을 분리시키는 분리막을 포함하는 이차 전지의 충전 상태를 추정하는 방법으로서,(a) 상기 이차 전지가 충전되는 동안, 상기 이차 전지의 동적 전압을 측정하는 단계;(b) 상기 측정된 동적 전압으로부터 변곡점 식별자를 계산하는 단계;(c) 상기 변곡점 식별자가 변곡점 발생 조건을 충족하면, 전이구간 전압 패턴에 대응되는 파라미터를 결정하는 단계; 및(d) 상기 파라미터와 충전 상태 사이의 미리 정의된 상관 관계를 이용하여 상기 결정된 파라미터로부터 이차 전지의 충전 상태를 추정하는 단계를 포함하는 것인, 이차 전지의 충전 상태 추정 방법.
- 서로 다른 동작 전압 범위를 갖는 제1양극재 및 제2양극재를 포함하는 혼합 양극재가 포함되어 있는 양극, 음극재를 포함하는 음극 및 상기 양극과 음극을 분리시키는 분리막을 포함하고 하이브리드(HEV) 모드가 지원되는 전기 구동 자동차에 탑재된 이차 전지의 충전 상태를 추정하는 방법으로서,(a) 상기 하이브리드 모드에서 상기 이차 전지의 충전이 개시되는 단계;(b) 상기 충전이 진행되는 동안 상기 이차 전지의 동적 전압을 측정하는 단계;(c) 상기 측정된 동적 전압으로부터 변곡점 식별자를 계산하는 단계;(d) 상기 변곡점 식별자가 변곡점 발생 조건을 충족하면, 전이구간 전압 패턴에 대응되는 파라미터를 결정하는 단계; 및(e) 상기 파라미터와 충전 상태 사이의 미리 정의된 상관 관계를 이용하여 상기 결정된 파라미터로부터 이차 전지의 충전 상태를 추정하는 단계를 포함하는 것인, 이차 전지의 충전 상태 추정 방법.
- 제36항 내지 제58항 중 어느 한 항에 따른 이차 전지의 전압 추정 방법을 프로그램화하여 수록한 컴퓨터로 읽을 수 있는 기록 매체.
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Also Published As
Publication number | Publication date |
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US20150100260A1 (en) | 2015-04-09 |
US10408886B2 (en) | 2019-09-10 |
EP2848953A1 (en) | 2015-03-18 |
CN104364669B (zh) | 2017-02-22 |
JP6251255B2 (ja) | 2017-12-20 |
PL3901642T3 (pl) | 2022-11-21 |
EP2848953B1 (en) | 2017-11-15 |
KR20130139760A (ko) | 2013-12-23 |
EP2848953A4 (en) | 2016-10-12 |
CN104364669A (zh) | 2015-02-18 |
EP3339870B1 (en) | 2021-08-04 |
EP3339870A1 (en) | 2018-06-27 |
KR101487495B1 (ko) | 2015-01-29 |
EP3901642A1 (en) | 2021-10-27 |
JP2015528101A (ja) | 2015-09-24 |
JP2017067790A (ja) | 2017-04-06 |
JP6280196B2 (ja) | 2018-02-14 |
PL3339870T3 (pl) | 2021-12-13 |
EP3901642B1 (en) | 2022-09-14 |
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